ALBERT

Description: Influence of biomass burning on CCN number and hygroscopicity during summertime in the eastern Mediterranean Atmospheric Chemistry and Physics Discussions, 15, 21539-21582, 2015 Author(s): A. Bougiatioti, S. Bezantakos, I. Stavroulas, N. Kalivitis, P. Kokkalis, G. Biskos, N. Mihalopoulos, A. Papayannis, and A. Nenes This study investigates the CCN activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from cloud condensation nuclei (CCN) measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the hygroscopicity parameter, κ, for all particle sizes. The reason, however, for this decrease was not the same for all size modes; smaller particle sizes appeared to be richer in less hygroscopic, less CCN-active components due to coagulation processes while larger particles become less hygroscopic during the biomass burning events due to condensation of less hygroscopic gaseous compounds. In addition, smaller particles exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of aging and retained high levels of CCN activity. These conclusions are further supported by the observed mixing state determined by the HTDMA measurements. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles and a large fraction of the CCN concentrations sampled. Based on Positive Matrix Factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend with the BBOA component, with enhancements of CCN in biomass burning plumes ranging between 65 and 150 %, for supersaturations ranging between 0.2 and 0.7 %. Using multilinear regression, we determine the hygroscopicity of the prime organic aerosol components (BBOA, OOA-BB and OOA); it is found that the total organic hygroscopicity is very close to the inferred hygroscopicity of the oxygenated organic aerosol components. Finally, the transformation of freshly-emitted biomass burning (BBOA) to more oxidized organic aerosol (OOA-BB) can result in a two-fold increase of the inferred organic hygroscopicity. Almost 10 % of the total aerosol hygroscopicity is related to the two biomass burning components (BBOA and OOA-BB), which in turn contribute almost 35 % to the fine-particle organic water of the aerosol. This is important as organic water can contribute to the atmospheric chemistry and the direct radiative forcing.

Description: Measurement-based direct radiative effect by brown carbon over Indo-Gangetic Plain Atmospheric Chemistry and Physics Discussions, 15, 21583-21606, 2015 Author(s): A. Arola, G. L. Schuster, M. R. A. Pitkänen, O. Dubovik, H. Kokkola, A. V. Lindfors, T. Mielonen, T. Raatikainen, S. Romakkaniemi, S. N. Tripathi, and H. Lihavainen The importance of light absorbing organic aerosols, often called brown carbon (BrC), has become evident in recent years. However, there are relatively few measurement-based estimates for the direct radiative effect of BrC so far. In those earlier studies, the AErosol RObotic NETwork (AERONET) measured Aerosol Absorption Optical Depth (AAOD) and Absorption Angstrom Exponent (AAE) have been exploited. However, these two pieces of information are clearly not sufficient to separate properly carbonaceous aerosols from dust, while imaginary indices of refraction would contain more and better justified information for this purpose. This is first time that the direct radiative effect (DRE) of BrC is estimated by exploiting the AERONET-retrieved imaginary indices. We estimated it for four sites in Indo-Gangetic Plain (IGP), Karachi, Lahore, Kanpur and Gandhi College. We found a distinct seasonality, which was generally similar among all the sites, but with slightly different strengths. The monthly warming effect up to 0.5 W m -2 takes place during spring season. On the other hand, BrC results in overall cooling effect in the winter season, which can reach levels close to −1W m -2 . We then estimated similarly also DRE of black carbon and total aerosol, in order to assess the relative significance of BrC radiative effect in the radiative effects of other components. Even though BrC impact seems minor in this context, we demonstrated that it is not insignificant and moreover that it is crucial to perform spectrally resolved radiative transfer calculations to obtain good estimates for DRE of BrC.

