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Global combustion sources of organic aerosols: model comparison with 84 AMS factor-analysis data sets

Emissions of organic compounds from biomass, biofuel, and fossil fuel combustion strongly influence the global atmospheric aerosol load. Some of the organics are directly released as primary organic aerosol (POA). Most are emitted in the gas phase and undergo chemical transformations (i.e., oxidation by hydroxyl radical) and form secondary organic aerosol (SOA). In this work we use the global chemistry climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) with a computationally efficient module for the description of organic aerosol (OA) composition and evolution in the atmosphere (ORACLE). The tropospheric burden of open biomass and anthropogenic (fossil and biofuel) combustion particles is estimated to be 0.59 and 0.63 Tg, respectively, accounting for about 30 and 32 % of the total tropospheric OA load. About 30 % of the open biomass burning and 10 % of the anthropogenic combustion aerosols originate from direct particle emissions, whereas the rest is formed in the atmosphere. A comprehensive data set of aerosol mass spectrometer (AMS) measurements along with factor-analysis results from 84 field campaigns across the Northern Hemisphere are used to evaluate the model results. Both the AMS observations and the model results suggest that over urban areas both POA (25–40 %) and SOA (60–75 %) contribute substantially to the overall OA mass, whereas further downwind and in rural areas the POA concentrations decrease substantially and SOA dominates (80–85 %). EMAC does a reasonable job in reproducing POA and SOA levels during most of the year. However, it tends to underpredict POA and SOA concentrations during winter indicating that the model misses wintertime sources of OA (e.g., residential biofuel use) and SOA formation pathways (e.g., multiphase oxidation).
Boundary-layer turbulent processes and mesoscale variability represented by numerical weather prediction models during the BLLAST campaign

This study evaluates the ability of three operational models, with resolution varying from 2.5 to 16 km, to predict the boundary-layer turbulent processes and mesoscale variability observed during the Boundary Layer Late-Afternoon and Sunset Turbulence (BLLAST) field campaign. We analyse the representation of the vertical profiles of temperature and humidity and the time evolution of near-surface atmospheric variables and the radiative and turbulent fluxes over a total of 12 intensive observing periods (IOPs), each lasting 24 h. Special attention is paid to the evolution of the turbulent kinetic energy (TKE), which was sampled by a combination of independent instruments. For the first time, this variable, a central one in the turbulence scheme used in AROME and ARPEGE, is evaluated with observations. In general, the 24 h forecasts succeed in reproducing the variability from one day to another in terms of cloud cover, temperature and boundary-layer depth. However, they exhibit some systematic biases, in particular a cold bias within the daytime boundary layer for all models. An overestimation of the sensible heat flux is noted for two points in ARPEGE and is found to be partly related to an inaccurate simplification of surface characteristics. AROME shows a moist bias within the daytime boundary layer, which is consistent with overestimated latent heat fluxes. ECMWF presents a dry bias at 2 m above the surface and also overestimates the sensible heat flux. The high-resolution model AROME resolves the vertical structures better, in particular the strong daytime inversion and the thin evening stable boundary layer. This model is also able to capture some specific observed features, such as the orographically driven subsidence and a well-defined maximum that arises during the evening of the water vapour mixing ratio in the upper part of the residual layer due to fine-scale advection. The model reproduces the order of magnitude of spatial variability observed at mesoscale (a few tens of kilometres). AROME provides a good simulation of the diurnal variability of the turbulent kinetic energy, while ARPEGE shows the right order of magnitude.
HCOOH distributions from IASI for 2008–2014: comparison with ground-based FTIR measurements and a global chemistry-transport model

