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Deforestation and drainage has made Indonesian peatlands susceptible to burning. Large fires occur regularly, destroying agricultural crops and forest, emitting large amounts of CO 2 and air pollutants, resulting in adverse health effects. In order to reduce fire, the Indonesian government has committed to restore 2.49 Mha of degraded peatland, with an estimated cost of US$3.2-7 billion. Here we combine fire emissions and land cover data to estimate the 2015 fires, the largest in recent years, resulted in economic losses totalling US$28 billion, whilst the six largest fire events between 2004 and 2015 caused a total of US$93.9 billion in economic losses. We estimate that if restoration had already been completed, the area burned in 2015 would have been reduced by 6%, reducing CO 2 emissions by 18%, and PM 2.5 emissions by 24%, preventing 12,000 premature mortalities. Peatland restoration could have resulted in economic savings of US$8.4 billion for 2004–2015, making it a cost-effective strategy for reducing the impacts of peatland fires to the environment, climate and human health. Deforestation and drainage have made Indonesian peatlands susceptible to burning. Here the authors find that Indonesia’s 2015 fires resulted in economic losses totaling US$28 billion, while the area burned and emissions released could have been significantly reduced had restoration been completed.

Nitrous acid (HONO) is a precursor of the hydroxyl radical in the atmosphere, which controls the degradation of greenhouse gases, contributes to photochemical smog and ozone production, and influences air quality. Although biomass burning is known to contribute substantially to global aerosols and reactive gas emissions, pyrogenic contributions to HONO emissions are poorly constrained and often omitted in models. Here we present a global survey of TROPOMI/Sentinel-5 Precursor satellite sounder observations and show that HONO emissions are consistently enhanced in fresh wildfire plumes. Comparing major ecosystems (savanna, grassland, shrubland and tropical and extratropical forests), we found that the enhancement ratios of HONO to nitrogen dioxide varied systematically with biome type, with the lowest in savannas and grasslands and highest in extratropical evergreen forests. Supported by airborne measurements, we demonstrate that previous assessments underestimate pyrogenic HONO emissions by a factor of 2–4 across all ecosystem types. We estimate that HONO emissions are responsible for two-thirds of the hydroxyl radical production in fresh wildfire plumes worldwide and act to accelerate oxidative plume chemistry and ozone production. Our findings suggest that pyrogenic HONO emissions have a substantial impact on atmospheric composition, which enhances regional ozone levels by up to 7 ppbv.Satellite observations reveal that fresh wildfire plumes are a globally important source of nitrous acid, enhancing oxidative plume chemistry and regional ozone levels.

The effect of dry and wet deposition of semi-volatile organic compounds (SVOCs) in the gas phase on the concentrations of secondary organic aerosol (SOA) is reassessed using recently derived water solubility information. The water solubility of SVOCs was implemented as a function of their volatility distribution within the WRF-Chem regional chemistry transport model, and simulations were carried out over the continental United States for the year 2010. Results show that including dry and wet removal of gas-phase SVOCs reduces annual average surface concentrations of anthropogenic and biogenic SOA by 48 and 63% respectively over the continental US. Dry deposition of gas-phase SVOCs is found to be more effective than wet deposition in reducing SOA concentrations (−40 vs. −8% for anthropogenics, and −52 vs. −11% for biogenics). Reductions for biogenic SOA are found to be higher due to the higher water solubility of biogenic SVOCs. The majority of the total mass of SVOC + SOA is actually deposited via the gas phase (61% for anthropogenics and 76% for biogenics). Results are sensitive to assumptions made in the dry deposition scheme, but gas-phase deposition of SVOCs remains crucial even under conservative estimates. Considering reactivity of gas-phase SVOCs in the dry deposition scheme was found to be negligible. Further sensitivity studies where we reduce the volatility of organic matter show that consideration of gas-phase SVOC removal still reduces average SOA concentrations by 31% on average. We consider this a lower bound for the effect of gas-phase SVOC removal on SOA concentrations. A saturation effect is observed for Henry's law constants above 108 M atm−1, suggesting an upper bound of reductions in surface level SOA concentrations by 60% through removal of gas-phase SVOCs. Other models that do not consider dry and wet removal of gas-phase SVOCs would hence overestimate SOA concentrations by roughly 50%. Assumptions about the water solubility of SVOCs made in some current modeling systems (H* = H* (CH3COOH); H* = 105 M atm−1; H* = H* (HNO3)) still lead to an overestimation of 35%/25%/10% compared to our best estimate.