Description: Uncertainties in calculating precipitation climatology in East Asia Hydrology and Earth System Sciences Discussions, 12, 7765-7783, 2015 Author(s): J. Kim and S. K. Park This study examines the uncertainty in calculating the fundamental climatological characteristics of precipitation in the East Asia region from multiple fine-resolution gridded analysis datasets based on in-situ rain gauge observations. Five observation-based gridded precipitation datasets are used to derive the long-term means, standard deviations in lieu of interannual variability and linear trends over the 28-year period from 1980 to 2007. Both the annual and summer (June–July–August) mean precipitation is examined. The agreement amongst these precipitation datasets are examined using multiple metrics including the signal-to-noise ratio (SNR) defined as the ratio between long-term means and the corresponding standard deviations, and Taylor diagrams which allows examinations of the pattern correlation, the standard deviation, and the centered root mean square error. It is found that the five gauge-based precipitation analysis datasets agree well in the long-term mean and interannual variability in most of the East Asia region including eastern China, Manchuria, South Korea, and Japan, which are densely populated and have fairly high density observation networks. The regions of large inter-dataset variations include Tibetan Plateau, Mongolia, northern Indo-China, and North Korea. The regions of large uncertainties are typically lightly populated and are characterized by severe terrain and/or extreme high elevations. Unlike the long-term mean and interannual variability, agreements between datasets in the linear trend is weak, both for the annual and summer mean values. In most of the East Asia region, the SNR for the linear trend is below 0.5, i.e., the inter-dataset variability exceeds the multi-data ensemble mean. The uncertainty in the spatial distribution of long-term means among these datasets occurs both in the spatial pattern and variability, but the uncertainty for the interannual variability and time trend is much larger in the variability than in the pattern correlation. Thus, care must be taken in using long-term trends calculated from gridded precipitation analysis data for climate studies over the East Asia region.

Description: Nonlinear effects of locally heterogeneous hydraulic conductivity fields on regional stream–aquifer exchanges Hydrology and Earth System Sciences Discussions, 12, 7727-7764, 2015 Author(s): J. Zhu, C. L. Winter, and Z. Wang Computational experiments are performed to evaluate the effects of locally heterogeneous conductivity fields on regional exchanges of water between stream and aquifer systems in the Middle Heihe River Basin (MHRB) of northwestern China. The effects are found to be nonlinear in the sense that simulated discharges from aquifers to streams are systematically lower than discharges produced by a base model parameterized with relatively coarse effective conductivity. A similar, but weaker, effect is observed for stream leakage. The study is organized around three hypotheses: (H1) small-scale spatial variations of conductivity significantly affect regional exchanges of water between streams and aquifers in river basins, (H2) aggregating small-scale heterogeneities into regional effective parameters systematically biases estimates of stream–aquifer exchanges, and (H3) the biases result from slow-paths in groundwater flow that emerge due to small-scale heterogeneities. The hypotheses are evaluated by comparing stream–aquifer fluxes produced by the base model to fluxes simulated using realizations of the MHRB characterized by local (grid-scale) heterogeneity. Levels of local heterogeneity are manipulated as control variables by adjusting coefficients of variation. All models are implemented using the MODFLOW simulation environment, and the PEST tool is used to calibrate effective conductivities defined over 16 zones within the MHRB. The effective parameters are also used as expected values to develop log-normally distributed conductivity ( K ) fields on local grid scales. Stream-aquifer exchanges are simulated with K fields at both scales and then compared. Results show that the effects of small-scale heterogeneities significantly influence exchanges with simulations based on local-scale heterogeneities always producing discharges that are less than those produced by the base model. Although aquifer heterogeneities are uncorrelated at local scales, they appear to induce coherent slow-paths in groundwater fluxes that in turn reduce aquifer–stream exchanges. Since surface water–groundwater exchanges are critical hydrologic processes in basin-scale water budgets, these results also have implications for water resources management.

Description: Near–surface air temperature and snow skin temperature comparison from CREST-SAFE station data with MODIS land surface temperature data Hydrology and Earth System Sciences Discussions, 12, 7665-7687, 2015 Author(s): C. L. Pérez Díaz, T. Lakhankar, P. Romanov, J. Muñoz, R. Khanbilvardi, and Y. Yu Land Surface Temperature (LST) is a key variable (commonly studied to understand the hydrological cycle) that helps drive the energy balance and water exchange between the Earth's surface and its atmosphere. One observable constituent of much importance in the land surface water balance model is snow. Snow cover plays a critical role in the regional to global scale hydrological cycle because rain-on-snow with warm air temperatures accelerates rapid snow-melt, which is responsible for the majority of the spring floods. Accurate information on near-surface air temperature ( T -air) and snow skin temperature ( T -skin) helps us comprehend the energy and water balances in the Earth's hydrological cycle. T -skin is critical in estimating latent and sensible heat fluxes over snow covered areas because incoming and outgoing radiation fluxes from the snow mass and the air temperature above make it different from the average snowpack temperature. This study investigates the correlation between MODerate resolution Imaging Spectroradiometer (MODIS) LST data and observed T -air and T -skin data from NOAA-CREST-Snow Analysis and Field Experiment (CREST-SAFE) for the winters of 2013 and 2014. LST satellite validation is imperative because high-latitude regions are significantly affected by climate warming and there is a need to aid existing meteorological station networks with the spatially continuous measurements provided by satellites. Results indicate that near-surface air temperature correlates better than snow skin temperature with MODIS LST data. Additional findings show that there is a negative trend demonstrating that the air minus snow skin temperature difference is inversely proportional to cloud cover. To a lesser extent, it will be examined whether the surface properties at the site are representative for the LST properties within the instrument field of view.

