ALBERT

Description: The sensitivity of global climate to the episodicity of fire aerosol emissions Atmospheric Chemistry and Physics Discussions, 13, 23691-23717, 2013 Author(s): S. K. Clark, D. S. Ward, and N. M. Mahowald One of the major ways in which forest and grass fires have an impact on global climate is through the release of aerosols. Most studies focusing on calculating the radiative forcing and other climate impacts of fire aerosols use monthly mean emissions derived from the Global Fire Emissions Database that captures only the seasonal cycle of fire aerosol emissions. Here we present the results of a sensitivity study that investigates the climate response to the episodicity of the fires, based on the standard approach which releases emissions every day, and contrasts that to the response when fires are represented as intense pulses of emissions that occur only over 1–2 days on a monthly, yearly, or five-yearly basis. Overall we find that in the modified cases with increased levels of episodicity, the all sky direct effect radiative forcing increases, the clear sky direct effect radiative forcing remains relatively constant, and the magnitude of the indirect effect radiative forcing decreases by about 1 W m −2 (from −1.6 to −0.6 W m −2 ). In the long term, we find that an increase in aerosol emission episodicity leads to an asymmetric change in indirect radiative forcing in the Northern Hemisphere compared to the Southern Hemisphere contributes to a slight shift in the annual average position of the intertropical convergence zone (ITCZ). This shift is found to have a mixed effect on the overall performance of the model at predicting precipitation rates in the tropics. Given these results we conclude that future studies that look to assess the present day global climate impacts of fire aerosols should consider the need to accurately represent fire episodicity.

Description: A new data set of soil mineralogy for dust-cycle modeling Atmospheric Chemistry and Physics Discussions, 13, 23943-23993, 2013 Author(s): E. Journet, Y. Balkanski, and S. P. Harrison The mineralogy of airborne dust affects the impact of dust particles on direct and indirect radiative forcing, on atmospheric chemistry and on biogeochemical cycling. It is determined partly by the mineralogy of the dust-source regions and partly by size-dependent fractionation during erosion and transport. Here we present a data set that characterizes the clay and silt sized fractions of global soil units in terms of the abundance of 12 minerals that are important for dust-climate interactions: quartz, feldspars, illite, smectite, kaolinite, chlorite, vermiculite, mica, calcite, gypsum, hematite and goethite. The basic mineralogical information is derived from the literature, and is then expanded following explicit rules, in order to characterize as many soil units as possible. We present three alternative realisations of the mineralogical maps that account for the uncertainties in the mineralogical data. We examine the implications of the new database for calculations of the single scattering albedo of airborne dust and thus for dust radiative forcing.

Description: Growth of sulphuric acid nanoparticles under wet and dry conditions Atmospheric Chemistry and Physics Discussions, 13, 24087-24125, 2013 Author(s): L. Škrabalová, D. Brus, T. Anttila, V. Ždímal, and H. Lihavainen New particle formation, which greatly influences the number concentrations and size distributions of an atmospheric aerosol, is often followed by a rapid growth of freshly formed particles. The initial growth of a newly formed aerosol is the crucial process determining the fraction of nucleated particles growing into cloud condensation nuclei sizes, which have a significant influence on climate. In this study, we report the laboratory observations of the growth of nanoparticles produced by nucleation of H 2 SO 4 and water in a laminar flow tube at temperatures of 283, 293 and 303 K, under dry (a relative humidity of 1%) and wet conditions (relative humidity of 30%) and residence times of 30, 45, 60 and 90 s. The initial H 2 SO 4 concentration spans the range from 2 × 10 8 to 1.4 × 10 10 molecule cm −3 and the calculated wall losses of H 2 SO 4 were assumed to be diffusion limited. The detected particle number concentrations, measured by the Ultrafine Condensation Particle Counter (UCPC) and Differential Mobility Particle Sizer (DMPS), were found to depend strongly on the residence time. Hygroscopic particle growth, presented by growth factors, was found to be in good agreement with the previously reported studies. The experimental growth rates ranged from 20 nm h −1 to 890 nm h −1 at RH 1% and from 7 nm h −1 to 980 nm h −1 at RH 30% and were found to increase significantly with the increasing concentration of H 2 SO 4 . Increases in the nucleation temperature had a slight enhancing effect on the growth rates under dry conditions. The influence of relative humidity on growth was not consistent – at lower H 2 SO 4 concentrations, the growth rates were higher under dry conditions while at H 2 SO 4 concentrations greater than 1×10 9 molecule cm −3 the growth rates were higher under wet conditions. The growth rates show only a weak dependence on the residence time. The experimental observations were compared with predictions made using a numerical model, which investigates the growth of particles with three different extents of neutralization by the ammonia NH 3 : (1) pure H 2 SO 4 – H 2 O particles (2) particles formed by ammonium bisulphate, (NH 4 )HSO 4 (3) particles formed by ammonium sulphate, (NH 4 ) 2 SO 4 . The highest growth rates were found for ammonium sulphate particles. Since the model accounting for the initial H 2 SO 4 concentration predicted the experimental growth rates correctly, our results suggest that the commonly presumed diffusional wall losses of H 2 SO 4 are not so significant. We therefore assume that there are not only losses of H 2 SO 4 on the wall but also a flux of H 2 SO 4 molecules from the wall into the flow tube, the effect being more profound under dry conditions and at higher temperatures of the tube wall. Based on a comparison with the atmospheric observations, our results indicate that sulphuric acid alone can not explain the growth rates of particles formed in the atmosphere.

Description: By using the monthly ERA-40 reanalysis data and observed rainfall data, we investigated the effect of the Indian summer monsoon (ISM) on the South Asian High (SAH) at 200 hPa, and the role played by the SAH in summer rainfall variation over China. It is found that in the interannual timescale the east–west shift is a prominent feature of the SAH, with its center either over the Iranian Plateau or over the Tibetan Plateau. When the ISM is stronger (weaker) than normal, the SAH shifts westward (eastward) to the Iranian Plateau (Tibetan Plateau). The east–west position of SAH has close relation to the summer rainfall over China. A westward (eastward) location of SAH corresponds to less (more) rainfall in the Yangtze-Huai River Valley and more (less) rainfall in North China and South China. A possible physical process that the ISM affects the summer rainfall over China via the SAH is proposed. A stronger (weaker) ISM associated with more (less) rainfall over India corresponds to more (less) condensation heat release and anomalous heating (cooling) in the upper troposphere over the northern Indian peninsula. The anomalous heating (cooling) stimulates positive (negative) height anomalies to its northwest and negative (positive) height anomalies to its northeast in the upper troposphere, causing a westward (eastward) shift of the SAH with its center over the Iranian Plateau (Tibetan Plateau). As a result, an anomalous cyclone (anticyclone) is formed over the eastern Tibetan Plateau and eastern China in the upper troposphere. The anomalous vertical motions in association with the circulation anomalies are responsible for the rainfall anomalies over China. Our present study reveals that the SAH may play an important role in the effect of ISM on the East Asian summer monsoon.

Description: National Centers for Environmental Prediction recently upgraded its operational seasonal forecast system to the fully coupled climate modeling system referred to as CFSv2. CFSv2 has been used to make seasonal climate forecast retrospectively between 1982 and 2009 before it became operational. In this study, we evaluate the model’s ability to predict the summer temperature and precipitation over China using the 120 9-month reforecast runs initialized between January 1 and May 26 during each year of the reforecast period. These 120 reforecast runs are evaluated as an ensemble forecast using both deterministic and probabilistic metrics. The overall forecast skill for summer temperature is high while that for summer precipitation is much lower. The ensemble mean reforecasts have reduced spatial variability of the climatology. For temperature, the reforecast bias is lead time-dependent, i.e., reforecast JJA temperature become warmer when lead time is shorter. The lead time dependent bias suggests that the initial condition of temperature is somehow biased towards a warmer condition. CFSv2 is able to predict the summer temperature anomaly in China, although there is an obvious upward trend in both the observation and the reforecast. Forecasts of summer precipitation with dynamical models like CFSv2 at the seasonal time scale and a catchment scale still remain challenge, so it is necessary to improve the model physics and parameterizations for better prediction of Asian monsoon rainfall. The probabilistic skills of temperature and precipitation are quite limited. Only the spatially averaged quantities such as averaged summer temperature over the Northeast China of CFSv2 show higher forecast skill, of which is able to discriminate between event and non-event for three categorical forecasts. The potential forecast skill shows that the above and below normal events can be better forecasted than normal events. Although the shorter the forecast lead time is, the higher deterministic prediction skill appears, the probabilistic prediction skill does not increase with decreased lead time. The ensemble size does not play a significant role in affecting the overall probabilistic forecast skill although adding more members improves the probabilistic forecast skill slightly.

Description: The south peninsular part of India gets maximum amount of rainfall during the northeast monsoon (NEM) season [October to November (OND)] which is the primary source of water for the agricultural activities in this region. A nonlinear method viz., Extreme learning machine (ELM) has been employed on general circulation model (GCM) products to make the multi-model ensemble (MME) based estimation of NEM rainfall (NEMR). The ELM is basically is an improved learning algorithm for the single feed-forward neural network (SLFN) architecture. The 27 year (1982–2008) lead-1 (using initial conditions of September for forecasting the mean rainfall of OND) hindcast runs (1982–2008) from seven GCM has been used to make MME. The improvement of the proposed method with respect to other regular MME (simple arithmetic mean of GCMs (EM) and singular value decomposition based multiple linear regressions based MME) has been assessed through several skill metrics like Spread distribution, multiplicative bias, prediction errors, the yield of prediction, Pearson’s and Kendal’s correlation coefficient and Wilmort’s index of agreement. The efficiency of ELM estimated rainfall is established by all the stated skill scores. The performance of ELM in extreme NEMR years, out of which 4 years are characterized by deficit rainfall and 5 years are identified as excess, is also examined. It is found that the ELM could expeditiously capture these extremes reasonably well as compared to the other MME approaches.

Description: The sea surface temperature anomaly pattern differs between the central Pacific (CP) and eastern Pacific (EP) El Niños during boreal summer. It is expected that the respective atmospheric response will be different. In order to identify differences in the responses to these two phenomena, we examine the Community Atmosphere Model Version 4 simulations forced with observed monthly sea surface temperature during 1979–2010 and compare with the corresponding observations. For CP El Niño, a triple precipitation anomaly pattern appears over East Asia. During EP El Niño, the triple pattern is not as significant as and shifts eastward and southward compared to CP El Niño. We also examine the influence of CP La Niña and EP La Niña on East Asia. In general, the impact of CP (EP) La Niña on tropics and East Asia seems to be opposite to that of CP (EP) El Niño. However, the impacts between the two types of La Niña are less independent compared to the two types of warm events. Both types of El Niño (La Niña) correspond to a stronger (weaker) western North Pacific summer monsoon. The sensitivity experiments support this result. But the CP El Niño (La Niña) may have more significant influence on East Asia summer climate than EP El Niño (La Niña), as the associated low-level anomalous wind pattern is more distinct and closer to the Asian continent compared to EP El Niño (La Niña).

Description: Since the Mediterranean Sea is halfway between subtropical and middle latitudes, and it represents a marginal oceanic region, research has tended to focus on how large-scale modes of atmospheric variability modulate its surface temperature. Conversely, the present study examines the potential influence of the Mediterranean Sea surface temperature (SST) anomalies on the Northern Hemisphere atmospheric circulation. In particular, this work explores the large-scale changes in the global circulation forced/influenced by the eastern Mediterranean summer-autumn SST pattern. To isolate the atmospheric response, AGCM sensitivity experiments with prescribed SST over the Mediterranean Sea and climatology elsewhere are analysed. Observational diagnostics upon the period used to define the boundary conditions (1979–2002) are also interpreted. Our results support the hypothesis of an atmospheric pattern initiated in the Mediterranean basin, pointing out both a local baroclinic response and a barotropic circumglobal anomaly. This atmospheric teleconnection pattern projects onto a hemispheric wave-like structure, reflecting the waveguide effect of the westerly jets. Results suggest, thereby, that the recurrent summer-autumn circumglobal teleconnection pattern can be excited locally by changes in the atmosphere over the Mediterranean region. A linear behaviour is found upon a regional impact over northeastern Africa. The remote impacts present however a nonlinear signature: anomalous warm conditions influencing on northern Europe and Euro–Asia, whereas anomalous cold conditions impacting more on the North Pacific basin. Limitations in our model setup are also discussed.

Description: Impacts of different plant functional types on ambient ozone predictions in the Seoul Metropolitan Areas (SMA), Korea Atmospheric Chemistry and Physics Discussions, 13, 24925-24973, 2013 Author(s): H.-K. Kim, J.-H. Woo, R. S. Park, C. H. Song, J.-H. Kim, S.-J. Ban, and J.-H. Park Plant functional type (PFT) distributions affect the results of biogenic emission modeling as well as O 3 and PM simulations using chemistry-transport models (CTMs). This paper analyzes the variations of both surface biogenic VOC emissions and O 3 concentrations due to changes in the PFT distributions in the Seoul Metropolitan Areas, Korea. Also, this paper attempts to provide important implications for biogenic emissions modeling studies for CTM simulations. MM5-MEGAN-SMOKE-CMAQ model simulations were implemented over the Seoul Metropolitan Areas in Korea to predict surface O 3 concentrations for the period of 1 May to 31 June 2008. Starting from MEGAN biogenic emissions analysis with three different sources of PFT input data, US EPA CMAQ O 3 simulation results were evaluated by surface O 3 monitoring datasets and further considered on the basis of geospatial and statistical analyses. The three PFT datasets considered were "(1)KORPFT", developed with a region specific vegetation database; (2) CDP, adopted from US NCAR; and (3) MODIS, reclassified from the NASA Terra and Aqua combined land cover products. Comparisons of MEGAN biogenic emission results with the three different PFT data showed that broadleaf trees (BT) are the most significant contributor, followed by needleleaf trees (NT), shrub (SB), and herbaceous plants (HB) to the total biogenic volatile organic compounds (BVOCs). In addition, isoprene from BT and terpene from NT were recognized as significant primary and secondary BVOC species in terms of BVOC emissions distributions and O 3 -forming potentials in the study domain. Multiple regression analyses with the different PFT data (δO 3 vs. δPFTs) suggest that KORPFT can provide reasonable information to the framework of MEGAN biogenic emissions modeling and CTM O 3 predictions. Analyses of the CMAQ performance statistics suggest that deviations of BT areas can significantly affect CMAQ isoprene and O 3 predictions. From further evaluations of the isoprene and O 3 prediction results, we explored the PFT area-loss artifact that occurs due to geographical disparity between the PFT and leaf area index distributions, and can cause increased bias in CMAQ O 3 . Thus, the PFT-loss artifact must be a source of limitation in the MEGAN biogenic emission modeling and the CTM O 3 simulation results. Time changes of CMAQ O 3 distributions with the different PFT scenarios suggest that hourly and local impacts from the different PFT distributions on occasional inter-deviations of O 3 are quite noticeable, reaching up to 10 ppb. Exponentially diverging hourly BVOC emissions and O 3 concentrations with increasing ambient temperature suggest that the use of representative PFT distributions becomes more critical for O 3 air quality modeling (or forecasting) in support of air quality decision-making and human health studies.

Description: Incidence of rough and irregular atmospheric ice particles from Small Ice Detector 3 measurements Atmospheric Chemistry and Physics Discussions, 13, 24975-25012, 2013 Author(s): Z. Ulanowski, P. H. Kaye, E. Hirst, R. S. Greenaway, R. J. Cotton, E. Hesse, and C. T. Collier The knowledge of properties of ice crystals such as size, shape, concavity and roughness is critical in the context of radiative properties of ice and mixed phase clouds. Limitations of current cloud probes to measure these properties can be circumvented by acquiring two-dimensional light scattering patterns instead of particle images. Such patterns were obtained in situ for the first time using the Small Ice Detector 3 (SID-3) probe during several flights in a variety of mid-latitude mixed phase and cirrus clouds. The patterns are analyzed using several measures of pattern texture, selected to reveal the magnitude of particle roughness or complexity. The retrieved roughness is compared to values obtained from a range of well-characterized test particles in the laboratory. It is found that typical in situ roughness corresponds to that found in the rougher subset of the test particles, and sometimes even extends beyond the most extreme values found in the laboratory. In this study we do not differentiate between small-scale, fine surface roughness and large-scale crystal complexity. Instead, we argue that both can have similar manifestations in terms of light scattering properties and also similar causes. Overall, the in situ data is consistent with ice particles with highly irregular or rough surfaces being dominant. Similar magnitudes of roughness were found in growth and sublimation zones of cirrus. The roughness was found to be negatively correlated with the halo ratio, but not with other thermodynamic or microphysical properties found in situ. Slightly higher roughness was observed in cirrus forming in clean oceanic airmasses than in a continental, polluted one. Overall, the roughness and complexity is expected to lead to increased shortwave cloud reflectivity, in comparison with cirrus composed of more regular, smooth ice crystal shapes. These findings put into question suggestions that climate could be modified through aerosol seeding to reduce cirrus cover and optical depth, as the seeding may result in decreased shortwave reflectivity.