A suite of offline and real-time gas- and particle-phase measurements was deployed at Look Rock, Tennessee (TN), during the 2013 Southern Oxidant and Aerosol Study (SOAS) to examine the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol (SOA) formation. High- and low-time-resolution PM2.5 samples were collected for analysis of known tracer compounds in isoprene-derived SOA by gas chromatography/electron ionization-mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography/diode array detection-electrospray ionization-high-resolution quadrupole time-of-flight mass spectrometry (UPLC/DAD-ESI-HR-QTOFMS). Source apportionment of the organic aerosol (OA) was determined by positive matrix factorization (PMF) analysis of mass spectrometric data acquired on an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Campaign average mass concentrations of the sum of quantified isoprene-derived SOA tracers contributed to ~ 9 % (up to 28 %) of the total OA mass, with isoprene-epoxydiol (IEPOX) chemistry accounting for ~ 97 % of the quantified tracers. PMF analysis resolved a factor with a profile similar to the IEPOX-OA factor resolved in an Atlanta study and was therefore designated IEPOX-OA. This factor was strongly correlated (r2 > 0.7) with 2-methyltetrols, C5-alkene triols, IEPOX-derived organosulfates, and dimers of organosulfates, confirming the role of IEPOX chemistry as the source. On average, IEPOX-derived SOA tracer mass was ~ 26 % (up to 49 %) of the IEPOX-OA factor mass, which accounted for 32 % of the total OA. A low-volatility oxygenated organic aerosol (LV-OOA) and an oxidized factor with a profile similar to 91Fac observed in areas where emissions are biogenic-dominated were also resolved by PMF analysis, whereas no primary organic aerosol (POA) sources could be resolved. These findings were consistent with low levels of primary pollutants, such as nitric oxide (NO ~ 0.03 ppb), carbon monoxide (CO ~ 116 ppb), and black carbon (BC ~ 0.2 μg m−3). Particle-phase sulfate is fairly correlated (r2 ~ 0.3) with both methacrylic acid epoxide (MAE)/hydroxymethyl-methyl-α-lactone (HMML)- (henceforth called methacrolein (MACR)-derived SOA tracers) and IEPOX-derived SOA tracers, and more strongly correlated (r2 ~ 0.6) with the IEPOX-OA factor, in sum suggesting an important role of sulfate in isoprene SOA formation. Moderate correlation between the MACR-derived SOA tracer 2-methylglyceric acid with sum of reactive and reservoir nitrogen oxides (NOy; r2 = 0.38) and nitrate (r2 = 0.45) indicates the potential influence of anthropogenic emissions through long-range transport. Despite the lack of a clear association of IEPOX-OA with locally estimated aerosol acidity and liquid water content (LWC), box model calculations of IEPOX uptake using the simpleGAMMA model, accounting for the role of acidity and aerosol water, predicted the abundance of the IEPOX-derived SOA tracers 2-methyltetrols and the corresponding sulfates with good accuracy (r2 ~ 0.5 and ~ 0.7, respectively). The modeling and data combined suggest an anthropogenic influence on isoprene-derived SOA formation through acid-catalyzed heterogeneous chemistry of IEPOX in the southeastern US. However, it appears that this process was not limited by aerosol acidity or LWC at Look Rock during SOAS. Future studies should further explore the extent to which acidity and LWC as well as aerosol viscosity and morphology becomes a limiting factor of IEPOX-derived SOA, and their modulation by anthropogenic emissions.