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the sources and sinks of HCOOH and therefore HCOOH is misrepresented by global chemistry-transport models. This work presents global distributions from 2008 to 2014 as derived from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI), based on conversion factors between brightness temperature differences and representative retrieved total columns over seven regions: Northern Africa, southern Africa, Amazonia, Atlantic, Australia, Pacific, and Russia. The dependence of the measured HCOOH signal on the thermal contrast is taken into account in the conversion method. This conversion presents errors lower than 20 % for total columns ranging between 0.5 and 1 × 1016 molec cm−2 but reaches higher values, up to 78 %, for columns that are lower than 0.3 × 1016 molec cm−2. Signatures from biomass burning events are highlighted, such as in the Southern Hemisphere and in Russia, as well as biogenic emission sources, e.g., over the eastern USA. A comparison between 2008 and 2014 with ground-based Fourier transform infrared spectroscopy (FTIR) measurements obtained at four locations (Maido and Saint-Denis at La Réunion, Jungfraujoch, and Wollongong) is shown. Although IASI columns are found to correlate well with FTIR data, a large bias (> 100 %) is found over the two sites at La Réunion. A better agreement is found at Wollongong with a negligible bias. The comparison also highlights the difficulty of retrieving total columns from IASI measurements over mountainous regions such as Jungfraujoch. A comparison of the retrieved columns with the global chemistry-transport model IMAGESv2 is also presented, showing good representation of the seasonal and interannual cycles over America, Australia, Asia, and Siberia. A global model underestimation of the distribution and a misrepresentation of the seasonal cycle over India are also found. A small positive trend in the IASI columns is observed over Australia, Amazonia, and India over the 2008–2014 period (from 0.7 to 1.5 % year−1), while a decrease of ∼ 0.8 % year−1 is measured over Siberia.
Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative correlation with the SSA NR-OM volume fractions after the peak of the blooms (i.e., Chl a maxima); i.e., the GF(85 %) values generally decreased when the NR-OM volume fractions increased. The GF(85 %) vs. NR-OM volume fraction relationship was interpreted using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule and used to estimate the GF(85 %) of the organic matter in the nascent SSA. The estimated pure NR-OM GF(85 %) values were 1.16 ± 0.09 and 1.23 ± 0.10 for the indoor and outdoor MARTS, respectively. These measurements demonstrate a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.
Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

In this work, the Aerodyne soot particle – aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m−3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ∼ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter) were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA) yielded four OA subcomponents, including hydrocarbon-like OA (HOA), cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The bivariate polar plots show that the SV-OOA was formed locally, and the variations of hydrogen-to-carbon (H ∕ C) and oxygen-to-carbon (O ∕ C) ratios in the Van Krevelen space further suggests an evolution pathway of SV-OOA to LV-OOA. Our findings regarding springtime aerosol chemistry in Nanjing may have important implications for the air quality remediation in the densely populated regions.
Upper-tropospheric CO and O3 budget during the Asian summer monsoon

During the Asian summer monsoon, the circulation in the upper troposphere/lower stratosphere (UTLS) is dominated by the Asian monsoon anticyclone (AMA). Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the Eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3) and its precursors, such as carbon monoxide (CO) and nitrogen oxides (NOx). Many studies based on global modeling and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN) into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the MetOp-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9 % and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26 % but the correlation between both is high (0.94). GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼  25 ppbv) than East Asian emissions (∼  10 ppbv). The correlation between enhanced emissions over the Indo-Gangetic Plain and monsoon deep convection is responsible for this larger impact. Consistently, South Asian anthropogenic NOx emissions also play a larger role in producing O3 within the AMA (∼  8 ppbv) than East Asian emissions (∼  5 ppbv), but Asian lightning-produced NOx is responsible for the largest O3 production (10–14 ppbv). Stratosphere-to-troposphere exchanges are also important in transporting O3 in the upper part of the AMA.
Increasing summer net CO2 uptake in high northern ecosystems inferred from atmospheric inversions and comparisons to remote-sensing NDVI

Warmer temperatures and elevated atmospheric CO2 concentrations over the last several decades have been credited with increasing vegetation activity and photosynthetic uptake of CO2 from the atmosphere in the high northern latitude ecosystems: the boreal forest and arctic tundra. At the same time, soils in the region have been warming, permafrost is melting, fire frequency and severity are increasing, and some regions of the boreal forest are showing signs of stress due to drought or insect disturbance. The recent trends in net carbon balance of these ecosystems, across heterogeneous disturbance patterns, and the future implications of these changes are unclear. Here, we examine CO2 fluxes from northern boreal and tundra regions from 1985 to 2012, estimated from two atmospheric inversions (RIGC and Jena). Both used measured atmospheric CO2 concentrations and wind fields from interannually variable climate reanalysis. In the arctic zone, the latitude region above 60° N excluding Europe (10° W–63° E), neither inversion finds a significant long-term trend in annual CO2 balance. The boreal zone, the latitude region from approximately 50–60° N, again excluding Europe, showed a trend of 8–11 Tg C yr−2 over the common period of validity from 1986 to 2006, resulting in an annual CO2 sink in 2006 that was 170–230 Tg C yr−1 larger than in 1986. This trend appears to continue through 2012 in the Jena inversion as well. In both latitudinal zones, the seasonal amplitude of monthly CO2 fluxes increased due to increased uptake in summer, and in the arctic zone also due to increased fall CO2 release. These findings suggest that the boreal zone has been maintaining and likely increasing CO2 sink strength over this period, despite browning trends in some regions and changes in fire frequency and land use. Meanwhile, the arctic zone shows that increased summer CO2 uptake, consistent with strong greening trends, is offset by increased fall CO2 release, resulting in a net neutral trend in annual fluxes. The inversion fluxes from the arctic and boreal zones covering the permafrost regions showed no indication of a large-scale positive climate–carbon feedback caused by warming temperatures on high northern latitude terrestrial CO2 fluxes from 1985 to 2012.
The importance of plume rise on the concentrations and atmospheric impacts of biomass burning aerosol