Description: Atlantic Multidecadal Variability (AMV) is investigated in a millennial control simulation with the Kiel Climate Model (KCM), a coupled atmosphere–ocean–sea ice model. An oscillatory mode with approximately 60 years period and characteristics similar to observations is identified with the aid of three-dimensional temperature and salinity joint empirical orthogonal function analysis. The mode explains 30 % of variability on centennial and shorter timescales in the upper 2,000 m of the North Atlantic. It is associated with changes in the Atlantic Meridional Overturning Circulation (AMOC) of ±1–2 Sv and Atlantic Sea Surface Temperature (SST) of ±0.2 °C. AMV in KCM results from an out-of-phase interaction between horizontal and vertical ocean circulation, coupled through Irminger Sea convection. Wintertime convection in this region is mainly controlled by salinity anomalies transported by the Subpolar Gyre (SPG). Increased (decreased) dense water formation in this region leads to a stronger (weaker) AMOC after 15 years, and this in turn leads to a weaker (stronger) SPG after another 15 years. The key role of salinity variations in the subpolar North Atlantic for AMV is confirmed in a 1,000 year long simulation with salinity restored to model climatology: No low frequency variations in convection are simulated, and the 60 year mode of variability is absent.

Description: Based on a generated time series for the central pressure of the Siberian High, and on defining a robust Siberian High Index (SHI), the behavior of this atmospheric center of action is examined from 1949 to 2010 with regard to inter-annual variations, persistence, trends, abrupt changes, spectral analysis and interactions. The interannual variability in the central pressure of the Siberian High is considerable. The mean downward linear and non-linear trend over the entire period (1949–2010) is estimated and is found to be statistically significant at the 95 % confidence level. Low frequency variation and linearity within the SHI time series are found from the persistence analysis. Using spectral analysis, the center of action of the Siberian High is characterized by non-periodic behavior; the peaks occur only at the lowest frequency and may be related to the Sea Surface Temperature (SST) over the El Niño region. The Siberian High is affected by the Hadley circulation cell; there is no detectable connection between the Walker circulation cell and the Siberian High. SSTs over the El Niño region may affect the Siberian High. Interactions between the Siberian High and the SSTs over the tropical Atlantic Ocean are absent. The SHI is positively correlated to surface air temperatures over Saudi Arabia, and this is statistically significant in the western and north-western regions.

Description: This study investigates the spatial and temporal characteristics of cold surges that propagates northward along the eastern flank of the Andes from subtropical to tropical South America analysing wintertime in situ daily minimum temperature observations from Argentina, Bolivia and Peru and ERA-40 reanalysis over the 1975–2001 period. Cold surges usually last 2 or 3 days but are generally less persistent in the southern La Plata basin compared to tropical regions. On average, three to four cold surges are reported each year. Our analysis reveals that 52 % of cold episodes registered in the south of La Plata basin propagate northward to the northern Peruvian Amazon at a speed of around 20 m s −1 . In comparison to cold surges that do not reach the tropical region, we demonstrate that these cold surges are characterized, before they reach the tropical region, by a higher occurrence of a specific circulation pattern associated to southern low-level winds progression toward low latitudes combined with subsidence and dry condition in the middle and low troposphere that reinforce the cold episode through a radiative effect. Finally, the relationship between cold surges and atmosphere dynamics is illustrated for the two most severe cold intrusions that reached the Peruvian and Bolivian Amazon in the last 20 years.

Description: The Greenland ice sheet is projected to be strongly affected by global warming. These projections are either issued from downscaling methods (such as Regional Climate Models) or they come directly from General Circulation Models (GCMs). In this context, it is necessary to evaluate the accuracy of the daily atmospheric circulation simulated by the GCMs, since it is used as forcing for downscaling methods. Thus, we use an automatic circulation type classification based on two indices (Euclidean distance and Spearman rank correlation using the daily 500 hPa geopotential height) to evaluate the ability of the GCMs from both CMIP3 and CMIP5 databases to simulate the main circulation types over Greenland during summer. For each circulation type, the GCMs are compared to three reanalysis datasets on the basis of their frequency and persistence differences. For the current climate (1961–1990), we show that most of the GCMs do not reproduce the expected frequency and the persistence of the circulation types and that they simulate poorly the observed daily variability of the general circulation. Only a few GCMs can be used as reliable forcings for downscaling methods over Greenland. Finally, when applying the same approach to the future projections of the GCMs, no significant change in the atmospheric circulation over Greenland is detected, besides a generalised increase of the geopotential height due to a uniform warming of the atmosphere.

Description: The East Asian summer monsoon (EASM) features strong humid low-level southerly flows and abundant rainfall over the subtropical East Asia. This study identified how condensational heating generated by the EASM rainfall can affect the EASM circulation by contrasting two 10-member ensembles of atmospheric General Circulation Model experiments with Community Climate Model version 3/National Center for Atmospheric Research respectively with and without feedback of condensational heating over the East Asian domain. Major results inferred from the experiments are as follows. Condensational heating is found to absolutely dominate diabatic heating over East Asia. Exclusion of the feedback of condensational heating leads to a significant weakening of summertime tropospheric warming over land and thus a large reduction of the land-sea thermal contrast between entire Asian continent and surrounding oceans. Associated with this, the lower-level EASM flows are weakened, South Asian High at 200 hPa migrates southward with reduced intensity and breaks over East Asia with southerly flows prevailing in the upper troposphere, in contrast to northerly flows in reality. Consequently, local EASM meridional cell disappears and the baroclinic structure featured by the EASM circulation that is dynamically determined by convective condensational heating over East Asia is altered to a barotropic structure. Therefore, it is concluded that the feedback of condensational heating acts to largely enhance lower-level flows of the EASM and essentially determine its baroclinic structure and meridional cell, once the solar radiation and inhomogeneity of the Earth’s surface form low-level monsoon flows in East Asia by enhancing land-sea thermal contrast.

Description: Based on experiments using a coupled general circulation model which resolves tropical ocean–atmosphere coupled phenomena such as El Niño/Southern Oscillation (ENSO) and the Indian Ocean Dipole, forcing mechanisms of the Indian Ocean subtropical dipole (IOSD) are investigated. In the control experiment, as in the observation, several types of the IOSD are generated by the variations in the Mascarene High during austral summer and characterized by a dipole pattern of sea surface temperature (SST) anomalies in the northeastern and southwestern parts of the southern Indian Ocean. In another experiment, where the SST outside the southern Indian Ocean is nudged toward the monthly climatology of the simulated SST, one type of the IOSD occurs, but it is less frequent and associated with the zonal wavenumber four pattern of equivalently barotropic geopotential height anomalies in high latitudes, suggesting an interesting link with the Antarctic Circumpolar Wave. This indicates that, even without the atmospheric teleconnection from tropical coupled climate modes, the IOSD may develop in association with the atmospheric variability in high latitudes of the Southern Hemisphere. In the other experiment, where only the southern Indian Ocean and the tropical Pacific are freely interactive with the atmosphere, two types of both positive and negative IOSD occur. Since the occurrence frequency of the IOSD significantly increases as compared to the second experiment, this result confirms that the atmospheric teleconnection from ocean-atmosphere coupled modes in the tropical Pacific such as ENSO may also induce the variations in the Mascarene High that generate the IOSD. The present research, even within the realm of model studies, shows clearly that the predictability of the IOSD in mid-latitudes is related to both low and high-latitudes climate variations.

Description: Factors controlling pollutant plume length downwind of major roadways in nocturnal surface inversions Atmospheric Chemistry and Physics Discussions, 13, 25253-25290, 2013 Author(s): W. Choi, A. M. Winer, and S. E. Paulson A curve fit method using a Gaussian dispersion model solution was successfully applied to obtain both dispersion coefficients and a particle number emission factor (PNEF) directly from ultrafine particle (UFP) concentration profiles observed downwind of major roadways in California's South Coast Air Basin (SoCAB). The Briggs' formulation for the vertical dispersion parameter σ z was adopted in this study due to its better performance in describing the observed profiles compared to other formulations examined. The two dispersion coefficients in Briggs' formulation, α and β, ranged from 0.02 to 0.07 and from −0.5 × 10 −3 to 2.8 × 10 −3 , respectively, for the four freeway transects studied and are significantly different for freeways passing over vs. under the street on which measurements of the freeway plume were made. These ranges are wider than literature values for α and β under stable conditions. The dispersion coefficients derived from observations showed strong correlations with both surface meteorology (wind speed/direction, temperature, and air stability) and differences in concentrations between the background and plume peak. The relationships were applied to predict freeway plume transport using a multivariate regression, and produced excellent agreement with observed UFP concentration profiles. The mean PNEF for a mixed vehicle fleet on the four freeways was estimated as 1.2 × 10 14 particles mi −1 vehicle −1 , which is about 15% of the value estimated in 2001 for the I-405 freeway, implying significant reductions in UFP emissions over the past decade in the SoCAB.

Description: Summer Sea Ice Albedo in the Arctic in CMIP5 models Atmospheric Chemistry and Physics Discussions, 13, 25219-25251, 2013 Author(s): T. Koenigk, A. Devasthale, and K.-G. Karlsson Spatial and temporal variations of summer sea ice albedo over the Arctic are analyzed using an ensemble of historical CMIP5 model simulations. The results are compared to the CLARA-SAL product that is based on long-term satellite observations. The summer sea ice albedo varies substantially among CMIP5 models and many models show large biases compared to the CLARA-SAL product. Single summer months show an extreme spread of ice albedo among models; July-values vary between 0.3 and 0.7 for individual models. The CMIP5 ensemble mean, however, agrees relatively well in the Central Arctic but shows too high ice albedo near the ice edges and coasts. In most models, the ice albedo is spatially too uniformly distributed. The summer to summer variations seem to be underestimated in many global models and almost no model is able to fully reproduce the temporal evolution of ice albedo throughout the summer. While the satellite observations indicate the lowest ice albedos during August, the models show minimum values in July and substantially higher values in August. Instead, the June values are often lower in the models than in the satellite observations. This is probably due to too high surface temperatures in June, leading to an early start of the melt season and too cold temperatures in August causing an earlier refreezing in the models. The summer sea ice albedo in the CMIP5 models is strongly governed by surface temperature and snow conditions, particularly during the period of melt onset in early summer and refreezing in late summer. The summer surface net solar radiation of the ice covered Arctic areas is highly related to the ice albedo in the CMIP5 models. However, the impact of the ice albedo on the sea ice conditions in the CMIP5 models is not clearly visible. This indicates the importance of other Arctic and large scale processes for the sea ice conditions.

Description: Intercontinental transport and deposition patterns of atmospheric mercury from anthropogenic emissions Atmospheric Chemistry and Physics Discussions, 13, 25185-25218, 2013 Author(s): L. Chen, H.-H. Wang, J.-F. Liu, W. Zhang, D. Hu, C. Chen, and X.-J. Wang Global policies that regulate anthropogenic mercury emissions to the environment require quantitative and comprehensive source–receptor relationships for mercury emissions, transport and deposition among major continental regions. In this study, we use the GEOS-Chem model to establish source–receptor relationships among eleven major continental regions worldwide. Source–receptor relationships for surface mercury concentrations (SMC) show that some regions (e.g. East Asia, the Indian subcontinent and Europe) should be responsible for their local surface Hg(II) and Hg(P) concentrations because of near-field transport and deposition contributions from their local anthropogenic emissions (up to 64% and 71% for Hg(II) and Hg(P), respectively, over East Asia). We define region of primary influence (RPI) and region of secondary influence (RSI) to establish intercontinental influence patterns. Results indicate that East Asia is SMC RPI for almost all other regions, while Europe, Russia and the Indian subcontinent also make some contributions to SMC over some receptor regions because they are dominant RSI source regions. Source–receptor relationships for mercury deposition show that approximately 16% and 17% of dry and wet deposition, respectively, over North America originate from East Asia, indicating that trans-pacific transport of East Asian emissions is the major foreign source of mercury deposition in North America. Europe, Southeast Asia and the Indian subcontinent are also important mercury deposition sources for some receptor regions because they are dominant RSI. We also quantify seasonal variation on mercury deposition contributions over other regions from East Asia. Results show that mercury deposition (including dry and wet) contributions from East Asia over the Northern Hemisphere receptor regions (e.g. North America, Europe, Russia, Middle East and Middle Asia) vary seasonally, with the maximum values in summer and minimum values in winter. The opposite seasonal pattern occurs on mercury dry deposition contributions over Southeast Asia and the Indian subcontinent.

Description: Previous studies have linked the rapid sea level rise (SLR) in the western tropical Pacific (WTP) since the early 1990s to the Pacific decadal climate modes, notably the Pacific Decadal Oscillation in the north Pacific or Interdecadal Pacific Oscillation (IPO) considering its basin wide signature. Here, the authors investigate the changing patterns of decadal (10–20 years) and multidecadal (〉20 years) sea level variability (global mean SLR removed) in the Pacific associated with the IPO, by analyzing satellite and in situ observations, together with reconstructed and reanalysis products, and performing ocean and atmosphere model experiments. Robust intensification is detected for both decadal and multidecadal sea level variability in the WTP since the early 1990s. The IPO intensity, however, did not increase and thus cannot explain the faster SLR. The observed, accelerated WTP SLR results from the combined effects of Indian Ocean and WTP warming and central-eastern tropical Pacific cooling associated with the IPO cold transition. The warm Indian Ocean acts in concert with the warm WTP and cold central-eastern tropical Pacific to drive intensified easterlies and negative Ekman pumping velocity in western-central tropical Pacific, thereby enhancing the western tropical Pacific SLR. On decadal timescales, the intensified sea level variability since the late 1980s or early 1990s results from the “out of phase” relationship of sea surface temperature anomalies between the Indian and central-eastern tropical Pacific since 1985, which produces “in phase” effects on the WTP sea level variability.

Description: Balloon-borne match measurements of mid-latitude cirrus clouds Atmospheric Chemistry and Physics Discussions, 13, 25417-25479, 2013 Author(s): A. Cirisan, B. P. Luo, I. Engel, F. G. Wienhold, U. K. Krieger, U. Weers, G. Romanens, G. Levrat, P. Jeannet, D. Ruffieux, R. Philipona, B. Calpini, P. Spichtinger, and T. Peter Observations of persistent high supersaturations with respect to ice inside cirrus clouds are challenging our understanding of cloud microphysics and of climate feedback processes in the upper troposphere. Single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information of the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer "SnowWhite" and a particle backscatter detector "COBALD" (Compact Optical Backscatter Aerosol Detector). Extensive trajectory calculations based on regional weather model COSMO forecasts are performed for flight planning and COSMO analyses are used as basis for comprehensive microphysical box modeling (with grid scale 2 km and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear sky or cloudy sky conditions, highlighting the importance of a proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive, 4-km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the extreme humidity conditions in the upper troposphere.

Description: An explicit study of aerosol mass conversion and its parameterization in warm rain formation of cumulus clouds Atmospheric Chemistry and Physics Discussions, 13, 25481-25536, 2013 Author(s): J. Sun, J. Fen, and R. K. Ungar The life time of atmospheric aerosols is highly affected by in-cloud scavenging processes. Aerosol mass conversion from aerosols embedded in cloud droplets into aerosols embedded in raindrops is a pivotal pathway for wet removal of aerosols in clouds. The aerosol mass conversion rate in the bulk microphysics parameterizations is always assumed to be linearly related to the precipitation production rate, which includes the cloud water autoconversion rate and the cloud water accretion rate. The ratio of the aerosol mass concentration conversion rate to the cloud aerosol mass concentration has typically been considered to be the same as the ratio of the precipitation production rate to the cloud droplet mass concentration. However, the mass of an aerosol embedded in a cloud droplet is not linearly proportional to the mass of the cloud droplet. A simple linear relationship cannot be drawn between the precipitation production rate and the aerosol mass concentration conversion rate. In this paper, we studied the evolution of aerosol mass concentration conversion rates in a warm rain formation process with a 1.5-dimensional non-hydrostatic convective cloud and aerosol interaction model in the bin microphysics. We found that the ratio of the aerosol mass conversion rate to the cloud aerosol mass concentration can be statistically expressed by the ratio of the precipitation production rate to the cloud droplet mass concentration with an exponential function. We further gave some regression equations to determine aerosol conversions in the warm rain formation under different threshold radii of raindrops and different aerosol size distributions.

Description: The goal of this study is to develop a high-resolution atmospheric hindcast over the Mediterranean area using the WRF-ARW model, focusing on offshore surface wind fields. In order to choose the most adequate model configuration, the study provides details on the calibration of the experimental saet-up through a sensitivity test considering the October–December 2001 period (the 2001 super-storm event in the West Mediterranean). A daily forecast outperforms the spectral technique of previous products and the boundary data from ERA-Interim reanalysis produces the most accurate estimates in terms of wind variability and hour-to-hour correspondence. According to the sensitivity test, two data sets of wind hindcast are produced: the SeaWind I (30-km horizontal resolution for a period of 60 years) and the SeaWind II (15-km horizontal resolution for 20 years). The validation of the resulting surface winds is undertaken considering two offshore observational datasets. On the one hand, hourly surface buoy stations are used to validate wind time series at specific locations; on the other hand, wind altimeter satellite observations are considered for spatial validation in the whole Mediterranean Sea. The results obtained from this validation process show a very good agreement with observations for the southern Europe region. Finally, SeaWind I and II are used to characterize offshore wind fields in the Mediterranean Sea. The statistical structure of sea surface wind is analyzed and the agreement with Weibull probability distribution is discussed. In addition, wind persistence and extreme wind speed (50 year return period) are characterized and relevant areas of wind power generation are described by estimating wind energy quantities.