New pathways to form secondary organic aerosol (SOA) have been postulated recently. Glyoxal, the smallest dicarbonyl, is one of the proposed precursors. It has both anthropogenic and biogenic sources, and readily partitions into the aqueous phase of cloud droplets and deliquesced particles where it undergoes both reversible and irreversible chemistry. In this work we extend the regional scale chemistry transport model WRF-Chem to include detailed gas-phase chemistry of glyoxal formation as well as a state-of-the-science module describing its partitioning and reactions in the aerosol aqueous-phase. A comparison of several proposed mechanisms is performed to quantify the relative importance of different formation pathways and their regional variability. The CARES/CalNex campaigns over California in summer 2010 are used as case studies to evaluate the model against observations. A month-long simulation over the continental United States (US) enables us to extend our results to the continental scale. In all simulations over California, the Los Angeles (LA) basin was found to be the hot spot for SOA formation from glyoxal, which contributes between 1% and 15% of the model SOA depending on the mechanism used. Our results indicate that a mechanism based only on a reactive (surface limited) uptake coefficient leads to higher SOA yields from glyoxal compared to a more detailed description that considers aerosol phase state and chemical composition. In the more detailed simulations, surface uptake is found to give the highest SOA mass yields compared to a volume process and reversible formation. We find that the yields of the latter are limited by the availability of glyoxal in aerosol water, which is in turn controlled by an increase in the Henry's law constant depending on salt concentrations (\"salting-in\"). A time dependence in this increase prevents substantial partitioning of glyoxal into aerosol water at high salt concentrations. If this limitation is removed, volume pathways contribute > 20% of glyoxal-SOA mass, and the total mass formed (5.8% of total SOA in the LA basin) is about a third of the simple uptake coefficient formulation without consideration of aerosol phase state and composition. Results from the continental US simulation reveal the much larger potential to form glyoxal-SOA over the eastern continental US. Interestingly, the low concentrations of glyoxal-SOA over the western continental US are not due to the lack of a potential to form glyoxal-SOA here. Rather these small glyoxal-SOA concentrations reflect dry conditions and high salt concentrations, and the potential to form SOA mass here will strongly depend on the water associated with particles.

This study examines the effect of a typical pre-monsoon season dust storm on tropospheric chemistry through a case study in northern India. Dust can alter photolysis rates by scattering and absorbing solar radiation and provide surface area for heterogeneous reactions. We use the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to simulate the dust storm that occurred during 17–22 April 2010 and investigate the contribution of different processes on mixing ratios of several key trace gases including ozone, nitrogen oxides, hydrogen oxides, methanol, acetic acid and formaldehyde. We revised the Fast Troposphere Ultraviolet Visible (F-TUV) photolysis scheme to include effects of dust aerosols on photolysis rates in a manner consistent with the calculations of aerosol optical properties for feedback to the meteorology radiation schemes. In addition, we added 12 heterogeneous reactions on the dust surface, for which 6 reactions have relative-humidity-dependent reactive uptake coefficients (γ). The inclusion of these processes in WRF-Chem is found to reduce the difference between observed and modeled O3 from 16 ± 9 to 2 ± 8 ppbv and that in NOy from 2129 ± 1425 to 372 ± 1225 pptv compared to measurements at the high-altitude site Nainital in the central Himalayas, and reduce biases by up to 30% in tropospheric column NO2 compared to OMI retrievals. The simulated dust storm acted as a sink for all the trace gases examined here and significantly perturbed their spatial and vertical distributions. The reductions in these gases are estimated as 5–100%, and more than 80% of this reduction was due to heterogeneous chemistry. The RH dependence of γ is also found to have substantial impact on the distribution of trace gases, with changes of up to 20–25% in O3 and HO2, 50% in H2O2 and 100% in HNO3. A set of sensitivity analyses revealed that dust aging could change H2O2 and CH3COOH levels by up to 50% but has a relatively small impact on other gases.

Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3-) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 mu m) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3- is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3- and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas-aerosol phase partitioning.