We quantified the effects of the plume rise of biomass burning aerosol and gases for the forest fires that occurred in Saskatchewan, Canada, in July 2010. For this purpose, simulations with different assumptions regarding the plume rise and the vertical distribution of the emissions were conducted. Based on comparisons with observations, applying a one-dimensional plume rise model to predict the injection layer in combination with a parametrization of the vertical distribution of the emissions outperforms approaches in which the plume heights are initially predefined. Approximately 30 % of the fires exceed the height of 2 km with a maximum height of 8.6 km. Using this plume rise model, comparisons with satellite images in the visible spectral range show a very good agreement between the simulated and observed spatial distributions of the biomass burning plume. The simulated aerosol optical depth (AOD) with data of an AERONET station is in good agreement with respect to the absolute values and the timing of the maximum. Comparison of the vertical distribution of the biomass burning aerosol with CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) retrievals also showed the best agreement when the plume rise model was applied. We found that downwelling surface short-wave radiation below the forest fire plume is reduced by up to 50 % and that the 2 m temperature is decreased by up to 6 K. In addition, we simulated a strong change in atmospheric stability within the biomass burning plume.
Model-based aviation advice on distal volcanic ash clouds by assimilating aircraft in situ measurements

The forecast accuracy of distal volcanic ash clouds is important for providing valid aviation advice during volcanic ash eruption. However, because the distal part of volcanic ash plume is far from the volcano, the influence of eruption information on this part becomes rather indirect and uncertain, resulting in inaccurate volcanic ash forecasts in these distal areas. In our approach, we use real-life aircraft in situ observations, measured in the northwestern part of Germany during the 2010 Eyjafjallajökull eruption, in an ensemble-based data assimilation system combined with a volcanic ash transport model to investigate the potential improvement on the forecast accuracy with regard to the distal volcanic ash plume. We show that the error of the analyzed volcanic ash state can be significantly reduced through assimilating real-life in situ measurements. After a continuous assimilation, it is shown that the aviation advice for Germany, the Netherlands and Luxembourg can be significantly improved. We suggest that with suitable aircrafts measuring once per day across the distal volcanic ash plume, the description and prediction of volcanic ash clouds in these areas can be greatly improved.
Large XCH4 anomaly in summer 2013 over northeast Asia observed by GOSAT

Extremely high levels of column-averaged dry-air mole fractions of atmospheric methane (XCH4) were detected in August and September 2013 over northeast Asia (∼  20 ppb above the averaged summertime XCH4 over 2009–2012, after removing a long-term trend), as being retrieved from the Short-Wavelength InfraRed (SWIR) spectral data observed with the Thermal And Near-infrared Sensor for carbon Observation – Fourier Transform Spectrometer (TANSO-FTS) onboard Greenhouse Gases Observing Satellite (GOSAT). Similar enhancements of XCH4 were also observed by the ground-based measurements at two Total Carbon Column Observing Network (TCCON) sites in Japan. The analysis of surface CH4 concentrations observed at three monitoring sites around the Japan archipelago suggest that the extreme increase of XCH4 has occurred in a limited area. The model analysis was conducted to investigate this anomalously high XCH4 event, using an atmospheric transport model. The results indicate that the extreme increase of XCH4 is attributed to the anomalous atmospheric pressure pattern over East Asia during the summer of 2013, which effectively transported the CH4-rich air to Japan from the strong CH4 source areas in east China. The two Japanese TCCON sites, ∼  1000 km east–west apart each other, coincidentally located along the substantially CH4-rich air flow from east China. This analysis demonstrates the capability of GOSAT to monitor an XCH4 event on a synoptic scale. We anticipate that the synoptic information of XCH4 from GOSAT data contributes to improve our understanding of regional carbon cycle and the regional flux estimation.