ALBERT

Description: The nonhydrostatic regional climate model CCLM was used for a long-term hindcast run (2002–2016) for the Weddell Sea region with resolutions of 15 and 5 km and two different turbulence parametrizations. CCLM was nested in ERA-Interim data and used in forecast mode (suite of consecutive 30 h long simulations with 6 h spin-up). We prescribed the sea ice concentration from satellite data and used a thermodynamic sea ice model. The performance of the model was evaluated in terms of temperature and wind using data from Antarctic stations, automatic weather stations (AWSs), an operational forecast model and reanalyses data, and lidar wind profiles. For the reference run we found a warm bias for the near-surface temperature over the Antarctic Plateau. This bias was removed in the second run by adjusting the turbulence parametrization, which results in a more realistic representation of the surface inversion over the plateau but resulted in a negative bias for some coastal regions. A comparison with measurements over the sea ice of the Weddell Sea by three AWS buoys for 1 year showed small biases for temperature around ±1 K and for wind speed of 1 m s−1. Comparisons of radio soundings showed a model bias around 0 and a RMSE of 1–2 K for temperature and 3–4 m s−1 for wind speed. The comparison of CCLM simulations at resolutions down to 1 km with wind data from Doppler lidar measurements during December 2015 and January 2016 yielded almost no bias in wind speed and a RMSE of ca. 2 m s−1. Overall CCLM shows a good representation of temperature and wind for the Weddell Sea region. Based on these encouraging results, CCLM at high resolution will be used for the investigation of the regional climate in the Antarctic and atmosphere–ice–ocean interactions processes in a forthcoming study.

Description: Low ozone and high water vapour mixing ratios are common features in the Asian summer monsoon (ASM) anticyclone; however, low ozone and low water vapour values were observed near the tropopause over Kunming, China, within the ASM using balloon-borne measurements performed during the SWOP (sounding water vapour, ozone, and particle) campaign in August 2009 and 2015. Here, we investigate low ozone and water vapour signatures in the upper troposphere and lower stratosphere (UTLS) using FengYun-2D, FengYun-2G, and Aura Microwave Limb Sounder (MLS) satellite measurements and backward trajectory calculations. Trajectories with kinematic and diabatic vertical velocities were calculated using the Chemical Lagrangian Model of the Stratosphere (CLaMS) trajectory module driven by both ERA-Interim and ERA5 reanalysis data. All trajectory calculations show that air parcels with low ozone and low water vapour values in the UTLS over Kunming measured by balloon-borne instruments originate from the western Pacific boundary layer. Deep convection associated with tropical cyclones over the western Pacific transports ozone-poor air from the marine boundary layer to the cold tropopause region. Subsequently, these air parcels are mixed into the strong easterlies on the southern side of the Asian summer monsoon anticyclone. Air parcels are dehydrated when passing the lowest temperature region (

Description: Emission of greenhouse gases (GHGs) and removals from land, including both anthropogenic and natural fluxes, require reliable quantification, including estimates of uncertainties, to support credible mitigation action under the Paris Agreement. This study provides a state-of-the-art scientific overview of bottom-up anthropogenic emissions data from agriculture, forestry and other land use (AFOLU) in the European Union (EU281). The data integrate recent AFOLU emission inventories with ecosystem data and land carbon models and summarize GHG emissions and removals over the period 1990–2016. This compilation of bottom-up estimates of the AFOLU GHG emissions of European national greenhouse gas inventories (NGHGIs), with those of land carbon models and observation-based estimates of large-scale GHG fluxes, aims at improving the overall estimates of the GHG balance in Europe with respect to land GHG emissions and removals. Whenever available, we present uncertainties, its propagation and role in the comparison of different estimates. While NGHGI data for the EU28 provide consistent quantification of uncertainty following the established IPCC Guidelines, uncertainty in the estimates produced with other methods needs to account for both within model uncertainty and the spread from different model results. The largest inconsistencies between EU28 estimates are mainly due to different sources of data related to human activity, referred to here as activity data (AD) and methodologies (tiers) used for calculating emissions and removals from AFOLU sectors. The referenced datasets related to figures are visualized at https://doi.org/10.5281/zenodo.3662371 (Petrescu et al., 2020).

