Biomass Burning Regions Research Articles

Spatio-temporal variations of tropospheric nitrogen dioxide in South Mato Grosso based on remote sensing by satellite

The study evaluates the characteristics of tropospheric nitrogen dioxide (NO2) concentrations from 2005 to 2020 in eight cities in the State of Mato Grosso do Sul (MS), Midwestern Brazil, using data available from the Ozone Monitoring Instrument (OMI). The average concentration varies from 2981 × 1015 molecules/cm2 in Campo Grande, where commercial, industrial and vehicular activities take place, to 2906 × 1015 molecules/cm2 in Corumbá and 3035 × 1015 molecules/cm2 in Porto Murtinho, regions of livestock and biomass burning. The results, based on the Mann–Kendall (MK) test, show a significant increase (p < 0.05) in the NO2 column levels in the region. For each of the eight cities studied, a significant seasonal cycle of NO2 columns was determined. The maximum value of NO2 concentration was observed in the dry period, from July to September, while the minimum value was registered in the rainy period, from October to March.Supplementary InformationThe online version contains supplementary material available at 10.1007/s00703-021-00855-5.

Assessment of the Contribution of Local and Regional Biomass Burning on PM2.5 in New York/New Jersey Metropolitan Area

The sources of fine particulate matter (PM2.5, particles with diameter < 2.5 μm) in four monitoring sites in the New York/New Jersey metropolitan statistical area from 2007 to 2017 was apportioned by positive matrix factorization (PMF) of chemical speciation data. Biomass burning, secondary inorganic (i.e., ammonium sulfate and nitrate) and primary traffic exhausts were the predominant PM2.5 sources. The declining trends of PM2.5 mass in all four sites were very well correlated with decreasing secondary sulfate levels due to SO2 emission reductions by coal-fired power plants. The contributions of secondary nitrate, primary traffic exhausts and diesel particles did not change (or slightly increased) over time except for the Queens site, where statistically significant declines were computed. Biomass burning contributions increased in the Queens and Chester sites but declined in the Division Str and Elizabeth Lab sites, although significant interannual variability was observed. Wintertime biomass burning aerosols were most likely due to combustion of contemporary biomass for industrial and domestic heating, and it was linked to the intensity (average minimum temperature) and duration (number of freezing days) of cold weather. The annual summertime biomass burning contributions were correlated with the number and area burnt by lightning-ignited wildfires. These results indicate that PM2.5 sources in urban environments is changing from anthropogenic secondary sulfate and nitrate to carbonaceous aerosol from local anthropogenic and regional climate-driven biomass burning. This trend may counterbalance emissions controls on anthropogenic activities and modify the biological and toxicological responses and resultant health effects.

In-vitro oxidative potential and inflammatory response of ambient PM2.5 in a rural region of Northwest China: Association with chemical compositions and source contribution

Overproduction of reactive oxygen species (ROS) induced by atmospheric particles and subsequent inflammatory responses are considered as one of the most important pathological mechanisms with regard to the adverse effects of air pollution exposure. In this study, fine particulate matter (PM2.5) samples were collected at a rural site in Guanzhong Basin, Northwest China, in both summer (August 3–23, 2016) and winter (January 5–February 1, 2017). Then, human bronchial epithelial BEAS-2B cells were exposed to the PM2.5, cultured for 24 h, and then assayed for particle-induced ROS and three inflammatory factors (tumor necrosis-α (TNF-α), interleukin-6 (IL-6), and interferon-γ (IFN-γ)) in vitro. The oxidative potential (OP) induced by winter PM2.5 samples was higher than that induced by summertime samples, whereas inflammatory values showed contrasting seasonal variations. Both OP and inflammatory factors were significantly correlated with most chemical compounds in winter, but not in summer, which was thought to be related mainly to the higher contribution from secondary aerosols formed during the warm season. Source apportionment results showed secondary aerosols formation have significant contribution to OP of PM2.5 in both seasons, but the dominant oxidation processes is different. Secondary nitrates-related process was the major contributors regulating the OP in winter; however, secondary sulfates formation were mainly responsible for the ROS responses in summer. For primary emission, biomass burning, rather than coal emission or vehicle exhaust, was the significant source for OP of PM2.5 in winter. In most cases, the source contribution of each inflammatory factor was similar to that of the ROS. Our results highlighted the significant health risk of atmospheric aerosols from biomass burning in the rural regions of Guanzhong Basin, Northwest China.