Description: Global and regional impacts of HONO on the chemical composition of clouds and aerosols Atmospheric Chemistry and Physics Discussions, 13, 23599-23638, 2013 Author(s): Y. F. Elshorban, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld Nitrous acid (HONO) photolysis can significantly increase HO x (OH+HO 2 ) radical formation, enhancing organic and inorganic oxidation products in polluted regions, especially during winter. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that HONO can significantly enhance aerosol sulphate (S(VI)), mainly due to the increased formation of H 2 SO 4 . Even though in-cloud aqueous phase oxidation of dissolved SO 2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H 2 O 2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO 3 formation and N 2 O 5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model-measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and the central role of cloud chemical processing in aerosol formation.

Description: Injection heights of springtime biomass burning plumes over the Peninsular Southeast Asia and their impacts on pollutant long-range transport Atmospheric Chemistry and Physics Discussions, 13, 23781-23816, 2013 Author(s): Y. Jian and T.-M. Fu We analyzed observations from the Multi-angle Imaging SpectroRadiometer (MISR) to determine the injection heights of biomass burning smoke plumes over the Peninsular Southeast Asia (PSEA) in spring, with the goal of evaluating the impacts on pollutant long-range transport. We retrieved the heights of twenty-two thousand MISR smoke pixels from 607 smoke plumes over the PSEA during February to April of the years 2001–2010. Forty-five percent of the analyzed smoke pixels were above the local mean boundary layer (1 km) at MISR overpass time (10:30 a.m. local time). We used the GEOS-Chem model to simulate the transport of PSEA biomass burning pollutants in March 2001. We found that the direct injection of 40% of the PSEA biomass burning emissions had little impact on the long-range transport of CO to downwind regions, compared to a control simulation where all biomass burning emissions were released in the boundary layer. This was because CO at the surface over the PSEA was efficiently lifted into the free troposphere by deep convection associated with synoptic-scale weather systems. For pollutants with lifetimes shorter than the synoptic timescale, such as black carbon aerosol (BC), their long-range transport was much more sensitive to the initial plume injection height. The direct injection of NO x from PSEA biomass burning into the free troposphere drove increased formation and transport of PAN, which in turn led to significant increases of ozone over downwind southern China and northwestern Pacific. The Pacific subtropical high transported PSEA biomass burning pollutants to the marine boundary layer over the tropical northwestern Pacific. We compared our model results to aircraft measurements over the northwestern Pacific during the TRACE-P campaign (March 2001). The direct injection of 40% of the PSEA biomass burning pollutants in the free troposphere in the model led to a more pronounced BC peak at 3 km over the northwestern Pacific, which was in better agreement with the aircraft observations compared to the control simulation. Our analyses highlighted the point that the injection heights of smoke plumes pose large uncertainty to the interpretation of BC measurements downwind of biomass burning regions.

Description: Influence of surface morphology on the immersion mode ice nucleation efficiency of hematite particles Atmospheric Chemistry and Physics Discussions, 13, 23757-23780, 2013 Author(s): N. Hiranuma, N. Hoffmann, A. Kiselev, A. Dreyer, K. Zhang, G. Kulkarni, T. Koop, and O. Möhler In this paper, the effect of the morphological modification of aerosol particles with respect to heterogeneous ice nucleation is comprehensively investigated for laboratory-generated hematite particles as a model substrate for atmospheric dust particles. The surface area-scaled ice nucleation efficiencies of monodisperse cubic hematite particles and milled hematite particles were measured with a series of expansion cooling experiments using the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud simulation chamber. Complementary off-line characterization of physico-chemical properties of both hematite subsets were also carried out with scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, dynamic light scattering (DLS), and an electro-kinetic particle charge detector to further constrain droplet-freezing measurements of hematite particles. Additionally, an empirical parameterization derived from our laboratory measurements was implemented in the single-column version of the Community Atmospheric Model version 5 (CAM5) to investigate the model sensitivity in simulated ice crystal number concentration on different ice nucleation efficiencies. From an experimental perspective, our results show that the immersion mode ice nucleation efficiency of milled hematite particles is almost an order of magnitude higher at −35.2 °C 〈 T 〈 −33.5 °C than that of the cubic hematite particles, indicating a substantial effect of morphological irregularities on immersion mode freezing. Our modeling results similarly show that the increased droplet-freezing rates of milled hematite particles lead to about one order magnitude higher ice crystal number in the upper troposphere than cubic hematite particles. Overall, our results suggest that the surface irregularities and associated active sites lead to greater ice activation through droplet-freezing.

Description: Study of the unknown HONO daytime source at an European suburban site during the MEGAPOLI summer and winter field campaigns Atmospheric Chemistry and Physics Discussions, 13, 23639-23690, 2013 Author(s): V. Michoud, A. Colomb, A. Borbon, K. Miet, M. Beekmann, M. Camredon, B. Aumont, S. Perrier, P. Zapf, G. Siour, W. Ait-Helal, C. Afif, A. Kukui, M. Furger, J. C. Dupont, M. Haeffelin, and J. F. Doussin Nitrous acid measurements were carried out during the MEGAPOLI summer and winter field campaigns at SIRTA observatory in Paris surroundings. Highly variable HONO levels were observed during the campaigns, ranging from 10 ppt to 500 ppt in summer and from 10 ppt to 1.7 ppb in winter. Significant HONO mixing ratios have also been measured during daytime hours, comprised between some tenth of ppt and 200 ppt for the summer campaign and between few ppt and 1 ppb for the winter campaign. Ancillary measurements, such as NO x , O 3 , photolysis frequencies, meteorological parameters (pressure, temperature, relative humidity, wind speed and wind direction), black carbon concentration, total aerosol surface area, boundary layer height and soil moisture, were conducted during both campaigns. In addition, for the summer period, OH radical measurements were made with a CIMS (Chemical Ionisation Mass Spectrometer). This large dataset has been used to investigate the HONO budget in a suburban environment. To do so, calculations of HONO concentrations using PhotoStationary State (PSS) approach have been performed, for daytime hours. The comparison of these calculations with measured HONO concentrations revealed an underestimation of the calculations making evident a missing source term for both campaigns. This unknown HONO source exhibits a bell shaped like average diurnal profile with a maximum around noon of approximately 0.7 ppb h −1 and 0.25 ppb h −1 , during summer and winter respectively. This source is the main HONO source during daytime hours for both campaigns. In both cases, this source shows a slight positive correlation with J (NO 2 ) and the product between J (NO 2 ) and soil moisture. This original approach had, thus, indicated that this missing source is photolytic and might be heterogeneous occurring on ground surface and involving water content available at the ground.

Description: Proxy-data suggest that the Last Interglacial (LIG; ~130–116 ka BP) climate was characterized by higher temperatures, a partially melted Greenland Ice Sheet (GIS) and a changed Atlantic meridional overturning circulation (AMOC). Notwithstanding the uncertainties in LIG palaeoclimatic reconstructions, this setting potentially provides an opportunity to evaluate the relation between GIS melt and the AMOC as simulated by climate models. However, first we need to assess the extent to which a causal relation between early LIG GIS melt and the weakened AMOC is plausible. With a series of transient LIG climate simulations with the LOVECLIM earth system model, we quantify the importance of the major known uncertainties involved in early LIG GIS melt scenarios. Based on this we construct a specific scenario that is within the parameter space of uncertainties and show that it is physically consistent that early LIG GIS melting kept the AMOC weakened. Notwithstanding, this scenario is at the extreme end of the parameter space. Assuming that proxy-based reconstructions of early LIG AMOC weakening offer a realistic representation of its past state, this indicates that either (1) the AMOC weakening was caused by other forcings than early LIG GIS melt or (2) the early LIG AMOC was less stable than indicated by our simulations and a small amount of GIS melt was sufficient to keep the AMOC in the weak state of a bi-stable regime. We argue that more intensive research is required because of the high potential of the early LIG to evaluate model performance in relation to the AMOC response to GIS melt.

Description: Relationship between Amazon biomass burning aerosols and rainfall over La Plata Basin Atmospheric Chemistry and Physics Discussions, 13, 23995-24021, 2013 Author(s): G. Camponogara, M. A. F. Silva Dias, and G. G. Carrió High aerosol loads are discharged into the atmosphere by biomass burning in Amazon and Central Brazil during the dry season. These particles can interact with clouds as cloud condensation nuclei (CCN) changing cloud microphysics and radiative properties and, thereby, affecting the radiative budget of the region. Furthermore, the biomass burning aerosols can be transported by the low level jet (LLJ) to La Plata Basin where many mesoscale convective systems (MCS) are observed during spring and summer. This work proposes to investigate whether the aerosols from biomass burning may affect the MCS in terms of rainfall over La Plata Basin during spring. Since the aerosol effect is very difficult to isolate because convective clouds are very sensitive to small environment disturbances, detailed analyses using different techniques are used. The binplot, 2D histograms and combined empirical orthogonal function (EOF) methods are used to separate certain environment conditions with the possible effects of aerosol loading. Reanalysis 2, TRMM-3B42 and AERONET data are used from 1999 up to 2012 during September-December. The results show that there are two patterns associated to rainfall-aerosol interaction in La Plata Basin: one in which the dynamic conditions are more important than aerosols to generate rain; and a second one where the aerosol particles have a role in rain formation, acting mainly to suppress rainfall over La Plata Basin.

Description: Size-resolved aerosol composition and link to hygroscopicity at a forested site in Colorado Atmospheric Chemistry and Physics Discussions, 13, 23817-23843, 2013 Author(s): E. J. T. Levin, A. J. Prenni, B. Palm, D. Day, P. Campuzano-Jost, P. M. Winkler, S. M. Kreidenweis, P. J. DeMott, J. Jimenez, and J. N. Smith Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions of non-refractory components were between 70–90%. Corresponding aerosol hygroscopicity was observed to range from κ = 0.15–0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an Aerosol Mass Spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study with an assumed value of κ org = 0.13 resulting in the best agreement.

Description: Atmospheric parameters in a subtropical cloud regime transition derived by AIRS+MODIS – observed statistical variability compared to ERA-Interim Atmospheric Chemistry and Physics Discussions, 13, 24051-24085, 2013 Author(s): M. M. Schreier, B. H. Kahn, K. Sušelj, J. Karlsson, S. C. Ou, Q. Yue, and S. L. Nasiri Cloud occurrence, microphysical and optical properties and atmospheric profiles within a subtropical cloud regime transition in the northeastern Pacific Ocean are obtained from a synergistic combination of the Atmospheric Infrared Sounder (AIRS) and the MODerate resolution Imaging Spectroradiometer (MODIS). The observed cloud parameters and atmospheric thermodynamic profile retrievals are binned by cloud type and analyzed based on their probability density functions (PDFs). Comparison of the PDFs to data from the European Center for Medium Range Weather Forecasting Re-analysis (ERA-Interim) shows a strong difference in the occurrence of the different cloud types compared to clear sky. An increasing non-Gaussian behavior is observed in cloud optical thickness (τ c ), effective radius ( r e ) and cloud top temperature ( T c ) distributions from Stratocumulus to Trade Cumulus, while decreasing values of lower tropospheric stability are seen. However, variations in the mean, width and shape of the distributions are found. The AIRS potential temperature (θ) and water vapor ( q ) profiles in the presence of varying marine boundary layer (MBL) cloud types show overall similarities to the ERA-Interim in the mean profiles, but differences arise in the higher moments at some altitudes. The differences between the PDFs from AIRS+MODIS and ERA-Interim make it possible to pinpoint systematic errors in both systems and helps to understand joint PDFs of cloud properties and coincident thermodynamic profiles from satellite observations.

Description: Establishing the contribution of lawn mowing to atmospheric aerosol levels in American suburbs Atmospheric Chemistry and Physics Discussions, 13, 24435-24480, 2013 Author(s): R. M. Harvey, J. Zahardis, and G. A. Petrucci Green leaf volatiles (GLVs) are a class of wound-induced volatile organic compounds emitted by several plant species. Turfgrasses emit a complex profile of GLVs upon mowing, as evidenced by the "freshly cut grass" smell, some of which are readily oxidized in the atmosphere to contribute to secondary organic aerosol (SOA). The contribution of lawn mowing-induced SOA production may be especially impactful at the urban/suburban interface, where urban hubs provide a source of anthropogenic oxidants and SOA while suburban neighborhoods have the potential to emit large quantities of reactive, mow-induced GLVs. This interface provides a unique opportunity to study aerosol formation in a multi-component system and at a regionally relevant scale. Freshly cut grass was collected from a study site in Essex Junction, Vermont and was placed inside a 775 L Teflon experimental chamber. Thermal desorption gas chromatography mass spectrometry (TD-GC/MS) was used to characterize the emitted GLV profile. Ozone was introduced to the experimental chamber and TD-GC/MS was used to monitor the consumption of these GLVs and the subsequent evolution of gas phase products while a scanning mobility particle sizer was used to continuously measure aerosol size distributions and mass loadings as a result of grass clipping ozonolysis. Freshly cut grass found to emit a complex mixture of GLVs, dominated by cis -3-hexenyl acetate and cis -3-hexenol, which were released at an initial rate of 1.8 (±0.5) μg and 0.07 (±0.03) μg per square meter of lawn mowed with each mowing. Chamber studies using pure standards of cis -3-hexenyl acetate (CHA) and cis -3-hexenol (HXL) were found to have aerosol yields of 1.2 (±1.1)% and 3.3 (±3.1)%, respectively. Using these aerosol yields and the emission rate of these CHA and HXL by grass, SOA evolution by ozonolysis of grass clippings was predicted. However, the measured SOA mass produced from the ozonolysis of grass clippings exceeded the predicted amount, by upwards of ~ 150%. The ozonolysis of a mixture of CHA and HXL representative of environmental mixing ratios also failed to accurately model the SOA mass produced by grass clippings. Aerial photographs and geospatial analysis were used to determine the turfgrass coverage in a suburban neighborhood, which was then used along with measured SOA production as a function of grass mowed to determine that lawn mowing has the potential to contribute 47 μg m −2 SOA to the atmosphere per mowing event by ozonolysis, which cannot be modeled solely by the ozonolysis of CHA, HXL or a representative mixture of the two.

Description: Global distributions and trends of atmospheric ammonia (NH 3 ) from IASI satellite observations Atmospheric Chemistry and Physics Discussions, 13, 24301-24342, 2013 Author(s): M. Van Damme, L. Clarisse, C. L. Heald, D. Hurtmans, Y. Ngadi, C. Clerbaux, A. J. Dolman, J. W. Erisman, and P. F. Coheur Ammonia (NH 3 ) emissions in the atmosphere have strongly increased in the past decades, largely because of the intensive livestock production and use of fertilizers. As a short-lived species, NH 3 is highly variable in the atmosphere and its concentration is generally small, except in and close to local source areas. While ground-based measurements are possible, they are challenging and sparse. Advanced infrared sounders in orbit have recently demonstrated their capability to measure NH 3 , offering a new tool to refine global and regional budgets. In this paper we describe an improved retrieval scheme of NH 3 total columns from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI). It exploits the hyperspectral character of this instrument by using an extended spectral range (800–1200 cm −1 ) where NH 3 is optically active. This scheme consists of the calculation of a dimensionless spectral index from the IASI level1C radiances, which is subsequently converted to a total NH 3 column using look-up-tables built from forward radiative transfer model simulations. We show how to retrieve the NH 3 total columns from IASI quasi-globally and twice daily, above both land and sea, without large computational resources and with an improved detection limit. The retrieval also provides error characterization on the retrieved columns. Five years of IASI measurements (1 November 2007 to 31 October 2012) have been processed to acquire the first global and multiple-year dataset of NH 3 total columns, which are evaluated and compared to similar products from other retrieval methods. Spatial distributions from the five years dataset are provided and analyzed at global and regional scales. We show in particular the ability of this method to identify smaller emission sources than those reported previously, as well as transport patterns above sea. The five year time series is further examined in terms of seasonality and inter-annual variability (in particular as a function of fire activity) separately for the Northern and Southern Hemispheres.

Description: We measured the annual variation in the stable isotopes of oxygen (δ 18 O) and hydrogen (δD) in tree rings of Abies georgei on the Batang–Litang Plateau of western China. Although correlations between tree-ring δ 18 O and δD are relatively weak in semi-arid regions, we found a strong correlation between the δ 18 O and δD time series from 1755 to 2009 under the wetter environment. Tree-ring δ 18 O and δD time series are both significantly and negatively correlated with moisture conditions from June to August, including relative humidity and total precipitation, respectively, from 1960 to 2009. Considering the difference in low-frequency domain between the two isotopes, the relative humidity histories from June to August, reconstructed separately from the tree-ring δ 18 O and δD data with instrumental climate data, reveal a persistent drying trend since 1850s, especially since the early 1970s. There is an obvious offset of reconstructed relative humidity from tree-ring δ 18 O and δD in the period 1755–1820, despite the strong similarity in their 21-year moving averages. The decreased relative humidity since the 1850s may be associated with the thermal contrast between the sea surface temperature of the Indian Ocean and the Qinghai-Tibetan Plateau, which determines the strength of moisture transfer via the Indian summer monsoon.