Description: Biosphere–atmosphere interactions strongly influence the chemical composition of the atmosphere. Simulating these interactions at a detailed process-based level has traditionally been computationally intensive and resource prohibitive, commonly due to complexities in calculating radiation and light at the leaf level within plant canopies. Here we describe a surrogate canopy physics model based on the MEGAN3 detailed canopy model parameterized using a statistical learning technique. This surrogate canopy model is specifically designed to rapidly calculate leaf-level temperature and photosynthetically active radiative (PAR) for use in large-scale chemical transport models (CTMs). Our surrogate model can reproduce the dominant spatiotemporal variability of the more detailed MEGAN3 canopy model to within 10 % across the globe. Implementation of this surrogate model into the GEOS-Chem CTM leads to small local changes in ozone dry deposition velocities of less than 5 % and larger local changes in isoprene emissions of up to ∼40 %, though annual global isoprene emissions remain largely consistent (within 5 %). These changes to surface–atmosphere exchange lead to small changes in surface ozone concentrations of ±1 ppbv, modestly reducing the northern hemispheric ozone bias, which is common to many CTMs, here from 8 to 7 ppbv. The use of this computationally efficient surrogate canopy model drives emissions of isoprene and concentrations of surface ozone closer to observationally constrained values. Additionally, this surrogate model allows for the further development and implementation of leaf-level emission factors in the calculation of biogenic emissions in the GEOS-Chem CTM. Though not the focus of this work, this ultimately enables a complete implementation of the MEGAN3 emissions framework within GEOS-Chem, which produces 570 Tg yr−1 of isoprene for 2012.

Description: Biogenic volatile organic compounds (BVOCs) are important components of the atmosphere due to their contribution to atmospheric chemistry and biogeochemical cycles. Tropical forests are the largest source of the dominant BVOC emissions (e.g. isoprene and monoterpenes). In this study, we report isoprene and total monoterpene flux measurements with a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) using the eddy covariance (EC) method at the Tapajós National Forest (2.857∘ S, 54.959∘ W), a primary rainforest in eastern Amazonia. Measurements were carried out from 1 to 16 June 2014, during the wet-to-dry transition season. During the measurement period, the measured daytime (06:00–18:00 LT) average isoprene mixing ratios and fluxes were 1.15±0.60 ppb and 0.55±0.71 mg C m−2 h−1, respectively, whereas the measured daytime average total monoterpene mixing ratios and fluxes were 0.14±0.10 ppb and 0.20±0.25 mg C m−2 h−1, respectively. Midday (10:00–14:00 LT) average isoprene and total monoterpene mixing ratios were 1.70±0.49 and 0.24±0.05 ppb, respectively, whereas midday average isoprene and monoterpene fluxes were 1.24±0.68 and 0.46±0.22 mg C m−2 h−1, respectively. Isoprene and total monoterpene emissions in Tapajós were correlated with ambient temperature and solar radiation. Significant correlation with sensible heat flux, SHF (r2=0.77), was also observed. Measured isoprene and monoterpene fluxes were strongly correlated with each other (r2=0.93). The MEGAN2.1 (Model of Emissions of Gases and Aerosols from Nature version 2.1) model could simulate most of the observed diurnal variations (r2=0.7 to 0.8) but declined a little later in the evening for both isoprene and total monoterpene fluxes. The results also demonstrate the importance of site-specific vegetation emission factors (EFs) for accurately simulating BVOC fluxes in regional and global BVOC emission models.