On June 24th 2018 one of the largest UK wildfires in recent history broke out on Saddleworth Moor, close to Manchester, in north-west England. Since wildfires close to large populations in the UK have been relatively small and rare in the past, there is little knowledge about the impacts. This has prevented the development of effective strategies to reduce them. This paper uses a high-resolution coupled atmospheric-chemistry model to assess the impact of the fires on particulate matter with a diameter less than 2.5 µm (PM2.5) across the region and the impact on health from short-term exposure. We find that the fires substantially degraded air quality. PM2.5 concentrations increased by more than 300% in Oldham and Manchester and up to 50% in areas up to 80 km away such as Liverpool and Wigan. This led to one quarter of the population (2.9 million people) in the simulation domain (−4.9-0.7°E and 53.0-54.4°N) being exposed to moderate PM2.5 concentrations on at least one day, according to the Daily Air Quality Index (36-53 µg m−3), between June 23rd and 30th 2018. This equates to 4.5 million people being exposed to PM2.5 above the WHO 24-hour guideline of 25 µg m−3 on at least one day. Using a concentration-response function we calculate the short-term health impact, which indicates that in total over the 7-day period 28 (95% CI: 14.1-42.1) deaths were brought forward, with a mean daily excess mortality of 3.5 deaths per day (95% CI: 1.8-5.3). The excess mortalities from PM2.5 from the fires represented up to 60% of the total excess mortality (5.7 of 9.5 excess deaths), representing an increase of 3.8 excess mortalities (165% increase) compared to if there were no fires. We find the impact of mortality due to PM2.5 from the fires on the economy was also substantial (£21.1 m).

Clouds are reaction chambers for atmospheric trace gases and aerosols, and the associated precipitation is a major sink for atmospheric constituents. The regional chemistry-climate model COSMO-ART has been lacking a description of wet scavenging of gases and aqueous-phase chemistry. In this work we present a coupling of COSMO-ART with a wet scavenging and aqueous-phase chemistry scheme. The coupling is made consistent with the cloud microphysics scheme of the underlying meteorological model COSMO. While the choice of the aqueous-chemistry mechanism is flexible, the effects of a simple sulfur oxidation scheme are shown in the application of the coupled system in this work. We give details explaining the coupling and extensions made, then present results from idealized flow-over-hill experiments in a 2-D model setup and finally results from a full 3-D simulation. Comparison against measurement data shows that the scheme efficiently reduces SO2 trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O3 and NOx unchanged. PM10 aerosol mass was increased by 10% on average. While total PM2.5 changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m−3 (up to −2 μg m−3 in the Po Valley) while sulfate mass is increased by 1–1.5 μg m−3 on average (up to 2.5 μg m−3 in Eastern Europe). The effect of cloud processing of aerosols on its size distribution, i.e. a shift towards larger diameters, is observed. Compared against wet deposition measurements the system tends to underestimate the total wet deposited mass for the simulated case study.

A volatility basis set (VBS) approach for the simulation of secondary organic aerosol (SOA) formation is incorporated in the online coupled atmospheric model system COSMO-ART and applied over Europe during the EUCAARI May 2008 campaign. Organic aerosol performance is improved when compared to the default SOA module of COSMO-ART (SORGAM) against high temporal resolution aerosol mass spectrometer ground measurements. The impact of SOA on the overall radiative budget was investigated. The mean direct surface radiative cooling averaged over Europe is −1.2 W m−2, representing approximately 20% of the total effect of aerosols on the radiative budget. However, responses are not spatially correlated with the radiative forcing, due to the nonlinear interactions among changes in particle chemical composition, water content, size distribution and cloud cover. These interactions initiated~by the effect of SOA on radiation are found to result even in a positive forcing in specific areas. Further model experiments showed that the availability of nitrogen oxides slightly affects SOA production, but that the aging rate constant used in the VBS approximation and boundary concentrations assumed in the model should be carefully selected. The aging of SOA is found to reduce hourly nitrate levels by up to 30%, while the condensation of inorganic species upon pre-existing, SOA-rich particles results in a monthly average increase of 5% in sulfate and ammonium formation in the accumulation mode.