Description: Aircraft measurements of polar organic tracer compounds in tropospheric particles (PM 10 ) over Central China Atmospheric Chemistry and Physics Discussions, 13, 24481-24516, 2013 Author(s): P. Q. Fu, K. Kawamura, Y. F. Cheng, S. Hatakeyama, A. Takami, H. Li, and W. Wang Atmospheric aerosol samples were collected by aircraft at low to middle altitudes (0.8–3.5 km a.g.l.) over Central East to West China during summer 2003 and spring 2004. The samples were analyzed for polar organic compounds using a technique of solvent extraction/BSTFA derivatization/gas chromatography-mass spectrometry. Biogenic secondary organic aerosol (SOA) tracers from the oxidation of isoprene were found to be more abundant in summer (3.3–138 ng m −3 , mean 39 ng m −3 ) than in spring (3.2–42 ng m −3 , 15 ng m −3 ), while α/β-pinene and β-caryophyllene SOA tracers showed similar abundance between these two seasons. A strong positive correlation ( R 2 =0.83) between levoglucosan and β-caryophyllinic acid was found in the spring samples versus a weak correlation ( R 2 =0.17) in the summer samples, implying substantial contributions from biomass burning to the β-caryophyllinic acid production in spring. Two organic nitrogen species (oxamic acid and carbamide) were detected in the aircraft aerosol samples and their concentrations were comparable to those of biogenic SOA tracers. Most of the POA and SOA tracers were less abundant at higher altitudes, suggesting they are of ground surface origin, either being directly emitted from anthropogenic/natural sources on the ground surface, or rapidly formed through photooxidation of their precursors emitted from the ground surface and then diluted during uplifting into the troposphere. This study demonstrates that primary biological aerosols, biogenic SOA, and organic nitrogen species are important components of organic aerosols in the troposphere over Central China.

Description: Observations show a multidecadal signal in the North Atlantic ocean, but the underlying mechanism and cause of its timescale remain unknown. Previous studies have suggested that it may be driven by the North Atlantic Oscillation (NAO), which is the dominant pattern of winter atmospheric variability. To further address this issue, the global ocean general circulation model, Nucleus for European Modelling of the Ocean (NEMO), is driven using a 2,000 years long white noise forcing associated with the NAO. Focusing on key ocean circulation patterns, we show that the Atlantic Meridional Overturning Circulation (AMOC) and Sub-polar gyre (SPG) strength both have enhanced power at low frequencies but no dominant timescale, and thus provide no evidence for a oscillatory ocean-only mode of variability. Instead, both indices respond linearly to the NAO forcing, but with different response times. The variability of the AMOC at 30°N is strongly enhanced on timescales longer than 90 years, while that of the SPG strength starts increasing at 15 years. The different response characteristics are confirmed by constructing simple statistical models that show AMOC and SPG variability can be related to the NAO variability of the previous 53 and 10 winters, respectively. Alternatively, the AMOC and the SPG strength can be reconstructed with Auto-regressive (AR) models of order seven and five, respectively. Both statistical models reconstruct interannual and multidecadal AMOC variability well, while on the other hand, the AR(5) reconstruction of the SPG strength only captures multidecadal variability. Using these methods to reconstruct ocean variables can be useful for prediction and model intercomparision.

Description: Driving data and physical parametrizations can significantly impact the performance of regional dynamical atmospheric models in reproducing hydrometeorologically relevant variables. Our study addresses the water budget sensitivity of the Weather Research and Forecasting Model System WRF (WRF-ARW) with respect to two cumulus parametrizations (Kain–Fritsch, Betts–Miller–Janjić), two global driving reanalyses (ECMWF ERA-INTERIM and NCAR/NCEP NNRP), time variant and invariant sea surface temperature and optional gridded nudging. The skill of global and downscaled models is evaluated against different gridded observations for precipitation, 2 m-temperature, evapotranspiration, and against measured discharge time-series on a monthly basis. Multi-year spatial deviation patterns and basin aggregated time series are examined for four globally distributed regions with different climatic characteristics: Siberia, Northern and Western Africa, the Central Australian Plane, and the Amazonian tropics. The simulations cover the period from 2003 to 2006 with a horizontal mesh of 30 km. The results suggest a high sensitivity of the physical parametrizations and the driving data on the water budgets of the regional atmospheric simulations. While the global reanalyses tend to underestimate 2 m-temperature by 0.2–2 K, the regional simulations are typically 0.5–3 K warmer than observed. Many configurations show difficulties in reproducing the water budget terms, e.g. with long-term mean precipitation biases of 150 mm month −1 and higher. Nevertheless, with the water budget analysis viable setups can be deduced for all four study regions.

Description: Black carbon emissions from in-use ships: a California regional assessment Atmospheric Chemistry and Physics Discussions, 13, 24675-24712, 2013 Author(s): G. M. Buffaloe, D. A. Lack, E. J. Williams, D. Coffman, K. L. Hayden, B. M. Lerner, S-M. Li, I. Nuaaman, P. Massoli, T. B. Onasch, P. K. Quinn, and C. D. Cappa Black carbon (BC) mass emission factors (EF BC ; g-BC (kg-fuel) −1 ) from a variety of ocean going vessels have been determined from measurements of BC and carbon dioxide (CO 2 ) concentrations in ship plumes intercepted by the R/V Atlantis during the 2010 California Nexus (CalNex) campaign. The ships encountered were all operating within 24 nautical miles of the California coast and were utilizing relatively low sulphur fuels. Black carbon concentrations within the plumes, from which EF BC values are determined, were measured using four independent instruments: a photoacoustic spectrometer and a particle soot absorption photometer, which measure light absorption, and a single particle soot photometer and soot particle aerosol mass spectrometer, which measure the mass concentration of refractory BC directly. The measured EF BC have been divided into vessel type categories and engine type categories, from which averages have been determined. The geometric average EF BC , determined from over 71 vessels and 135 plumes encountered, was 0.31 g-BC (kg-fuel) −1 . The most frequent engine type encountered was the slow speed diesel (SSD), and the most frequent SSD vessel type was the cargo ship sub-category. Average and median EF BC values from the SSD category are compared with previous observations from the Texas Air Quality Study (TexAQS) in 2006, during which the ships encountered were predominately operating on high sulphur fuels. There is a statistically significant difference between the EF BC values from CalNex and TexAQS for SSD vessels and for the cargo and tanker ship types within this engine category. The CalNex EF BC values are lower than those from TexAQS, suggesting that operation on lower sulphur fuels is associated with smaller EF BC values.

Description: A case study into the measurement of ship emissions from plume intercepts of the NOAA Ship Miller Freeman Atmospheric Chemistry and Physics Discussions, 13, 24635-24674, 2013 Author(s): C. D. Cappa, E. J. Williams, D. A. Lack, G. M. Buffaloe, D. Coffman, K. L. Hayden, S. C. Herndon, B. M. Lerner, S-M. Li, P. Massoli, R. McLaren, I. Nuaaman, T. B. Onasch, and P. K. Quinn Emissions factors (EFs) for gas and sub-micron particle-phase species were measured in intercepted plumes as a function of vessel speed from an underway research vessel, the NOAA Ship Miller Freeman , operating a medium-speed diesel engine on low-sulfur marine gas oil. For many of the particle-phase species, EFs were determined using multiple measurement methodologies, allowing for an assessment of how well EFs from different techniques agree. The total sub-micron PM (PM 1 ) was dominated by particulate black carbon (BC) and particulate organic matter (POM), with an average POM / BC ratio of 1.3. Consideration of the POM / BC ratios observed here with literature studies suggests that laboratory and in-stack measurement methods may over-estimate primary POM EFs relative to those observed in emitted plumes. Comparison of four different methods for black carbon measurement indicates that careful attention must be paid to instrument limitations and biases when assessing EF BC . Particulate sulfate (SO 4 2− ) EFs were extremely small and the particles emitted by Miller Freeman were inefficient as cloud condensation nuclei (CCN), even at high super saturations, consistent with the use of very low sulfur fuel and the overall small emitted particle sizes. All measurement methodologies consistently demonstrate that the measured EFs (fuel mass basis) for PM 1 mass, BC and POM decreased as the ship slowed. Particle number EFs were approximately constant across the speed change, with a shift towards smaller particles being emitted at slower speeds. Emissions factors for gas-phase CO and formaldehyde (HCHO) both increased as the vessel slowed, while EFs for NO x decreased and SO 2 EFs were approximately constant.

Description: Heterogeneous reaction of N 2 O 5 with illite and Arizona Test Dust particles Atmospheric Chemistry and Physics Discussions, 13, 24855-24884, 2013 Author(s): M. J. Tang, G. Schuster, and J. N. Crowley The heterogeneous reaction of N 2 O 5 with airborne illite and Arizona Test Dust particles was investigated at room temperature and at different relative humidities using an atmospheric pressure aerosol flow tube. N 2 O 5 at concentrations in the range 8 to 24×10 12 molecule cm −3 was monitored using thermal-dissociation cavity ring-down spectroscopy at 662 nm. At zero relative humidity a large uptake coefficient of N 2 O 5 to illite was obtained, γ(N 2 O 5 ) = 0.09, which decreased to 0.04 as relative humidity was increased to 67%. In contrast, the uptake coefficient derived for ATD is much lower (~ 0.006) and, within experimental uncertainty, independent of relative humidity (0–67%). Potential explanations are given for the significant differences between the uptake behaviour for ATD and illite and the results are compared with uptake coefficients for N 2 O 5 on other mineral surfaces.

Description: A case study of sea breeze blocking regulated by sea surface temperature along the English south coast Atmospheric Chemistry and Physics Discussions, 13, 24785-24807, 2013 Author(s): J. K. Sweeney, J. M. Chagnon, and S. L. Gray The sensitivity of sea breeze structure to sea surface temperature (SST) and coastal orography is investigated in convection-permitting Met Office Unified Model simulations of a case study along the south coast of England. Changes in SST of 1 K are shown to significantly modify the structure of the sea breeze. On the day of the case study the sea breeze was partially blocked by coastal orography, particularly within Lyme Bay. The extent to which the flow is blocked depends strongly on the static stability of the marine boundary layer. In experiments with colder SST, the marine boundary layer is more stable, and the degree of blocking is more pronounced. The implications of prescribing fixed SST from climatology in numerical weather prediction model forecasts of the sea breeze are discussed.

Description: Using a WRF simulation to examine regions where convection impacts the Asian summer monsoon anticyclone Atmospheric Chemistry and Physics Discussions, 13, 24809-24853, 2013 Author(s): N. K. Heath and H. E. Fuelberg The Asian summer monsoon is a prominent feature of the global circulation that is associated with an upper-level anticyclone (ULAC) that stands out vividly in satellite observations of trace gases. The ULAC also is an important region of troposphere-to-stratosphere transport. We ran the Weather Research and Forecasting (WRF) model at convective-permitting scales (4 km grid spacing) between 10–20 August 2012 to understand the role of convection in transporting boundary layer air into the upper-level anticyclone. Such high-resolution modeling of the Asian ULAC previously has not been documented in the literature. Comparison of our WRF simulation with reanalysis and satellite observations showed that WRF simulated the atmosphere sufficiently well to be used to study convective transport into the ULAC. A back-trajectory analysis based on hourly WRF output showed that 〉 90% of convectively influenced parcels reaching the ULAC came from the Tibetan Plateau (TP) and the southern slope (SS) of the Himalayas. A distinct diurnal cycle is seen in the convective trajectories, with their greatest impact occurring between 1600–2300 local solar time. This finding highlights the role of "everyday" diurnal convection in transporting boundary layer air into the ULAC. WRF output at 15 min intervals was produced for 16 August to examine the convection in greater detail. This high-temporal output revealed that the weakest convection in the study area occurred over the TP. However, because the TP is at 3000–5000 m a.m.s.l., its convection does not have to be as strong to reach the ULAC as in lower altitude regions. In addition, because the TP's elevated heat source is a major cause of the ULAC, we propose that convection over the TP and the neighboring SS is ideally situated geographically to impact the ULAC. The vertical mass flux of water vapor into the ULAC also was calculated. Results show that the TP and SS regions dominate other Asian regions in transporting moisture vertically into the ULAC. Because convection reaching the ULAC is more widespread over the TP than nearby, we propose that the abundant convection partially explains the TP's dominant water vapor fluxes. In addition, greater outgoing longwave radiation reaches the upper levels of the TP due to its elevated terrain. This creates a warmer ambient upper level environment, allowing parcels with greater saturation mixing ratios to enter the ULAC. Lakes in the Tibetan Plateau are shown to provide favorable conditions for deep convection during the night.

Description: El Niño/Southern Oscillation (ENSO) is the predominant interannual variability of the global climate system. How might ENSO change in a warmer world? The dominant two Combined Empirical Orthogonal Functions (CEOF) of the equatorial ocean temperature and zonal and vertical motion identify two modes that shown a transition in the eastern Pacific from a warming eastward/downward motion to a cooling westward/upward flow. These results also suggest consistent changes to the west and at depths down to 300 m. These dominate CEOFs provide a compact tool for assessing Coupled Model Intercomparison Project Phase 5 ocean model output for both the recent historical period and for the latter part of the twenty first century. Most of the analyzed models replicate well the spatial patterns of the dominant observational CEOF modes, but nearly always underestimate the magnitudes. Comparing model output for the twentieth and twenty first centuries there is very little change between the spatial patterns of the ENSO modes of the two periods. This lack of response to climate change is shown to be partly related to competing influences of climatic changes in the mean ocean circulation.

Description: In this work, authors examine the variabilities of precipitation and surface air temperature (T2m) in Northeast China during 1948–2012, and their global connection, as well as the predictability. It is noted that both the precipitation and T2m variations in Northeast China are dominated by interannual and higher frequency variations. However, on interdecadal time scales, T2m is shifted significantly from below normal to above normal around 1987/1988. Statistically, the seasonal mean precipitation and T2m are largely driven by local internal atmospheric variability rather than remote forcing. For the precipitation variation, circulation anomalies in the low latitudes play a more important role in spring and summer than in autumn and winter. For T2m variations, the associated sea surface pressure (SLP) and 850-hPa wind (uv850) anomalies are similar for all seasons in high latitudes with significantly negative correlations for SLP and westerly wind anomaly for uv850, suggesting that a strong zonal circulation in the high latitudes favors warming in Northeast China. The predictability of precipitation and T2m in Northeast China is assessed by using the Atmospheric Model Inter-comparison Project type experiments which are forced by observed sea surface temperature (SST) and time-evolving greenhouse gas (GHG) concentrations. Results suggest that T2m has slightly higher predictability than precipitation in Northeast China. To some extent, the model simulates the interdecadal shift of T2m around 1987/1988, implying a possible connection between SST (and/or GHG forcing) and surface air temperature variation in Northeast China on interdecadal time scales. Nevertheless, the precipitation and T2m variations are mainly determined by the unpredictable components which are caused by the atmospheric internal dynamic processes, suggesting low predictability for the climate variation in Northeast China.

Description: A land–sea surface warming ratio (or φ ) that exceeds unity is a robust feature of both observed and modelled climate change. Interestingly, though climate models have differing values for φ , it remains almost time-invariant for a wide range of twenty-first century climate transient warming scenarios, while varying in simulations of the twentieth century. Here, we present an explanation for time-invariant land–sea warming ratio that applies if three conditions on radiative forcing are met: first, spatial variations in the climate forcing must be sufficiently small that the lower free troposphere warms evenly over land and ocean; second, the temperature response must not be large enough to change the global circulation to zeroth order; third, the temperature response must not be large enough to modify the boundary layer amplification mechanisms that contribute to making φ exceed unity. Projected temperature changes over this century are too small to breach the latter two conditions. Hence, the mechanism appears to show why both twenty-first century and time-invariant CO 2 forcing lead to similar values of φ in climate models despite the presence of transient ocean heat uptake, whereas twentieth century forcing—which has a significant spatially confined anthropogenic tropospheric aerosol component that breaches the first condition—leads to modelled values of φ that vary widely amongst models and in time. Our results suggest an explanation for the behaviour of φ when climate is forced by other regionally confined forcing scenarios such as geo-engineered changes to oceanic clouds. Our results show how land–sea contrasts in surface and boundary layer characteristics act in tandem to produce the land–sea surface warming contrast.