Coupling interactive fire with atmospheric composition and climate in the UK Earth System Model

Abstract. Fire constitutes a key process in the Earth system (ES), being driven by climate as well as affecting the climate by changing atmospheric composition and impacting the terrestrial carbon cycle. However, studies on the effects of fires on atmospheric composition, radiative forcing and climate have been limited to date, as the current generation of ES models (ESMs) does not include fully atmosphere–composition–vegetation coupled fires feedbacks. The aim of this work is to develop and evaluate a fully coupled fire–composition–climate ES model. For this, the INteractive Fires and Emissions algoRithm for Natural envirOnments (INFERNO) fire model is coupled to the atmosphere-only configuration of the UK's Earth System Model (UKESM1). This fire–atmosphere interaction through atmospheric chemistry and aerosols allows for fire emissions to influence radiation, clouds and generally weather, which can consequently influence the meteorological drivers of fire. Additionally, INFERNO is updated based on recent developments in the literature to improve the representation of human and/or economic factors in the anthropogenic ignition and suppression of fire. This work presents an assessment of the effects of interactive fire coupling on atmospheric composition and climate compared to the standard UKESM1 configuration that uses prescribed fire emissions. Results show a similar performance when using the fire–atmosphere coupling (the “online” version of the model) when compared to the offline UKESM1 that uses prescribed fire. The model can reproduce observed present-day global fire emissions of carbon monoxide (CO) and aerosols, despite underestimating the global average burnt area. However, at a regional scale, there is an overestimation of fire emissions over Africa due to the misrepresentation of the underlying vegetation types and an underestimation over equatorial Asia due to a lack of representation of peat fires. Despite this, comparing model results with observations of CO column mixing ratio and aerosol optical depth (AOD) show that the fire–atmosphere coupled configuration has a similar performance when compared to UKESM1. In fact, including the interactive biomass burning emissions improves the interannual CO atmospheric column variability and consequently its seasonality over the main biomass burning regions – Africa and South America. Similarly, for aerosols, the AOD results broadly agree with the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Aerosol Robotic Network (AERONET) observations.

Insights into high concentrations of particle-bound imidazoles in the background atmosphere of southern China: Potential sources and influencing factors

Imidazoles are important constituents in atmospheric brown carbon and have gained increasing attention in the past decade. Although imidazoles have been studied widely in laboratories, the sparse field observations severely limit the understanding of imidazole's abundance and sources in the atmosphere. In this study, we measured particle-bound imidazoles and their precursors at a background forest site in the Nanling Mountains of southern China. The average concentration of imidazoles (4.17 ± 3.76 ng/m3) was found to be significantly higher than other background sites worldwide. Further analyses revealed that a majority of imidazoles (59.1%) at the site originated from secondary formation through reactions of dicarbonyls (e.g., glyoxal and methylglyoxal) and reduced nitrogen species, with relatively minor contributions from regional transport (32.8%) and biomass burning (8.1%). In addition, the key factors influencing secondary formation of imidazoles, such as relative humidity, water-soluble inorganic ions, and pH, were analyzed. Our results indicated that the secondary formation of imidazoles can be greatly enhanced under high humidity conditions, particularly during fog events. Overall, this study offers valuable insights into potential sources and influencing factors of ambient imidazoles in background atmospheres.

PM2.5 composition and sources in the San Joaquin Valley of California: A long-term study using ToF-ACSM with the capture vaporizer

The San Joaquin Valley (SJV) of California has suffered persistent particulate matter (PM) pollution despite many years of control efforts. To further understand the chemical drivers of this problem and to support the development of State Implementation Plan for PM, a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) outfitted with a PM2.5 lens and a capture vaporizer has been deployed at the Fresno-Garland air monitoring site of the California Air Resource Board (CARB) since Oct. 2018. The instrument measured non-refractory species in PM2.5 continuously at 10-min resolution. In this study, the data acquired from Oct. 2018 to May 2019 were analyzed to investigate the chemical characteristics, sources and atmospheric processes of PM2.5 in the SJV. Comparisons of the ToF-ACSM measurement with various co-located aerosol instruments show good agreements. The inter-comparisons indicated that PM2.5 in Fresno was dominated by submicron particles during the winter whereas refractory species accounted for a major fraction of PM2.5 mass during the autumn associated with elevated PM10 loadings. A rolling window positive matrix factorization analysis was applied to the organic aerosol (OA) mass spectra using the Multilinear Engine (ME-2) algorithm. Three distinct OA sources were identified, including vehicle emissions, local and regional biomass burning, and formation of oxygenated species. There were significant seasonal variations in PM2.5 composition and sources. During the winter, residential wood burning and oxidation of nitrogen oxides were major contributors to the occurrence of haze episodes with PM2.5 dominated by biomass burning OA and nitrate. In autumn, agricultural activities and wildfires were found to be the main cause of PM pollution. PM2.5 concentrations decreased significantly after spring and were dominated by oxygenated OA during March to May. Our results highlight the importance of using seasonally dependent control strategies to mitigate PM pollution in the SJV.