Description: Cirque erosion contributes significantly to mountain denudation and is a key element of glaciated mountain topography. Despite long-standing efforts, rates of rockwall retreat and the proportional contributions of low-, mid- and high-magnitude rockfalls have remained poorly constrained. Here, a unique, terrestrial-lidar-derived rockfall inventory (2011–2017) of two glaciated cirques in the Hohe Tauern range, Central Alps, Austria, is analysed. The mean cirque wall retreat rate of 1.9 mm a−1 ranks in the top range of reported values and is mainly driven by enhanced rockfall from the lowermost, freshly deglaciated rockwall sections. Retreat rates are significantly elevated over decades subsequent to glacier downwasting. Elongated cirque morphology and recorded cirque wall retreat rates indicate headward erosion is clearly outpacing lateral erosion, most likely due to the cataclinal backwalls, which are prone to large dip-slope failures. The rockfall magnitude–frequency distribution – the first such distribution derived for deglaciating cirques – follows a distinct negative power law over 4 orders of magnitude. Magnitude–frequency distributions in glacier-proximal and glacier-distal rockwall sections differ significantly due to an increased occurrence of large rockfalls in recently deglaciated areas. In this paper, the second of two companion pieces, we show how recent climate warming shapes glacial landforms, controls spatiotemporal rockfall variation in glacial environments and indicates a transient signal with decadal-scale exhaustion of rockfall activity immediately following deglaciation crucial for future hazard assessments.

Description: Plants emit a diverse range of biogenic volatile organic compounds (BVOCs) whose oxidation leads to secondary organic aerosol (SOA) formation. The majority of studies of biogenic SOA have focused on single or simple multicomponent BVOC mixtures thought to be representative of Northern hemispheric deciduous or mixed forest conditions. Gaps remain in our understanding of SOA formation from complex mixtures of real plant emissions in other environments. Towards the goal of understanding SOA in other regions, we conducted the first comprehensive study of SOA from oxygenated monoterpenes. These are the dominant emissions from the most common plant species in southern California's coastal sage ecosystem: black sage (Salvia mellifera) and California sagebrush (Artemisia californica). Emissions from sage plants, as well as single compounds representing their major emissions (camphor, camphene and eucalyptol), were oxidised in an Aerodyne potential aerosol mass oxidation flow reactor (PAM-OFR). The chemical composition of SOA was characterised using a high-resolution time-of-flight iodide-anion chemical-ionisation mass spectrometer equipped with a Filter Inlet for Gases and AEROsols (FIGAERO-I-HR-ToF-CIMS) under low- and medium-NOx conditions. SOA from oxygenated monoterpenes showed a higher-order oligomer content and a greater presence of highly oxygenated organic molecules (HOMs) than non-oxygenated monoterpenes, with HOM contributing 27 %–47 % and 12 %–14 % of SOA product signal from oxygenated and non-oxygenated monoterpenes respectively. This study highlights the potential importance of oxygenated monoterpene emissions for SOA formation in woody shrub ecosystems.