Description: We present a validation analysis of a regional climate model coupled to a distributed one dimensional (1D) lake model for the Caspian Sea Basin. Two model grid spacings are tested, 50 and 20 km, the simulation period is 1989–2008 and the lateral boundary conditions are from the ERA-Interim reanalysis of observations. The model is validated against atmospheric as well as lake variables. The model performance in reproducing precipitation and temperature mean seasonal climatology, seasonal cycles and interannual variability is generally good, with the model results being mostly within the observational uncertainty range. The model appears to overestimate cloudiness and underestimate surface radiation, although a large observational uncertainty is found in these variables. The 1D distributed lake model (run at each grid point of the lake area) reproduces the observed lake-average sea surface temperature (SST), although differences compared to observations are found in the spatial structure of the SST, most likely as a result of the absence of 3 dimensional lake water circulations. The evolution of lake ice cover and near surface wind over the lake area is also reproduced by the model reasonably well. Improvements resulting from the increase of resolution from 50 to 20 km are most significant in the lake model. Overall the performance of the coupled regional climate—1D lake model system appears to be of sufficient quality for application to climate change scenario simulations over the Caspian Sea Basin.

Description: Climate changes over China from the present (1990–1999) to future (2046–2055) under the A1FI (fossil fuel intensive) and A1B (balanced) emission scenarios are projected using the Regional Climate Model version 3 (RegCM3) nests with the National Center for Atmospheric Research (NCAR) Community Climate System Model (CCSM). For the present climate, RegCM3 downscaling corrects several major deficiencies in the driving CCSM, especially the wet and cold biases over the Sichuan Basin. As compared with CCSM, RegCM3 produces systematic higher spatial pattern correlation coefficients with observations for precipitation and surface air temperature except during winter. The projected future precipitation changes differ largely between CCSM and RegCM3, with strong regional and seasonal dependence. The RegCM3 downscaling produces larger regional precipitation trends (both decreases and increases) than the driving CCSM. Contrast to substantial trend differences projected by CCSM, RegCM3 produces similar precipitation spatial patterns under different scenarios except autumn. Surface air temperature is projected to consistently increase by both CCSM and RegCM3, with greater warming under A1FI than A1B. The result demonstrates that different scenarios can induce large uncertainties even with the same RCM-GCM nesting system. Largest temperature increases are projected in the Tibetan Plateau during winter and high-latitude areas in the northern China during summer under both scenarios. This indicates that high elevation and northern regions are more vulnerable to climate change. Notable discrepancies for precipitation and surface air temperature simulated by RegCM3 with the driving conditions of CCSM versus the model for interdisciplinary research on climate under the same A1B scenario further complicated the uncertainty issue. The geographic distributions for precipitation difference among various simulations are very similar between the present and future climate with very high spatial pattern correlation coefficients. The result suggests that the model present climate biases are systematically propagate into the future climate projections. The impacts of the model present biases on projected future trends are, however, highly nonlinear and regional specific, and thus cannot be simply removed by a linear method. A model with more realistic present climate simulations is anticipated to yield future climate projections with higher credibility.

Description: Teleconnections associated with warm El Niño/southern oscillation (ENSO) events in 20 climate model intercomparison project 5 (CMIP5) models have been compared with reanalysis observations. Focus has been placed on compact time and space indices, which can be assigned a specific statistical confidence. Nearly all of the models have surface temperature, precipitation and 250 hPa geopotential height departures in the Tropics that are in good agreement with the observations. Most of the models also have realistic anomalies of Northern Hemisphere near-surface temperature, precipitation and 500 hPa geopotential height. Model skill for these variables is significantly related to the ability of a model to accurately simulate Tropical 250 hPa height departures. Additionally, most models have realistic temperature and precipitation anomalies over North America, which are linked to a model’s ability to simulate Tropical 250 hPa and Northern Hemisphere 500 hPa height departures. The skills of temperature and precipitation departures over the Northern Hemisphere and North America are associated with the ability to realistically simulate realistic ENSO frequency and length. Neither horizontal nor vertical resolution differences for either the model atmosphere or ocean are significantly related at the 95 % level to variations in El Niño simulation quality. Overall, recent versions of earlier models have improved in their ability to simulate El Niño teleconnections. For instance, the average model skills of temperature and precipitation for the Tropics, Northern Hemisphere and North America for 11 CMIP5 models are all larger than those for prior versions.

Description: In the eastern Mediterranean in general and in Turkey in particular, temperature reconstructions based on tree rings have not been achieved so far. Furthermore, centennial-long chronologies of stable isotopes are generally also missing. Recent studies have identified the tree species Juniperus excelsa as one of the most promising tree species in Turkey for developing long climate sensitive stable carbon isotope chronologies because this species is long-living and thus has the ability to capture low-frequency climate signals. We were able to develop a statistically robust, precisely dated and annually resolved chronology back to AD 1125. We proved that variability of δ 13 C in tree rings of J. excelsa is mainly dependent on winter-to-spring temperatures (January–May). Low-frequency trends, which were associated with the medieval warm period and the little ice age, were identified in the winter-to-spring temperature reconstruction, however, the twentieth century warming trend found elsewhere could not be identified in our proxy record, nor was it found in the corresponding meteorological data used for our study. Comparisons with other northern-hemispherical proxy data showed that similar low-frequency signals are present until the beginning of the twentieth century when the other proxies derived from further north indicate a significant warming while the winter-to-spring temperature proxy from SW-Turkey does not. Correlation analyses including our temperature reconstruction and seven well-known climate indices suggest that various atmospheric oscillation patterns are capable of influencing the temperature variations in SW-Turkey.

Description: The latest version of the state-of-the-art global land–atmosphere–ocean coupled climate forecast system of NCEP has shown considerable improvement in various aspects of the Indian summer monsoon. However, climatological mean dry bias over the Indian sub-continent is further increased as compared to the previous version. Here we have attempted to link this dry bias with climatological mean bias in the Eurasian winter/spring snow, which is one of the important predictors of the Indian summer monsoon rainfall (ISMR). Simulation of interannual variability of the Eurasian snow and its teleconnection with the ISMR are quite reasonable in the model. Using composite analysis it is shown that a positive snow anomaly, which is comparable to the systematic bias in the model, results into significant decrease in the summer monsoon rainfall over the central India and part of the Equatorial Indian Ocean. Decrease in the summer monsoon rainfall is also found to be linked with weaker northward propagation of intraseasonal oscillation (ISO). A barotropic stationary wave triggered by positive snow anomaly over west Eurasia weakens the upper level monsoon circulation, which in turn reduces the zonal wind shear and hence, weakens the northward propagation of summer monsoon ISOs. A sensitivity experiment by reducing snow fall over Eurasian region causes decrease in winter and spring snow depth, which in turn leads to decrease in Indian summer monsoon rainfall. Results from the sensitivity experiment corroborate with those of composite analysis based on long free run. This study suggests that further improvements in the snow parametrization schemes as well as Arctic sea ice are needed to reduce the Eurasian snow bias during winter/spring, which may reduce the dry bias over Indian sub-continent and hence predictability aspect of the model.

Description: An assessment of the performance of the Monitor for AeRosols and GAses in ambient air (MARGA): a semi-continuous method for soluble compounds Atmospheric Chemistry and Physics Discussions, 13, 25067-25124, 2013 Author(s): I. C. Rumsey, K. A. Cowen, J. T. Walker, T. J. Kelly, E. A. Hanft, K. Mishoe, C. Rogers, R. Proost, G. M. Beachley, G. Lear, T. Frelink, and R. P. Otjes Ambient air monitoring as part of the US Environmental Protection Agency's (US EPA's) Clean Air Status and Trends Network (CASTNet) currently uses filter packs to measure weekly integrated concentrations. The US EPA is interested in supplementing CASTNet with semi-continuous monitoring systems at select sites to characterize atmospheric chemistry and deposition of nitrogen and sulfur compounds at higher time resolution than the filter pack. The Monitor for AeRosols and GAses in ambient air (MARGA) measures water-soluble gases and aerosols at hourly temporal resolution. The performance of the MARGA was assessed under the US EPA Environmental Technology Verification (ETV) program. The assessment was conducted in Research Triangle Park, North Carolina from 8 September–8 October 2010 and focused on gaseous SO 2 , HNO 3 and NH 3 and aerosol SO 4 − , NO 3 − and NH 4 + . Precision of the MARGA was evaluated by calculating the median absolute relative percent difference (MARPD) between paired hourly results from duplicate MARGA units (MUs), with a performance goal of

Description: We examine the influence of the South-American land-mass and its mountains on the significant cyclic diurnal and semidiurnal components of the average circulation in the adjacent area of the southeastern tropical Pacific (SEP). Our approach is based on a number of numerical simulations with the regional atmospheric model weather research and forecasting forced by the National Centers for Environmental Prediction’s final analysis operational analysis data. In the control simulation the model domain covers the SEP and a large part of South America. In several sensitivity experiments the domain is reduced to progressively exclude continental areas. We find that the mean diurnal cycle is sensitive to model domain in ways that reveal the existence of different contributions originating from the Chilean and Peruvian land-masses. The experiments suggest that diurnal variations in circulations and thermal structures over the SEP (mainly forced by local insolation) are influenced by convection over the Peruvian sector of the Andes cordillera, while the mostly dry mountain-breeze circulations force an additional component that results in semi-diurnal variations near the coast. A series of numerical tests, however, reveal sensitivity of the simulations to the choice of vertical grid, limiting the possibility of solid quantitative statements on the amplitudes and phases of the diurnal and semidiurnal components across the domain.

Description: Sensitivity of simulated climate to latitudinal distribution of solar insolation reduction in SRM geoengineering methods Atmospheric Chemistry and Physics Discussions, 13, 25387-25415, 2013 Author(s): A. Modak and G. Bala Solar radiation management (SRM) geoengineering has been proposed as a potential option to counteract climate change. We perform a set of idealized geoengineering simulations to understand the global hydrological implications of varying the latitudinal distribution of solar insolation reduction in SRM methods. We find that for a fixed total mass of sulfate aerosols (12.6 Mt of SO 4 ), relative to a uniform distribution which mitigates changes in global mean temperature, global mean radiative forcing is larger when aerosol concentration is maximum at the poles leading to a warmer global mean climate and consequently an intensified hydrological cycle. Opposite changes are simulated when aerosol concentration is maximized in the tropics. We obtain a range of 1 K in global mean temperature and 3% in precipitation changes by varying the distribution pattern: this range is about 50% of the climate change from a doubling of CO 2 . Hence, our study demonstrates that a range of global mean climate states, determined by the global mean radiative forcing, are possible for a fixed total amount of aerosols but with differing latitudinal distribution, highlighting the need for a careful evaluation of SRM proposals.

Description: Source apportionment of PM 10 in a North-Western Europe regional urban background site (Lens, France) using Positive Matrix Factorization and including primary biogenic emissions Atmospheric Chemistry and Physics Discussions, 13, 25325-25385, 2013 Author(s): A. Waked, O. Favez, L. Y. Alleman, C. Piot, J.-E. Petit, T. Delaunay, E. Verlinden, B. Golly, J.-L. Besombes, J.-L. Jaffrezo, and E. Leoz-Garziandia In this work, the source of ambient particulate matter (PM 10 ) collected over a one year period at an urban background site in Lens (France) were determined and investigated using a~Positive Matrix Factorization receptor model (US EPA PMF v3.0). In addition, a Potential Source Contribution Function (PSCF) was performed by means of the Hysplit v4.9 model to assess prevailing geographical origins of the identified sources. A selective iteration process was followed for the qualification of the more robust and meaningful PMF solution. Components measured and used in the PMF include inorganic and organic species: soluble ionic species, trace elements, elemental carbon (EC), sugars alcohols, sugar anhydride, and organic carbon (OC). The mean PM 10 concentration measured from March 2011 to March 2012 was about 21 μg m −3 with typically OM, nitrate and sulfate contributing to most of the mass and accounting respectively for 5.8, 4.5 and 2.3 μg m −3 on a yearly basis. Accordingly, PMF outputs showed that the main emission sources were (in a decreasing order of contribution): secondary inorganic aerosols (28% of the total PM 10 mass), aged marine emissions (19%), with probably predominant contribution of shipping activities, biomass burning (13%), mineral dust (13%), primary biogenic emissions (9%), fresh sea salts (8%), primary traffic emissions (6%) and heavy oil combustion (4%). Significant temporal variations were observed for most of the identified sources. In particular, biomass burning emissions were negligible in summer but responsible for about 25% of total PM 10 and 50% of total OC at wintertime. Conversely, primary biogenic emissions were found to be negligible in winter but to represent about 20% of total PM 10 and 40% of total OC in summer. The latter result calls for more investigations of primary biogenic aerosols using source apportionment studies, which quite usually disregards this type of sources. This study furthermore underlines the major influence of secondary processes during daily threshold exceedances. Finally, apparent discrepancies that could be generally observed between filter-based studies (such as the present one) and Aerosol Mass Spectrometer-based PMF analyses (organic fractions) are also discussed here.

Description: Wind extraction potential from 4D-Var assimilation of O 3 , N 2 O, and H 2 O using a global shallow water model Atmospheric Chemistry and Physics Discussions, 13, 25291-25323, 2013 Author(s): D. R. Allen, K. W. Hoppel, and D. D. Kuhl The wind extraction due to assimilation of trace gas (tracer) data is examined using a 4D-Var data assimilation system based on the shallow water equations coupled to the tracer continuity equation. The procedure is outlined as follows. First, a Nature Run is created, simulating middle stratospheric winter conditions. Second, ozone (O 3 ), nitrous oxide (N 2 O), and water vapor (H 2 O) (treated in this study as passive tracers) are initialized using Microwave Limb Sounder (MLS) mixing ratios at 850 K potential temperature and advected by the Nature Run winds. Third, the initial dynamical conditions are perturbed by using a 6 h offset. Fourth, observations based on the simulated tracer data are then assimilated with a 4D-Var system in which the tracer and winds are coupled via the adjoint of the tracer continuity equation. Finally, the wind extraction potential (WEP) is calculated as the reduction of the Root Mean Square (RMS) vector wind error due to tracer assimilation relative to the total possible reduction from the initial perturbed conditions. For a single 6 h assimilation cycle of "perfect" tracer (unbiased and no imposed random errors), WEP values are 70% for O 3 , 49% for N 2 O and 16% for H 2 O. O 3 and N 2 O provide more wind information than H 2 O due to stronger background gradients relative to the tracer precisions. 10 day multi-cycle simulations with "perfect" tracer result in WEP of 98% for O 3 , 97% for N 2 O, and 90% for H 2 O. There is therefore sufficient information in these fields to nearly completely specify the dynamics, even without assimilation of dynamical information. For assimilation of tracer observations with realistic random noise (based on MLS precision at 10 hPa), the WEP after 10 days decreases to 57% for O 3 , 42% for N 2 O, and 28% for H 2 O. The root-mean-square (RMS) wind errors level out at ~ 1–2 m s −1 for these runs, suggesting a limit to which realistic tracers could constrain the winds, given complete global coverage. With higher observation noise levels, the WEP values decrease further, with negative WEP occurring in cases of very large errors for H 2 O, indicating that assimilation of very noisy observations may worsen the wind fields.

Description: The simulations of sulfuric acid concentration and new particle formation in an urban atmosphere in China Atmospheric Chemistry and Physics Discussions, 13, 14977-15005, 2013 Author(s): Z. B. Wang, M. Hu, D. Mogensen, D. L. Yue, J. Zheng, R. Y. Zhang, Y. Liu, B. Yuan, X. Li, M. Shao, L. Zhou, Z. J. Wu, A. Wiedensohler, and M. Boy Simulations of sulfuric acid concentration and new particle formation are performed by using the zero-dimensional version of the model MALTE (Model to predict new Aerosol formation in the Lower TropospherE) and measurements from the Campaign of Air Quality Research in Beijing and Surrounding areas (CAREBeijing) in 2008. Chemical reactions from the Master Chemical Mechanism Version 3.2 (MCM v3.2) are used in the model. High correlation (slope = 0.72, R = 0.74) between the modelled and observed sulfuric acid concentrations is found during daytime (06:00–18:00). The aerosol dynamics are simulated by the University of Helsinki Multicomponent Aerosol (UHMA) model including several nucleation mechanisms. The results indicate that the model is able to predict the on- and offset of new particle formation in an urban atmosphere in China. In addition, the number concentrations of newly formed particles in kinetic-type nucleation including homogenous homomolecular ( J=K [H 2 SO 4 ] 2 ) and homogenous heteromolecular nucleation involving organic vapours ( J=K het [H 2 SO 4 ][Org]) are in satisfactory agreement with the observations. However, the specific organic compounds possibly participate in the nucleation process should be investigated in further studies.

Description: Reductions in aircraft particulate emissions due to the use of Fischer–Tropsch fuels Atmospheric Chemistry and Physics Discussions, 13, 15105-15139, 2013 Author(s): A. J. Beyersdorf, M. T. Timko, L. D. Ziemba, D. Bulzan, E. Corporan, S. C. Herndon, R. Howard, R. Miake-Lye, K. L. Thornhill, E. Winstead, C. Wey, Z. Yu, and B. E. Anderson The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January–February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer–Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions of 84% averaged over all powers) and blended fuels (64%) relative to the JP-8 baseline with the largest reductions at idle conditions. The alternative fuels also produced smaller soot (e.g. at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30–44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near-zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (−4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to −1.2 × 10 6 # (kg fuel) −1 °C −1 for particle number emissions and −9.7 mm 3 (kg fuel) −1 °C −1 for particle volume emissions. The temperature dependence of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols with a smaller fraction as a soot coating. Conversion efficiencies of up to 3.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO 2 ) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.