Description: Does drought alter hydrological functions in forest soils? An infiltration experiment Hydrology and Earth System Sciences Discussions, 12, 7689-7725, 2015 Author(s): K. F. Gimbel, H. Puhlmann, and M. Weiler The water cycle is expected to change in future and severely affect precipitation patterns across central Europe and in other parts of the world, leading to more frequent and severe droughts. Usually, it is assumed that system properties, like soil properties, remain stable and will not be affected by drought events. To study if this assumption is appropriate, we address the effects of drought on the infiltration behavior of forest soils using dye tracer experiments on six sites in three regions across Germany, which were forced into drought conditions. The sites cover clayey, loamy and sandy textured soils. In each region, we compared a deciduous and a coniferous forest stand to address differences between the main tree species. The results of the dye tracer experiments show clear evidence for changes in infiltration behavior at the sites. The infiltration changed at the clayey plots from regular and homogeneous flow to fast preferential flow. Similar behavior was observed at the loamy plots, where large areas in the upper layers remained dry, displaying signs of strong water repellency. This was confirmed by WDPT tests, which revealed, in all except one plot, moderate to severe water repellency. Water repellency was also accountable for the change of regular infiltration to fingered flow in the sandy soils. The results of this study suggest that the "drought-history" or generally the climatic conditions in the past of a soil are more important than the actual antecedent soil moisture status regarding hydrophobicity and infiltration behavior; and also, that drought effects on infiltration need to be considered in hydrological models to obtain realistic predictions concerning water quality and quantity in runoff and groundwater recharge.

Description: Size distribution and optical properties of mineral dust aerosols transported in the western Mediterranean Atmospheric Chemistry and Physics Discussions, 15, 21607-21669, 2015 Author(s): C. Denjean, F. Cassola, A. Mazzino, S. Triquet, S. Chevaillier, N. Grand, T. Bourrianne, G. Momboisse, K. Sellegri, A. Schwarzenbock, E. Freney, M. Mallet, and P. Formenti This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of tranport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried higher concentration of pollution particles at intermediate altitude (1–3 km) than at elevated altitude (〉 3 km), resulting in scattering Angstrom exponent up to 2.2 within the intermediate altitude. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate light absorption of the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00 ± 0.04. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assimilated to those of native dust in radiative transfer simulations, modeling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational dataset necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin.