Description: Volatile halogenated organic compounds (VHOCs), such as methyl halides (CH3X; X is Br, Cl and I) and very short-lived halogenated substances (VSLSs; bromoform – CHBr3, dibromomethane – CH2Br2, bromodichloromethane – CHBrCl2, trichloroethylene – C2HCl3, chloroform – CHCl3 – and dibromochloromethane – CHBr2Cl) are well known for their significant influence on ozone concentrations and oxidation capacity of the troposphere and stratosphere and for their key role in aerosol formation. Insufficient characterization of the sources and the emission rate of VHOCs limits our ability to understand and assess their impact in both the troposphere and stratosphere. Over the last two decades, several natural terrestrial sources for VHOCs, including soil and vegetation, have been identified, but our knowledge of emission rates from these sources and their responses to changes in ambient conditions remains limited. Here we report measurements of the mixing ratios and fluxes of several chlorinated and brominated VHOCs from different landscapes and natural and agricultural vegetated sites at the Dead Sea during different seasons. Fluxes were generally positive (emission into the atmosphere), corresponding to elevated mixing ratios, but were highly variable. Fluxes (and mixing ratios) for the investigated VHOCs ranged as follows: CHBr3 from −79 to 187 nmol m−2 d−1 (1.9 to 22.6 pptv), CH2Br2 from −55 to 71 nmol m−2 d−1 (0.7 to 19 pptv), CHBr2Cl from −408 to 768 nmol m−2 d−1 (0.4 to 11 pptv), CHBrCl2 from −29 to 45 nmol m−2 d−1 (0.5 to 9.6 pptv), CHCl3 from −577 to 883 nmol m−2 d−1 (15 to 57 pptv), C2HCl3 from −74 to 884 nmol m−2 d−1 (0.4 to 11 pptv), methyl chloride (CH3Cl) from -5300 to 10,800 nmol m−2 d−1 (530 to 730 pptv), methyl bromide (CH3Br) from −111 to 118 nmol m−2 d−1 (7.5 to 14 pptv) and methyl iodide (CH3I) from −25 to 17 nmol m−2 d−1 (0.4 to 2.8 pptv). Taking into account statistical uncertainties, the coastal sites (particularly those where soil is mixed with salt deposits) were identified as sources of all VHOCs, but this was not statistically significant for CHCl3. Further away from the coastal area, the bare soil sites were sources for CHBrCl2, CHBr2Cl, CHCl3, and probably also for CH2Br2 and CH3I, and the agricultural sites were sources for CHBr3, CHBr2Cl and CHBrCl2. In contrast to previous reports, we also observed emissions of brominated trihalomethanes, with net molar fluxes ordered as follows: CHBr2Cl 〉 CHCl3 〉 CHBr3 〉 CHBrCl2 and lowest positive flux incidence for CHCl3 among all trihalomethanes; this finding can be explained by the soil's enrichment with Br. Correlation analysis, in agreement with recent studies, indicated common controls for the emission of CHBr2Cl and CHBrCl2 and likely also for CHBr3. There were no indications for correlation of the brominated trihalomethanes with CHCl3. Also in line with previous reports, we observed elevated emissions of CHCl3 and C2HCl3 from mixtures of soil and different salt-deposited structures; the flux correlations between these compounds and methyl halides (particularly CH3I) suggested that at least CH3I is also emitted via similar mechanisms or is subjected to similar controls. Overall, our results indicate elevated emission of VHOCs from bare soil under semiarid conditions. Along with other recent studies, our findings point to the strong emission potential of a suite of VHOCs from saline soils and salt lakes and call for additional studies of emission rates and mechanisms of VHOCs from saline soils and salt lakes.

Description: Here we report the measurement results of nitrous acid (HONO) and a suite of relevant parameters on the NCAR C-130 research aircraft in the southeastern US during the NOMADSS 2013 summer field study. The daytime HONO concentration ranged from low parts per trillion by volume (pptv) in the free troposphere (FT) to mostly within 5–15 pptv in the background planetary boundary layer (PBL). There was no discernible vertical HONO gradient above the lower flight altitude of 300 m in the PBL, and the transport of ground surface HONO was not found to be a significant contributor to the tropospheric HONO budget. The total in situ HONO source mean (±1 SD) was calculated as 53 (±21) pptv h−1 during the day. The upper-limit contribution from NOx-related reactions was 10 (±5) pptv h−1, and the contribution from photolysis of particulate nitrate (pNO3) was 38 (±23) pptv h−1, based on the measured pNO3 concentrations and the median pNO3 photolysis rate constant of 2.0 × 10−4 s−1 determined in the laboratory using ambient aerosol samples. The photolysis of HONO contributed to less than 10 % of the primary OH source. However, a recycling NOx source via pNO3 photolysis was equivalent to ∼ 2.3 × 10−6 mol m−2 h−1 in the air column within the PBL, a considerable supplementary NOx source in the low-NOx background area. Up to several tens of parts per trillion by volume of HONO were observed in power plant and urban plumes during the day, mostly produced in situ from precursors including NOx and pNO3. Finally, there was no observable accumulation of HONO in the nocturnal residual layer and the nocturnal FT in the background southeastern US, with an increase in the HONO ∕ NOx ratio of ≤ 3 × 10−4 h−1 after sunset.

Description: Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m−3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O:C up to O:C∼1.0, and then decreased as O:C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C=C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign, multilinear regression analysis was performed between measured SOA formation and the concentration of gas-phase tracers representing different precursor sources. The majority of SOA-forming gases present during both seasons were of biogenic origin. Urban sources also contributed substantially in both seasons, while biomass burning sources were more important during the dry season. This study enables a better understanding of SOA formation in environments with diverse emission sources.