Description: Undisturbed and disturbed above canopy ponderosa pine emissions: PTR-TOF-MS measurements and MEGAN 2.1 model results Atmospheric Chemistry and Physics Discussions, 13, 15333-15375, 2013 Author(s): L. Kaser, T. Karl, A. Guenther, M. Graus, R. Schnitzhofer, A. Turnipseed, L. Fischer, P. Harley, M. Madronich, D. Gochis, F. N. Keutsch, and A. Hansel We present the first eddy covariance flux measurements of volatile organic compounds (VOCs) using a proton-transfer-reaction time-of-flight mass-spectrometer (PTR-TOF-MS) above a ponderosa pine forest in Colorado, USA. The high mass resolution of the PTR-TOF-MS enabled the identification of chemical sum formulas. During a 30 day measurement period in August and September 2010, 649 different ion mass peaks were detected in the ambient air mass spectrum (including primary ions and mass calibration compounds). Eddy covariance with the vertical wind speed was calculated for all ion mass peaks. On a typical day, 17 ion mass peaks including protonated parent compounds, their fragments and isotopes as well as VOC-H + -water clusters showed a significant flux with daytime average emissions above a reliable flux threshold of 0.1 mg compound m −2 h −1 . These ion mass peaks could be assigned to seven compound classes. The main flux contributions during daytime (10:00–18:00 LT) are attributed to the sum of 2-methyl-3-buten-2-ol (MBO) and isoprene (50%), methanol (12%), the sum of acetic acid and glycolaldehyde (10%) and the sum of monoterpenes (10%). The total MBO + isoprene flux was composed of 10% isoprene and 90% MBO. There was good agreement between the light and temperature dependency of the sum of MBO and isoprene observed for this work and those of earlier studies. The above canopy flux measurements of the sum of MBO and isoprene and the sum of monoterpenes were compared to emissions calculated using the Model of Emissions of Gases and Aerosols from Nature (MEGAN 2.1). The best agreement between MEGAN 2.1 and measurements was reached using emission factors determined from site specific leaf cuvette measurements. While the modelled and measured MBO + isoprene fluxes agree well the emissions of the sum of monoterpenes is underestimated by MEGAN 2.1. This is expected as some factors impacting monoterpene emissions, such as physical damage of needles and branches due to storms, are not included in MEGAN 2.1. After a severe hailstorm event, 22 ion mass peaks (attributed to six compound classes plus some unknown compounds) showed an elevated flux for the two following days. The sum of monoterpene emissions was 4–23 times higher compared to emissions prior to the hailstorm while MBO emissions remained unchanged. If one heavy storm occurs at this site every month we calculate that the monthly monoterpene emissions (in mg compound m −2 ) would be underestimated by 40% if this disturbance source is not considered.

Description: Aerosol variability and atmospheric transport in the Himalayan region from CALIOP 2007–2010 observations Atmospheric Chemistry and Physics Discussions, 13, 15271-15299, 2013 Author(s): S. Bucci, C. Cagnazzo, F. Cairo, L. Di Liberto, and F. Fierli Himalayan Plateau is surrounded by regions with high natural and anthropogenic aerosol emissions that have a strong impact on regional climate. This is particularly critical for the Himalayan glaciers whose equilibrium is also largely influenced by radiative direct and indirect effects induced by aerosol burden. This work focuses on the spatial and vertical distribution of different aerosol types, their seasonal variability and sources. The analysis of the 2007–2010 yr of CALIPSO vertically resolved satellite data allows the identification of spatial patterns of desert dust and carbonaceous particles in different atmospheric layers. Clusters of Lagrangian back-trajectories highlight the transport pathways from source regions during the dusty spring season. The analysis shows a prevalence of dust; at low heights they are distributed mainly north (with a main contribution from the Gobi and Taklamakan deserts) and west of the Tibetan Plateau (originating from the deserts of South-West Asia and advected by the westerlies). Above the Himalayas the dust amount is minor but still not negligible (detectable in around 20% of the measurements), and transport from more distant deserts (Sahara and Arabian Peninsula) is important. Smoke aerosol, produced mainly in North India and East China, is subject to shorter range transport and is indeed observed closer to the sources while there is a limited amount reaching the top of the plateau. Data analysis reveals a clear seasonal variability in the frequencies of occurrence for the main aerosol types; dust is regulated principally by the monsoon dynamics, with maxima of occurrence in spring. The study also highlights relevant interannual differences, showing a larger presence of aerosol in the region during 2007 and 2008 yr.

Description: Quantifying aerosol mixing state with entropy and diversity measures Atmospheric Chemistry and Physics Discussions, 13, 15615-15662, 2013 Author(s): N. Riemer and M. West This paper presents the first quantitative metric for aerosol population mixing state, defined as the distribution of per-particle chemical species composition. This new metric, the mixing state index χ, is an affine ratio of the average per-particle species diversity D α and the bulk population species diversity D γ , both of which are based on information-theoretic entropy measures. The mixing state index χ enables the first rigorous definition of the spectrum of mixing states from so-called external mixture to internal mixture, which is significant for aerosol climate impacts, including aerosol optical properties and cloud condensation nuclei activity. We illustrate the usefulness of this new mixing state framework with model results from the stochastic particle-resolved model PartMC-MOSAIC. These results demonstrate how the mixing state metrics evolve with time for several archetypal cases, each of which isolates a specific process such as coagulation, emission, or condensation. Further, we present an analysis of the mixing state evolution for a complex urban plume case, for which these processes occur simultaneously. We additionally derive theoretical properties of the mixing state index and present a family of generalized mixing state indexes that vary in the importance assigned to low-mass-fraction species.

Description: Long-term observations of positive cluster ion concentration, sources and sinks at the high altitude site of the Puy de Dôme Atmospheric Chemistry and Physics Discussions, 13, 14927-14975, 2013 Author(s): C. Rose, J. Boulon, M. Hervo, H. Holmgren, E. Asmi, M. Ramonet, P. Laj, and K. Sellegri Cluster particles (0.8–1.9 nm) are key entities involved in nucleation and new particle formation processes in the atmosphere. Cluster ions were characterized in clear sky conditions at the Puy de Dôme station (1465 m a.s.l). The studied dataset spread over five years (February 2007–February 2012), which provided a unique chance to catch seasonal variations of cluster ion properties at high altitude. Statistical values of the cluster ion concentration and diameter are reported for both positive and negative polarities. Cluster ions were found to be ubiquitous at the Puy de Dôme and displayed an annual variation with lower concentrations in spring. Positive cluster ions were less numerous than negative ones but were larger in diameters. Negative cluster ion properties seemed insensitive to the occurrence of a new particle formation (NPF) event while positive cluster ions appeared to be significantly more numerous and larger on event days. The parameters of the balance equation for the positive cluster concentration are reported, separately for the different seasons and for the NPF event days and non-event days. The steady state assumption suggests that the ionization rate is balanced with two sinks which are the ion recombination and the attachment on aerosol particles, referred as "aerosol ion sink". The aerosol ion sink was found to be higher during the warm season and dominated the loss of ions. The positive ionization rates derived from the balance equation were well correlated with the ionization rates obtained from radon measurement, and they were on average higher in summer and fall compared to winter and spring. Neither the aerosol ion sink nor the ionization rate were found to be significantly different on event days compared to non-event days, and thus they were not able to explain the different positive cluster concentrations between event and non-event days. Hence, the excess of positive small ions on event days may derive from an additional source of ions coupled with the fact that the steady state was not verified on event days.

Description: Review and uncertainty assessment of size-resolved scavenging coefficient formulations for snow scavenging of atmospheric aerosols Atmospheric Chemistry and Physics Discussions, 13, 14823-14869, 2013 Author(s): L. Zhang, X. Wang, M. D. Moran, and J. Feng Theoretical parameterizations for the size-resolved scavenging coefficient for atmospheric aerosol particles scavenged by snow (Λ snow ) need assumptions regarding (i) snow particle–aerosol particle collection efficiency E , (ii) snow particle size distribution N ( D p ), (iii) snow particle terminal velocity V D , and (iv) snow particle cross-sectional area A . Existing formulas for these parameters are reviewed in the present study and uncertainties in Λ snow caused by various combinations of these parameters are assessed. Different formulations of E can cause uncertainties in Λ snow of more than one order of magnitude for all aerosol sizes for typical snowfall intensities. E is the largest source of uncertainty among all the input parameters, similar to rain scavenging of atmospheric aerosols (Λ rain ) as was found in a previous study by Wang et al. (2010). However, other parameters can also cause significant uncertainties in Λ snow , and the uncertainties from these parameters are much larger than for Λ rain . Specifically, different N ( D p ) formulations can cause one-order-of-magnitude uncertainties in Λ snow for all aerosol sizes, as is also the case for a combination of uncertainties from both V D and A . In comparison, uncertainties in Λ rain from N ( D p ) are smaller than a factor of 5 and those from V D are smaller than a factor of 2. Λ snow estimated from one empirical formula generated from field measurements falls in the upper range of, or is slightly higher than, theoretically estimated values. The predicted aerosol concentrations obtained using different Λ snow formulas can differ by a factor of two for just a one-centimeter snowfall (liquid water equivalent of approximately 1 mm). It is likely that, for typical rain and snow event the removal of atmospheric aerosol particles by snow is more effective than removal by rain for equivalent precipitation amounts, although a firm conclusion requires much more evidence.

Description: Atmospheric waves as scaling, turbulent phenomena Atmospheric Chemistry and Physics Discussions, 13, 14797-14822, 2013 Author(s): J. Pinel and S. Lovejoy It is paradoxical that while atmospheric dynamics are highly nonlinear and turbulent that atmospheric waves are commonly modelled by linear or weakly nonlinear theories. We postulate that the laws governing atmospheric waves are on the contrary high Reynold's number ( Re ), emergent laws so that – in common with the emergent high Re turbulent laws – they are also constrained by scaling symmetries. We propose an effective turbulence – wave propagator which corresponds to a fractional and anisotropic extension of the classical wave equation propagator with dispersion relations similar to those of inertial gravity waves (and Kelvin waves) yet with an anomalous (fractional) order H wav /2. Using geostationary IR radiances, we estimate the parameters finding that H wav /2 ≈ 0.17 ± 0.04 (the classical value = 2).

Description: Optimizing Saharan dust CALIPSO retrievals Atmospheric Chemistry and Physics Discussions, 13, 14749-14795, 2013 Author(s): V. Amiridis, U. Wandinger, E. Marinou, E. Giannakaki, A. Tsekeri, S. Basart, S. Kazadzis, A. Gkikas, M. Taylor, J. Baldasano, and A. Ansmann We demonstrate improvements in CALIPSO dust extinction retrievals over North Africa and Europe when corrections are applied regarding the Saharan dust lidar ratio assumption, the separation of dust portion in detected dust mixtures, and the averaging scheme introduced in the Level 3 CALIPSO product. First, a universal, spatially constant lidar ratio of 58 sr instead of 40 sr is applied to individual Level 2 dust-related backscatter products. The resulting aerosol optical depths show an improvement compared with synchronous and co-located AERONET measurements. An absolute bias of the order of −0.03 has been found, improving on the statistically significant biases of the order of −0.10 reported in the literature for the original CALIPSO product. When compared with the MODIS co-located AOD product, the CALIPSO negative bias is even less for the lidar ratio of 58 sr. After introducing the new lidar ratio for the domain studied, we examine potential improvements to the climatological CALIPSO Level 3 extinction product: (1) by introducing a new methodology for the calculation of pure dust extinction from dust mixtures and (2) by applying an averaging scheme that includes zero extinction values for the non-dust aerosol types detected. The scheme is applied at a horizontal spatial resolution of 1° × 1° for ease of comparison with the instantaneous and co-located dust extinction profiles simulated by the BSC-DREAM8b dust model. Comparisons show that the extinction profiles retrieved with the proposed methodology reproduce the well-known model biases per sub-region examined. The very good agreement of the proposed CALIPSO extinction product with respect to AERONET, MODIS and the BSC-DREAM8b dust model, makes this dataset an ideal candidate for the provision of an accurate and robust multi-year dust climatology over North Africa and Europe.

Description: Climatology of pure Tropospheric profiles and column contents of ozone and carbon monoxide using MOZAIC in the mid-northern latitudes (24° N to 50° N) from 1994 to 2009 Atmospheric Chemistry and Physics Discussions, 13, 14695-14747, 2013 Author(s): R. M. Zbinden, V. Thouret, P. Ricaud, F. Carminati, J.-P. Cammas, and P. Nédélec The objective of this paper is to deliver the most accurate ozone (O 3 ) and carbon monoxide (CO) climatology for the pure troposphere only, i.e. exclusively from the ground to the dynamical tropopause on an individual profile basis. The results (profiles and columns) are derived solely from the M easurements of OZ one and water vapour by in-service AI rbus air C raft programme (MOZAIC) over fifteen years (1994–2009). The study, focused on the northern mid-latitudes [24° N–50° N] and [120° W–140° E], includes more than 40 000 profiles over 11 sites to give a quasi-global zonal picture. Considering all the sites, the pure tropospheric column peak-to-peak seasonal cycle ranges are 23.7–43.2 DU for O 3 and 1.7–6.9 × 10 18 mol cm −2 for CO. The maxima of the seasonal cycles are not in phase, occurring in February–April for CO and May–July for O 3 . The phase shift is related to the photochemistry and OH removal efficiencies. The purely tropospheric seasonal profiles are characterized by a typical autumn-winter/spring-summer O 3 dichotomy, (except in Los Angeles, Eastmed – a cluster of Cairo and Tel Aviv – and the regions impacted by the summer monsoon) and a summer-autumn/winter-spring CO dichotomy. We revisit the boundary-layer, mid-tropospheric (MT) and upper-tropospheric (UT) partial columns, using a new monthly-varying MT ceiling. Interestingly, the seasonal cycle maximum of the UT partial columns is shifted from summer to spring for O 3 and to very early spring for CO. Conversely, the MT maximum is shifted from spring to summer and is associated with a summer (winter) MT thickening (thinning). Lastly, the pure tropospheric seasonal cycles derived from our analysis are consistent with the cycles derived from spaceborne measurements, the correlation coefficients being r = 0.6–0.9 for O 3 , and r 〉 0.9 for CO. The cycles observed from space are nevertheless greater than MOZAIC for O 3 (by 9–18 DU) and smaller for CO (up to 1 × 10 18 mol cm −2 ). The larger winter O 3 difference between the two data sets suggests probable stratospheric contamination in satellite data due to the tropopause position. The study underlines the importance of rigorously discriminating between the stratospheric and tropospheric reservoirs and avoiding use of a monthly-averaged tropopause position without this strict discrimination, in order to assess the pure O 3 and CO tropospheric trends.

Description: A climatology of formation conditions for aerodynamic contrails Atmospheric Chemistry and Physics Discussions, 13, 14667-14693, 2013 Author(s): K. Gierens and F. Dilger Aerodynamic contrails are defined in this paper as line shaped ice clouds caused by aerodynamically triggered cooling over the wings of an aircraft in cruise which become visible immediately at the trailing edge of the wing or close to it. Effects at low altitudes like condensation to liquid droplets and their potential heterogeneous freezing are excluded from our definition. We study atmospheric conditions that allow formation of aerodynamic contrails. These conditions are stated and then applied to atmospheric data, first to a special case where an aerodynamic contrail was actually observed and then to a full year of global reanalysis data. We show where, when (seasonal variation), and how frequently (probability) aerodynamic contrails can form, and how this relates to actual patterns of air traffic. We study the formation of persistent aerodynamic contrails as well. Finally we check whether aerodynamic and exhaust contrails can coexist in the atmosphere. We show that visible aerodynamic contrails are possible only in an altitude range between roughly 540 and 250 hPa, and that the ambient temperature is the most important parameter, not the relative humidity. Finally we give an argument for our believe that currently aerodynamic contrails have a much smaller climate effect than exhaust contrails, which may however change in future with more air traffic in the tropics.

Description: Expansion of global drylands under a warming climate Atmospheric Chemistry and Physics Discussions, 13, 14637-14665, 2013 Author(s): S. Feng and Q. Fu Global drylands encompassing hyper-arid, arid, semiarid, and dry subhumid areas cover about 41% of the earth's terrestrial surface and are home to more than a third of the world's population. By analyzing observations for 1948–2008 and climate model simulations for 1948–2100, we show that global drylands have expanded in last sixty years and will continue to expand in the 21st century. By the end of this century, the world's drylands under a high greenhouse gas emission scenario are projected to be 5.8 × 10 6 km 2 (or 10%) larger than in the 1961–1990 climatology. The major expansion of arid regions will occur over southwest North America, the northern fringe of Africa, southern Africa, and Australia, while major expansions of semiarid regions will occur over the north side of the Mediterranean, southern Africa, and North and South America. The global dryland expansions will increase the population affected by water scarcity and land degradations.