Description: Identification of particulate organosulfates in three megacities at the middle and lower reaches of the Yangtze River Atmospheric Chemistry and Physics Discussions, 15, 21415-21448, 2015 Author(s): X. K. Wang, S. Rossignol, Y. Ma, L. Yao, M. Y. Wang, J. M. Chen, C. George, and L. Wang PM 2.5 filter samples have been collected in three megacities i.e., Wuhan (WH), Nanjing (NJ), and Shanghai (SH) at the middle and lower reaches of the Yangtze River, respectively. Analysis of those samples using an ultra-high performance liquid chromatography (UHPLC) coupled to an orbitrap mass spectrometer (MS) allowed detection of about two hundred particulate organosulfates (OSs), including dozens of nitrooxy-organosulfates, at each location. While aliphatic OSs represented more than 78 % of the detected OSs at the three locations, aromatic OSs were much less abundant. OSs with two to four isomers accounted for about 50 % of the total OSs on average in these megacities, and the percentage of OSs with six and more isomers in WH was more significant than those in SH and NJ. The average molecular weight, and the degrees of oxidation and saturation of OSs in the WH summer samples were greater than those in WH winter samples. In SH, the average molecular weight and the degree of oxidation of OSs in summer samples were greater than those in winter samples, but the degree of saturation was similar between the two seasons. In summer, the average molecular weight, and the degrees of oxidation and unsaturation of OSs were smallest in WH among the three cities. Between NJ and SH, the average molecular weight and the degree of saturation of OSs were close and the degree of oxidation of OSs in NJ was smaller. Kendrick mass defect diagrams and Van Krevelen diagrams indicated that the characteristics of identified OSs between in NJ and in SH shared better similarity. In addition, the identity and abundance of OSs in SH showed clear seasonal and diurnal variations. OSs in summer were more abundant than they were in winter due to stronger photochemical reactions in summer. The relative abundance of OSs at night was greater than that in the daytime and more nitrooxy-OSs existed at night, probably because of active NO 3 radical chemistry at night. In SH summer samples, OSs with 5 and 10 carbons (C 5 and C 10 ) were the most abundant, indicating the importance of isoprene and monoterpenes as precursors of OSs, whereas the relative abundances of OSs with 8, 9, and more than 14 carbons (C 8 , C 9 , and C 14+ ) were also high in SH winter samples, urging the need to further understand the precursors of OSs.

Description: The tropopause inversion layer in baroclinic life cycles experiments: the role of diabatic and mixing processes Atmospheric Chemistry and Physics Discussions, 15, 21495-21537, 2015 Author(s): D. Kunkel, P. Hoor, and V. Wirth Recent studies on the formation of a quasi-permanent layer of enhanced static stability above the thermal tropopause revealed the contributions of dynamical and radiative processes. Dry dynamics lead to the evolution of a tropopause inversion layer (TIL) which is, however, too weak compared to observations and thus diabatic contributions are required. In this study we aim to assess the importance of diabatic as well as mixing processes in the understanding of TIL formation at midlatitudes. The non-hydrostatic model COSMO is applied in an idealized mid-latitude channel configuration to simulate baroclinic life cycles. The effect of individual diabatic, i.e. related to humidity and radiation, and turbulent processes is studied first to estimate the additional contribution of these processes to dry dynamics. In a second step these processes are stepwise included in the model to increase the complexity and finally estimate the relative importance of each process. The results suggest that including turbulence leads to a weaker TIL than in a dry reference simulation. In contrast, the TIL evolves stronger when radiation is included but the temporal occurrence is still comparable to the reference. Using various cloud schemes in the model shows that latent heat release and consecutive increased vertical motions foster an earlier and stronger appearance of the TIL than in all other life cycles. Furthermore, updrafts moisten the upper troposphere and as such increase the radiative effect from water vapor. Particularly, this process becomes more relevant for maintaining the TIL during later stages of the life cycles. Increased convergence of the vertical wind induced by updrafts and by propagating and potentially dissipating inertia-gravity waves further contributes to the enhanced stability of the lower stratosphere. Furthermore, radiative feedback of ice clouds reaching up to the tropopause is identified to potentially further affect the strength of the TIL in the region of the cloud.

Description: Does the Budyko curve reflect a maximum power state of hydrological systems? A backward analysis Hydrology and Earth System Sciences Discussions, 12, 7821-7842, 2015 Author(s): M. Westhoff, E. Zehe, P. Archambeau, and B. Dewals Almost all catchments plot within a small envelope around the Budyko curve. This apparent behaviour suggests that organizing principles may play a role in the evolution of catchments. In this paper we applied the thermodynamic principle of maximum power as the organizing principle. In a top-down approach we derived mathematical formulations of the relation between relative wetness and gradients driving runoff and evaporation for a simple one-box model. We did this in such a way that when the conductances are optimized with the maximum power principle, the steady state behaviour of the model leads exactly to a point on the Budyko curve. Subsequently we derived gradients that, under constant forcing, resulted in a Budyko curve following the asymptotes closely. With these gradients we explored the sensitivity of dry spells and dynamics in actual evaporation. Despite the simplicity of the model, catchment observations compare reasonably well with the Budyko curves derived with dynamics in rainfall and evaporation. This indicates that the maximum power principle may be used (i) to derive the Budyko curve and (ii) to move away from the empiricism in free parameters present in many Budyko functions. Future work should focus on better representing the boundary conditions of real catchments and eventually adding more complexity to the model.