Description: The role of horizontal model resolution in assessing the transport of CO in a middle latitude cyclone using WRF-Chem Atmospheric Chemistry and Physics Discussions, 13, 14871-14925, 2013 Author(s): C. A. Klich and H. E. Fuelberg We use the Weather Research and Forecasting with Chemistry (WRF-Chem) online chemical transport model to simulate a middle latitude cyclone in East Asia at three different horizontal resolutions (45, 15, and 5 km grid spacing). The cyclone contains a typical warm conveyor belt (WCB) with an embedded squall line that passes through an area having large surface concentrations (〉400 ppbv) of carbon monoxide (CO). Model output from WRF-Chem is used to compare differences between the large-scale CO vertical transport by the WCB (the 45 km simulation) with the smaller-scale transport due to its convection (the 5 km simulation). Forward trajectories are calculated from WRF-Chem output using HYSPLIT. At 45 km grid spacing, the WCB exhibits gradual ascent, lofting surface CO to 6–7 km. Upon reaching the warm front, the WCB and associated CO ascend more rapidly and later turn eastward over the Pacific Ocean. Convective transport at 5 km resolution with explicitly resolved convection occurs much more rapidly, with surface CO lofted to altitudes greater than 10 km in 1 h or less. We also compute CO vertical mass fluxes to compare differences in transport due to the different grid spacings. Upward CO flux exceeds 110 000 t h −1 in the domain with explicit convection when the squall line is at peak intensity, while fluxes from the two coarser resolutions are an order of magnitude smaller. Specific areas of interest within the 5 km domain are defined to compare the magnitude of convective transport to that within the entire 5 km region. Although convection encompasses only a small portion of the 5 km domain, it is responsible for ~40% of the upward CO transport. We also examine the vertical transport due to a short wave trough and its associated area of convection, not related to the cyclone, that lofts CO to the upper troposphere. Results indicate that fine-scale resolution with explicitly resolved convection is important when assessing the vertical transport of surface emissions in areas of deep convection.

Description: The seasonal melt-freeze transitions are fundamental features of the Arctic climate system. The representation of the pan-Arctic melt and freeze onset (north of 60°N) is assessed in two reanalyses and eleven CMIP5 global circulation models (GCMs). The seasonal melt-freeze transitions are retrieved from surface air temperature (SAT) across the land and sea-ice domains and evaluated against surface observations. While monthly averages of SAT are reasonably well represented in models, large model-observation and model–model disparities of timing of melt and freeze onset are evident. The evaluation against surface observations reveals that the ERA-Interim reanalysis performs the best, closely followed by some of the climate models. GCMs and reanalyses capture the seasonal melt-freeze transitions better in the central Arctic than in the marginal seas and across the land areas. The GCMs project that during the 21st century, the summer length—the period between melt and freeze onset—will increase over land by about 1 month at all latitudes, and over sea ice by 1 and 3 months at low and high latitudes, respectively. This larger summer-length increase over sea ice at progressively higher latitudes is related to a retreat of summer sea ice during the 21st century, since open water freezes roughly 40 days later than ice-covered ocean. As a consequence, by the year 2100, the freeze onset is projected to be initiated within roughly 10 days across the whole Arctic Ocean, whereas this transition varies by about 80 days today.

Description: A Lagrangian view of ozone production tendency in North American outflow in summers 2009 and 2010 Atmospheric Chemistry and Physics Discussions, 13, 15141-15190, 2013 Author(s): B. Zhang, R. C. Owen, J. A. Perlinger, A. Kumar, S. Wu, M. Val Martin, L. Kramer, D. Helmig, and R. E. Honrath The Pico Mountain Observatory, located at 2225 m a.s.l. in the Azores Islands, was established in 2001 to observe long-range transport from North America to the central North Atlantic. In previous research conducted at the Observatory, ozone enhancement (〉55 ppbv) in North American outflows was observed, and efficient ozone production in these outflows was postulated. This study is focused on determining the causes for high d [O 3 ]/ d [CO] values (~1 ppbv ppbv −1 ) observed in summers of 2009 and 2010. The folded retroplume technique, developed by Owen and Honrath (2009), was applied to combine upwind FLEXPART transport pathways with GEOS-Chem chemical fields. This folded result provides a semi-Lagrangian view of polluted North American outflow in terms of physical properties and chemical processes, including production/loss rate of ozone and NO x produced by lightning and thermal decomposition of PAN. Two transport events from North America were identified for detailed analysis. High d [O 3 ]/ d [CO] was observed in both events, but due to differing transport mechanisms, ozone production tendency differed between the two. A layer of net ozone production was found at 2 km a.s.l. over the Azores in the first event plume, apparently driven by PAN decomposition during subsidence of air mass in the Azores-Bermuda High. In the second event, net ozone loss occurred during transport in the lower free troposphere, yet observed d [O 3 ]/ d [CO] was high. We estimate that in both events, CO loss through oxidation contributed significantly to d [O 3 ]/ d [CO] enhancement. Thus, CO is not appropriately used as a passive tracer of pollution in these events. In general, use of d [O 3 ]/ d [CO] as an indicator of net ozone production/loss may be invalid for any situation in which oxidants are elevated. Based on our analysis, use of d [O 3 ]/ d [CO] to diagnose ozone enhancement without verifying the assumption of negligible CO loss is not advisable.

Description: Free troposphere ozone and carbon monoxide over the North Atlantic for 2001–2011 Atmospheric Chemistry and Physics Discussions, 13, 15377-15407, 2013 Author(s): A. Kumar, S. Wu, M. F. Weise, R. Honrath, R. C. Owen, D. Helmig, L. Kramer, M. Val Martin, and Q. Li In-situ measurements of carbon monoxide (CO) and ozone (O 3 ) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal are analyzed together with results from atmospheric chemical transport modeling (GEOS-Chem) and satellite remote sensing (AIRS for CO and TES for O 3 ) to examine the evolution of free-troposphere CO and O 3 over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O 3 well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O 3 based on harmonic regression analysis of the measurement data. The best estimates of the trend for CO and O 3 measurements are −0.31 ± 0.30 (2-σ) ppbv yr −1 and −0.21 ± 0.11 (2-σ) ppbv yr −1 , respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The major factor contributing to the reported decrease in CO and O 3 mixing ratios at PMO over the past decade is the decline in anthropogenic CO and O 3 -precursor emissions in regions such as North America and Europe. The increase in Asian emissions does not seem to outweigh the impact of these declines resulting in overall decreasing trends for both CO and O 3 . For O 3 , however, increase in atmospheric water vapor content associated with climate change also appears to be a contributing factor causing enhanced destruction of the O 3 during transport from source regions. These hypotheses are supported by results from the GEOS-Chem tagged CO and tagged O 3 simulations.

Description: Mesoscale modeling of smoke transport over the Southeast Asian Maritime Continent: coupling of smoke direct radiative feedbacks below and above the low-level clouds Atmospheric Chemistry and Physics Discussions, 13, 15443-15492, 2013 Author(s): C. Ge, J. Wang, and J. S. Reid The online-coupled Weather Research and Forecasting model with Chemistry (WRF-Chem) is used to simulate the direct and semi-direct radiative impacts of smoke particles over the Southeast Asian Marine Continents (MC, 10° S–10° N, 90° E–150° E) during October 2006 when a significant El Nino event caused the highest biomass burning activity since 1997. With the use of OC (Organic Carbon)/BC (Black Carbon) ratio of 10 in the smoke emission inventory, the baseline simulation shows that the low-level clouds amplifying effect on smoke absorption led to a warming effect at the top-of-atmosphere (TOA) with a domain/monthly average forcing value of ~20 W m −2 over the islands of Borneo and Sumatra. The smoke-induced monthly average daytime heating (0.3 K) that is largely confined above the low-level clouds results in the local convergence over the smoke source region. This heating-induced convergence coupled with daytime planetary boundary layer turbulent mixing, transports more smoke particles above the planetary boundary layer height (PBLH), hence rendering a positive feedback. This positive feedback contrasts with the decrease of cloud fraction resulted from the combined effects of smoke heating within the cloud layer and the more stability in the boundary layer; the latter can be considered as a negative feedback in which decrease of cloud fraction weakens the heating by smoke particles above the clouds. During nighttime, the elevated smoke layer (above clouds in daytime) is decoupled from boundary layer, and the reduction of PBLH due to the residual surface cooling from the daytime lead to the accumulation of smoke particles near the surface. Because of smoke radiative extinction, on monthly basis, the amount of the solar input at the surface is reduced as large as 60 W m −2 , which lead to the decrease of sensible heat, latent heat, 2 m air temperature, and PBLH by a maximum of 20 W m −2 , 20 W m −2 , 1 K, 120 m, respectively. The decrease of boundary layer mixing and the generation of convergence above the PBL also results in a reduction of precipitable water 1–2 km above the PBLH and more precipitable water near the surface and in upper part of the middle troposphere with changes around 0.1 mm. Overall, there is less of a change of column water vapor over the land, and an increase of water vapor amount over the Karimata Strait. The cloud changes over continents are mostly occurred over the islands of Sumatra and Borneo during the daytime, where the low-level cloud fraction decreases more than 10%. However, the change of local wind (include sea breeze) induced by the smoke radiative feedback leads to more convergence over Karimata Strait and south coastal area of Kalimantan during both daytime and night time; consequently, cloud fraction is increased there up to 20%. The sensitivities with different OC/BC ratio show the importance of the smoke single scattering albedo for the smoke semi-direct effects. A case study on 31 October 2006 further demonstrated a much larger (more than twice of the monthly average) feedback induced by smoke aerosols. The decreased sea breeze during big events can lead to prominent increase (40%) of low-level cloud over coastal water. Lastly, the direct and semi-direct radiative impact of smoke particles over the Southeast Asian Marine Continents is summarized as a conceptual model.

Description: Global carbon monoxide products from combined AIRS, TES and MLS measurements on A-train satellites Atmospheric Chemistry and Physics Discussions, 13, 15409-15441, 2013 Author(s): J. X. Warner, R. Yang, Z. Wei, F. Carminati, A. Tangborn, Z. Sun, W. Lahoz, J.-L. Attié, L. El Amraoui, and B. Duncan This study tests a novel methodology to add value to satellite datasets. This methodology, data fusion, is similar to data assimilation, except that the background model-based field is replaced by a satellite dataset, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these datasets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS/TES and AIRS/MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20–30% and above 20%, respectively) as compared with AIRS-only retrievals, and improved coverage compared with TES and MLS CO data.

Description: An inverse modeling method to assess the source term of the Fukushima nuclear power plant accident using gamma dose rate observations Atmospheric Chemistry and Physics Discussions, 13, 15567-15614, 2013 Author(s): O. Saunier, A. Mathieu, D. Didier, M. Tombette, D. Quélo, V. Winiarek, and M. Bocquet The Chernobyl nuclear accident and more recently the Fukushima accident highlighted that the largest source of error on consequences assessment is the source term including the time evolution of the release rate and its distribution between radioisotopes. Inverse modeling methods, which combine environmental measurements and atmospheric dispersion models, have proven efficient in assessing source term due to an accidental situation (Gudiksen, 1989; Krysta and Bocquet, 2007; Stohl et al., 2012a; Winiarek et al., 2012). Most existing approaches are designed to use air sampling measurements (Winiarek et al., 2012) and some of them also use deposition measurements (Stohl et al., 2012a; Winiarek et al., 2013) but none of them uses dose rate measurements. However, it is the most widespread measurement system, and in the event of a nuclear accident, these data constitute the main source of measurements of the plume and radioactive fallout during releases. This paper proposes a method to use dose rate measurements as part of an inverse modeling approach to assess source terms. The method is proven efficient and reliable when applied to the accident at the Fukushima Daiichi nuclear power plant (FD-NPP). The emissions for the eight main isotopes 133 Xe, 134 Cs, 136 Cs, 137 Cs, 137m Ba, 131 I, 132 I and 132 Te have been assessed. Accordingly, 103 PBq of 131 I, 35.5 PBq of 132 I, 15.5 PBq of 137 Cs and 12 100 PBq of noble gases were released. The events at FD-NPP (such as venting, explosions, etc.) known to have caused atmospheric releases are well identified in the retrieved source term. The estimated source term is validated by comparing simulations of atmospheric dispersion and deposition with environmental observations. The result is that the model-measurement agreement for all of the monitoring locations is correct for 80% of simulated dose rates that are within a factor of 2 of the observed values. Changes in dose rates over time have been overall properly reconstructed, especially in the most contaminated areas to the northwest and south of the FD-NPP. A comparison with observed atmospheric activity concentration and surface deposition shows that the emissions of caesiums and 131 I are realistic but that 132 I and 132 Te are probably underestimated and noble gases are likely overestimated. Finally, an important outcome of this study is that the method proved to be perfectly suited to emergency management and could contribute to improve emergency response in the event of a nuclear accident.

Description: The dynamics of a low-order coupled wind-driven ocean–atmosphere system is investigated with emphasis on its predictability properties. The low-order coupled deterministic system is composed of a baroclinic atmosphere for which 12 dominant dynamical modes are only retained (Charney and Straus in J Atmos Sci 37:1157–1176, 1980 ) and a wind-driven, quasi-geostrophic and reduced-gravity shallow ocean whose field is truncated to four dominant modes able to reproduce the large scale oceanic gyres (Pierini in J Phys Oceanogr 41:1585–1604, 2011 ). The two models are coupled through mechanical forcings only. The analysis of its dynamics reveals first that under aperiodic atmospheric forcings only dominant single gyres (clockwise or counterclockwise) appear, while for periodic atmospheric solutions the double gyres emerge. In the present model domain setting context, this feature is related to the level of truncation of the atmospheric fields, as indicated by a preliminary analysis of the impact of higher wavenumber (“synoptic” scale) modes on the development of oceanic gyres. In the latter case, double gyres appear in the presence of a chaotic atmosphere. Second the dynamical quantities characterizing the short-term predictability (Lyapunov exponents, Lyapunov dimension, Kolmogorov–Sinaï (KS) entropy) displays a complex dependence as a function of the key parameters of the system, namely the coupling strength and the external thermal forcing. In particular, the KS-entropy is increasing as a function of the coupling in most of the experiments, implying an increase of the rate of loss of information about the localization of the system on its attractor. Finally the dynamics of the error is explored and indicates, in particular, a rich variety of short term behaviors of the error in the atmosphere depending on the (relative) amplitude of the initial error affecting the ocean, from polynomial ( at 2  +  bt 3  +  ct 4 ) up to exponential-like evolutions. These features are explained and analyzed in the light of the recent findings on error growth (Nicolis et al. in J Atmos Sci 66:766–778, 2009 ).

Description: The ocean heat transport into the Arctic and the heat budget of the Barents Sea are analyzed in an ensemble of historical and future climate simulations performed with the global coupled climate model EC-Earth. The zonally integrated northward heat flux in the ocean at 70°N is strongly enhanced and compensates for a reduction of its atmospheric counterpart in the twenty first century. Although an increase in the northward heat transport occurs through all of Fram Strait, Canadian Archipelago, Bering Strait and Barents Sea Opening, it is the latter which dominates the increase in ocean heat transport into the Arctic. Increased temperature of the northward transported Atlantic water masses are the main reason for the enhancement of the ocean heat transport. The natural variability in the heat transport into the Barents Sea is caused to the same extent by variations in temperature and volume transport. Large ocean heat transports lead to reduced ice and higher atmospheric temperature in the Barents Sea area and are related to the positive phase of the North Atlantic Oscillation. The net ocean heat transport into the Barents Sea grows until about year 2050. Thereafter, both heat and volume fluxes out of the Barents Sea through the section between Franz Josef Land and Novaya Zemlya are strongly enhanced and compensate for all further increase in the inflow through the Barents Sea Opening. Most of the heat transported by the ocean into the Barents Sea is passed to the atmosphere and contributes to warming of the atmosphere and Arctic temperature amplification. Latent and sensible heat fluxes are enhanced. Net surface long-wave and solar radiation are enhanced upward and downward, respectively and are almost compensating each other. We find that the changes in the surface heat fluxes are mainly caused by the vanishing sea ice in the twenty first century. The increasing ocean heat transport leads to enhanced bottom ice melt and to an extension of the area with bottom ice melt further northward. However, no indication for a substantial impact of the increased heat transport on ice melt in the Central Arctic is found. Most of the heat that is not passed to the atmosphere in the Barents Sea is stored in the Arctic intermediate layer of Atlantic water, which is increasingly pronounced in the twenty first century.

Description: Forcing of stratospheric chemistry and dynamics during the Dalton Minimum Atmospheric Chemistry and Physics Discussions, 13, 15061-15104, 2013 Author(s): J. G. Anet, S. Muthers, E. Rozanov, C. C. Raible, T. Peter, A. Stenke, A. I. Shapiro, J. Beer, F. Steinhilber, S. Brönnimann, F. Arfeuille, Y. Brugnara, and W. Schmutz The response of atmospheric chemistry and climate to volcanic eruptions and a decrease in solar activity during the Dalton Minimum is investigated with the fully coupled atmosphere-ocean-chemistry general circulation model SOCOL-MPIOM covering the time period 1780 to 1840 AD. We carried out several sensitivity ensemble experiments to separate the effects of (i) reduced solar ultra-violet (UV) irradiance, (ii) reduced solar visible and near infrared irradiance, (iii) enhanced galactic cosmic ray intensity as well as less intensive solar energetic proton events and auroral electron precipitation, and (iv) volcanic aerosols. The introduced changes of UV irradiance and volcanic aerosols significantly influence stratospheric climate in the early 19th century, whereas changes in the visible part of the spectrum and energetic particles have smaller effects. A reduction of UV irradiance by 15% causes global ozone decrease below the stratopause reaching 8% in the midlatitudes at 5 hPa and a significant stratospheric cooling of up to 2 °C in the midstratosphere and to 6 °C in the lower mesosphere. Changes in energetic particle precipitation lead only to minor changes in the yearly averaged temperature fields in the stratosphere. Volcanic aerosols heat the tropical lower stratosphere allowing more water vapor to enter the tropical stratosphere, which, via HO x reactions, decreases upper stratospheric and mesospheric ozone by roughly 4%. Conversely, heterogeneous chemistry on aerosols reduces stratospheric NO x leading to a 12% ozone increase in the tropics, whereas a decrease in ozone of up to 5% is found over Antarctica in boreal winter. The linear superposition of the different contributions is not equivalent to the response obtained in a simulation when all forcing factors are applied during the DM – this effect is especially well visible for NO x /NO y . Thus, this study highlights the non-linear behavior of the coupled chemistry-climate system. Finally, we conclude that especially UV and volcanic eruptions dominate the changes in the ozone, temperature and dynamics while the NO x field is dominated by the EPP. Visible radiation changes have only very minor effects on both stratospheric dynamics and chemistry.

Description: Estimation of aerosol water and chemical composition from AERONET at Cabauw, the Netherlands Atmospheric Chemistry and Physics Discussions, 13, 15191-15232, 2013 Author(s): A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann Remote sensing of aerosols provides important information on the atmospheric aerosol abundance. However, due to the hygroscopic nature of aerosol particles observed aerosol optical properties are influenced by atmospheric humidity, and the measurements do not unambiguously characterize the aerosol dry mass and composition which complicates the comparison with aerosol models. In this study we derive aerosol water and chemical composition by a modeling approach that combines individual measurements of remotely sensed aerosol properties (e.g. optical thickness, single scattering albedo, refractive index and size distribution) from an AERONET (Aerosol Robotic Network) sun-photometer with radiosonde measurements of relative humidity. The model simulates water uptake by aerosols based on the chemical composition and size distribution. A minimization method is used to calculate aerosol composition and concentration, which are then compared to in situ measurements from the Intensive Measurement Campaign At the Cabauw Tower (IMPACT, May 2008, the Netherlands). Computed concentrations show reasonable agreement with surface observations and follow the day-to-day variability in observations. Total dry mass (33 ± 12 μg m −3 ) and black carbon concentrations (0.7 ± 0.3 μg m −3 ) are generally accurately computed. The uncertainty in the AERONET (real) refractive index (0.025–0.05) introduces larger uncertainty in the modeled aerosol composition (e.g. sulfates, ammonium nitrate or organic matter) and leads to an uncertainty of 0.1–0.25 in aerosol water volume fraction. Water volume fraction is highly variable depending on composition, up to 〉0.5 at 70–80% and

Description: Evaluation of various methods to measure particulate bound mercury and associated artifacts Atmospheric Chemistry and Physics Discussions, 13, 8585-8614, 2013 Author(s): S. Wang, T. M. Holsen, J. Huang, and Y.-J. Han This study was performed to determine how sampling artifacts associated with various sampling methods including open faced filter (OFF) pack, micro orifice uniform deposit impactor (MOUDI), and Tekran speciation system (TekSpec) impact particulate bound mercury (PBM) measurements. PBM measured by the MOUDI for 48 h was statistically lower than that measured with the TekSpec every 2 h, indicating that negative artifacts were significant for long sampling durations. Negative artifacts were also identified in lab experiments as the Hg 0 and HgCl 2 concentrations associated with particulate matter on the filter significantly decreased when the filter was exposed to zero air. Positive artifacts were also investigated. The OFF sampling for 48 h, which is likely to be associated with both positive and negative artifacts, measured a significantly lower PBM concentration than the TekSpec while the OFF and MOUDI (48 h sampling – minimal positive artifacts) showed similar results, suggesting that positive artifacts were minor under the rural condition encountered (low atmospheric gaseous oxidized mercury and typical oxidants concentrations). The Hg speciation associated with particles varied with atmospheric temperature, with the contribution of less volatile species including HgO and HgS increasing and more volatile Hg 0 and HgCl 2 decreasing as atmospheric temperature increased. There was significant correlation for PBM larger than 2.5 μm between TekSpec frit and MOUDI in this study, indicating that TekSpec frit is a good alternative sampler for measuring the concentration of coarse PBM.

Description: Aerosol and precipitation chemistry in the southwestern United States: spatiotemporal trends and interrelationships Atmospheric Chemistry and Physics Discussions, 13, 8615-8662, 2013 Author(s): A. Sorooshian, T. Shingler, A. Harpold, C. W. Feagles, T. Meixner, and P. D. Brooks This study characterizes the spatial and temporal patterns of aerosol and precipitation composition at six sites across the United States Southwest between 1995 and 2010. Precipitation accumulation occurs mostly during the wintertime (December–February) and during the monsoon season (July–September). Rain and snow pH levels are usually between 5–6, with crustal-derived species playing a major role in acid neutralization. These species (Ca 2+ , Mg 2+ , K + ,Na + ) exhibit their highest concentrations between March and June in both PM 2.5 and precipitation due mostly to dust. Crustal-derived species concentrations in precipitation exhibit positive relationships with SO 4 2− , NO 3 − , and Cl − , suggesting that acidic gases likely react with and partition to either crustal particles or hydrometeors enriched with crustal constituents. Concentrations of particulate SO 4 2− show a statistically significant correlation with rain SO 4 2− unlike snow SO 4 2− , which may be related to some combination of the vertical distribution of SO 4 2− (and precursors) and the varying degree to which SO 4 2− -enriched particles act as cloud condensation nuclei versus ice nuclei in the region. The coarse : fine aerosol mass ratio was correlated with crustal species concentrations in snow unlike rain, suggestive of a preferential role of coarse particles (mainly dust) as ice nuclei in the region. Precipitation NO 3 − : SO 4 2− ratios exhibit the following features with potential explanations discussed: (i) they are higher in precipitation as compared to PM 2.5 ; (ii) they exhibit the opposite annual cycle compared to particulate NO 3 − : SO 4 2− ratios; and (iii) they are higher in snow relative to rain during the wintertime. Long-term trend analysis for the monsoon season shows that the NO 3 − : SO 4 2− ratio in rain decreased at the majority of sites due mostly to air pollution regulations of SO 4 2− precursors.

Description: Effects of relative humidity on aerosol light scattering: results from different European sites Atmospheric Chemistry and Physics Discussions, 13, 8939-8984, 2013 Author(s): P. Zieger, R. Fierz-Schmidhauser, E. Weingartner, and U. Baltensperger The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σ sp ) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l., Ny-Ålesund, located on Spitsbergen in the Arctic, Mace Head, a coastal site in Ireland, Cabauw, a rural site in the Netherlands and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f (RH,λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σ sp (RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f (RH) largely varied at the five sites starting from very low values of f (RH = 85%,λ = 550 nm) around 1.28 for mineral dust to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch due to the absence of sea salt. Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f (RH). Both parameters are also needed to successfully predict f (RH). Finally, the measurement results were compared to the widely used aerosol model OPAC (Hess et al., 1998). Significant discrepancies were seen especially at intermediate RH ranges, which were mainly attributed to inappropriate implemented hygroscopic growth within OPAC. Replacement of the hygroscopic growth with recent literature values showed a clear improvement of the OPAC model.

Description: Spectro-microscopic measurements of carbonaceous aerosol aging in Central California Atmospheric Chemistry and Physics Discussions, 13, 9179-9216, 2013 Author(s): R. C. Moffet, T. C. Rödel, S. T. Kelly, X. Y. Yu, G. T. Carroll, J. Fast, R. A. Zaveri, A. Laskin, and M. K. Gilles Carbonaceous aerosols are responsible for large uncertainties in climate models, degraded visibility, and adverse health effects. The Carbonaceous Aerosols and Radiative Effects Study (CARES) was designed to study carbonaceous aerosols in the natural environment of Central Valley, California, and learn more about their atmospheric formation and aging. This paper presents results from spectro-microscopic measurements of carbonaceous particles collected during CARES at the time of pollution accumulation event (27–29 June 2010), when in situ measurements indicated an increase in the organic carbon content of aerosols as the Sacramento urban plume aged. Computer controlled scanning electron microscopy coupled with an energy dispersive X-ray detector (CCSEM/EDX) and scanning transmission X-ray microscopy coupled with near edge X-ray absorption spectroscopy (STXM/NEXAFS) were used to probe the chemical composition and morphology of individual particles. It was found that the mass of organic carbon on individual particles increased through condensation of secondary organic aerosol. STXM/NEXAFS indicated that the number fraction of homogenous organic particles lacking inorganic inclusions (greater than ~50 nm diameter) increased with plume age as did the organic mass per particle. Comparison of the CARES spectro-microscopic data set with a similar dataset obtained in Mexico City during the MILAGRO campaign showed that individual particles in Mexico City contained twice as much carbon as those sampled during CARES. The number fraction of soot particles at the Mexico City urban site (30%) was larger than at the CARES urban site (10%) and the most aged samples from CARES contained less carbon-carbon double bonds. Differences between carbonaceous particles in Mexico City and California result from different sources, photochemical conditions, gas phase reactants, and secondary organic aerosol precursors. The detailed results provided by these spectro-microscopic measurements will allow for a comprehensive evaluation of aerosol process models used in climate research.

Description: Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles Atmospheric Chemistry and Physics Discussions, 13, 8701-8767, 2013 Author(s): Z. A. Kanji, A. Welti, C. Chou, O. Stetzer, and U. Lohmann Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature ( T ) and relative humidity (RH), as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulphate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 〈 T 〈 263 K that will represent ageing but not internal mixing with in(organic) compounds. Heterogeneous ice nucleation of untreated kaolinite (Ka) and Arizona Test Dust (ATD) particles is compared to corresponding aged particles that are subjected to ozone exposures of 0.4–4.3 ppmv in a stainless steel aerosol tank. The portable ice nucleation counter (PINC) and immersion chamber combined with the Zurich ice nucleation chamber (IMCA – ZINC) are used to conduct deposition and immersion mode measurements respectively. Ice active fractions as well as ice active surface site densities ( n s ) are reported and observed to increase as a function of temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. Additionally, these are also the first results to show a suppression of heterogeneous ice nucleation without the condensation of a coating of (in)organic material. In immersion mode, low exposure Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka whereas high exposure ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low exposure Ka had ice active fractions of an order of magnitude higher than untreated Ka, where as high exposure ATD had ice active fractions up to a factor of 4 lower than untreated ATD. Based on our results, we present parameterizations in terms of n s ( T ) that can represent ice nucleation of atmospherically aged and non-aged particles for both immersion and deposition mode. We find excellent agreement (to within less than a factor of 2) with field measurements when parameterizations derived from our results are used to predict ice nuclei concentrations in the troposphere.

Description: Retrieval of the Eyjafjallajökull volcanic aerosol optical and microphysical properties from POLDER/PARASOL measurements Atmospheric Chemistry and Physics Discussions, 13, 8663-8699, 2013 Total and polarized radiances provided by the Polarization and Directionality of Earth Reflectances (POLDER) satellite sensor are used to retrieve the microphysical and optical properties of the volcanic plume observed during the Eyjafjallajökull volcano eruption in 2010, over cloud-free and cloudy ocean scenes. We selected two plume conditions, fresh aerosols near the sources (three cases) and a downwind volcanic plume observed over the North Sea 30 h after its injection into the atmosphere (aged aerosols). In the near-source conditions, the aerosol properties depend on the distance to the plume. Within the plume, aerosols are mainly non-spherical and in the coarse mode with an effective radius equal to 1.50 (± 0.15) μm and an Ångström Exponent (AE) close to 0.0. Far from the plume, in addition to the coarse mode, there are smaller particles retrieved in the accumulation mode suggesting a mixture of sulfate aerosols and volcanic dust, resulting in an AE around 0.8. The properties of the aerosols also depend on whether the plume is fresh or aged. For the downwind (aged) plume, if non-spherical coarse particles as well as some fine mode particles are still retrieved, the AE is smaller, around ~ 0.4. In addition, the real refractive index (RR) values are larger for the downwind plume (1.42 〈 RR 〈 1.58) than for the near-source plume (1.38 〈 RR 〈 1.48). The mean Single Scattering Albedo (SSA) retrieved at 0.865 μm was estimated at 0.97 over some parts of the downwind and near-source plumes; despite the low accuracy of our retrievals, the derived SSA values suggest that the ash particles are rather absorbing. To consider the particle shape, a combination of spheroid models is used. Although the employed model enabled accurate modeling of the POLDER signal in case of non-spherical ash, our approach failed to model the signal over the optically thickest parts of the near-source plume. The most probable reason for this is speculated to be the presence of ice crystals within the plume. For the Aerosol Above Clouds (AAC) scenes, polarized measurements allowed the retrieval of the Optical Thickness (OT) and the AE of optically thin volcanic ash. We found that all the cloud parameters retrieved by passive sensors were biased due to the presence of the elevated volcanic plumes. Finally, thermal infrared measurements were used to identify the type of multi-layer scene (i.e. cirrus clouds or volcanic dust above liquid clouds) and the retrieval method also provided the OT of thin cirrus layers above the clouds near Iceland.

Description: Present and future nitrogen deposition to national parks in the United States: critical load exceedances Atmospheric Chemistry and Physics Discussions, 13, 9151-9178, 2013 Author(s): R. A. Ellis, D. J. Jacob, M. Payer, L. Zhang, C. D. Holmes, B. A. Schichtel, T. Blett, E. Porter, L. H. Pardo, and J. A. Lynch National parks in the United States are protected areas wherein the natural habitat is to be conserved for future generations. Deposition of anthropogenic nitrogen (N) transported from areas of human activity (fuel combustion, agriculture) may affect these natural habitats if it exceeds an ecosystem-dependent critical load (CL). We quantify and interpret the deposition to Class I US national parks for present-day and future (2050) conditions using the GEOS-Chem global chemical transport model with 1/2° × 2/3° horizontal resolution over North America. We estimate CL values in the range 2.5–5 kg N ha −1 yr −1 for the different parks with the goal of protecting the most sensitive ecosystem receptors. For present-day conditions, we find 24 out of 45 parks to be in CL exceedance and 14 more to be marginally so. Many of these are in remote areas of the West. Most (40–85%) of the deposition originates from NO x emissions (fuel combustion). We then project future changes in N deposition using the Representative Concentration Pathway (RCP) emission scenarios for 2050. These feature 52–73% declines in US NO x emissions relative to present but 19–50% increases in US ammonia (NH 3 ) emissions. Nitrogen deposition at US national parks then becomes dominated by domestic NH 3 emissions. While deposition decreases in the East relative to present, there is little progress in the West and increases in some regions. We find that 17–25 US national parks will have CL exceedances in 2050 based on the RCP scenarios. Even in total absence of anthropogenic NO x emissions, 14–18 parks would still have a CL exceedance. Returning all parks to N deposition below CL by 2050 will require at least a 55% decrease in anthropogenic NH 3 emissions relative to RCP-projected 2050 levels.

Description: Redox activity of naphthalene secondary organic aerosol Atmospheric Chemistry and Physics Discussions, 13, 9107-9149, 2013 Author(s): R. D. McWhinney, S. Zhou, and J. P. D. Abbatt Chamber secondary organic aerosol (SOA) from low-NO x photooxidation of naphthalene by hydroxyl radical was examined with respect to its redox cycling behaviour using the dithiothreitol (DTT) assay. Naphthalene SOA was highly redox active, consuming DTT at an average rate of 118 ± 14 pmol per minute per μg of SOA material. Measured particle-phase masses of the major previously identified redox active products, 1,2- and 1,4-naphthoquinone, accounted for only 21 ± 3% of the observed redox cycling activity. The redox-active 5-hydroxy-1,4-naphthoquinone was identified as a new minor product of naphthalene oxidation, and including this species in redox activity predictions increased the predicted DTT reactivity to 30 ± 5% of observations. Similar attempts to predict redox behaviour of oxidised two-stroke engine exhaust particles by measuring 1,2-naphthoquinone, 1,4-naphthoquinone and 9,10-phenanthrenequinone predicted DTT decay rates only 4.9 ± 2.5% of those observed. Together, these results suggest that there are substantial unidentified redox-active SOA constituents beyond the small quinones that may be important toxic components of these particles. A gas-to-SOA particle partitioning coefficient was calculated to be (7.0 ± 2.5) × 10 −4 m 3 μg −1 for 1,4-naphthoquinone at 25 °C. This value suggests that under typical warm conditions, 1,4-naphthoquinone is unlikely to contribute strongly to redox behaviour of ambient particles, although further work is needed to determine the potential impact under conditions such as low temperatures where partitioning to the particle is more favourable. As well, higher order oxidation products that likely account for a substantial fraction of the redox cycling capability of the naphthalene SOA are likely to partition much more strongly to the particle phase.