Wintertime Air Quality in Megacity Dhaka, Bangladesh Strongly Affected by Influx of Black Carbon Aerosols from Regional Biomass Burning.

Clean air is a key parameter for a sustainable society, and currently, megacity Dhaka has among the worst air qualities in the world. This results from poorly constrained contributions of a variety of sources from both local emissions and regional influx from the highly polluted Indo-Gangetic Plain, impacting the respiratory health of the 21 million inhabitants in the Greater Dhaka region. An important component of the fine particulate matter (PM2.5) is black carbon (BC) aerosols. In this study, we investigated the combustion sources of BC using a dual carbon isotope (δ13C and Δ14C) in Dhaka during the high-loading winter period of 2013/14 (regular and lockdown/hartal period) in order to guide mitigation policies. On average, BC (13 ± 6 μg m-3) contributed about 9% of the PM2.5 (145 ± 79 μg m-3) loadings. The relative contribution from biomass combustion under regular conditions was 44 ± 1% (with the rest from fossil combustion), while during periods of politically motivated large-scale lockdown of business and traffic, the biomass burning contribution increased to 63 ± 1%. To reduce the severe health impact of BC and other aerosol pollution in Dhaka, mitigation should therefore target regional-scale biomass/agricultural burning in addition to local traffic.

Stable nitrogen isotope composition of NOx of biomass burning in China

Owing to the local characteristics of stable nitrogen isotopes in nitrogen oxides (δ15N-NOx) emitted from biomass burning, the lack of data on δ15N-NOx values associated with biomass burning in China limits the use of this parameter in identifying and quantifying the sources of atmospheric nitrate (NO3-) and NOx. The results showed that the δ15N-NOx values of open burning and rural cooking stoves in China ranged from -3.7‰ to 3.1‰ and -11.9‰ to 1.5‰, respectively. The δ15N values of nine biomass fuel sources (δ15N-biomass) ranged from 0.1‰ to 4.1‰. Significant linear relationships between the δ15N-biomass values and δ15N-NOx values of open burning (δ15N-NOx = 1.1δ15N-biomass - 2.7; r2 = 0.63; p < 0.05) and rural cooking stoves (δ15N-NOx = 1.7δ15N-biomass - 9.8; r2 = 0.72; p < 0.01) suggested that the variations in δ15N-NOx values from biomass burning were mainly controlled by the biomass fuel source. The isotopic fractionation of nitrogen during the biomass burning process might have led to the higher δ15N-NOx values from open burning in comparison to rural cooking stoves. By combining the δ15N-NOx values of biomass burning with biomass burning emission inventory data, a model for calculating the δ15N-NOx values of biomass burning in different regions of China was established, and the estimated δ15N-NOx value of biomass burning at the national scale was -0.8 ± 1.2‰. But the limited δ15N-biomass values increase the uncertainty of model in national scale.

The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition

Abstract. The particularly strong dry season in Indonesia in 2015, caused by an exceptionally strong El Niño, led to severe peatland fires resulting in high volatile organic compound (VOC) biomass burning emissions. At the same time, the developing Asian monsoon anticyclone (ASMA) and the general upward transport in the Intertropical Convergence Zone (ITCZ) efficiently transported the resulting primary and secondary pollutants to the upper troposphere and lower stratosphere (UTLS). In this study, we assess the importance of these VOC emissions for the composition of the lower troposphere and the UTLS and investigate the effect of in-cloud oxygenated VOC (OVOC) oxidation during such a strong pollution event. This is achieved by performing multiple chemistry simulations using the global atmospheric model ECHAM/MESSy (EMAC). By comparing modelled columns of the biomass burning marker hydrogen cyanide (HCN) and carbon monoxide (CO) to spaceborne measurements from the Infrared Atmospheric Sounding Interferometer (IASI), we find that EMAC properly captures the exceptional strength of the Indonesian fires. In the lower troposphere, the increase in VOC levels is higher in Indonesia compared to other biomass burning regions. This has a direct impact on the oxidation capacity, resulting in the largest regional reduction in the hydroxyl radical (OH) and nitrogen oxides (NOx). While an increase in ozone (O3) is predicted close to the peatland fires, simulated O3 decreases in eastern Indonesia due to particularly high phenol concentrations. In the ASMA and the ITCZ, the upward transport leads to elevated VOC concentrations in the lower stratosphere, which results in the reduction of OH and NOx and the increase in the hydroperoxyl radical (HO2). In addition, the degradation of VOC emissions from the Indonesian fires becomes a major source of lower stratospheric nitrate radicals (NO3), which increase by up to 20 %. Enhanced phenol levels in the upper troposphere result in a 20 % increase in the contribution of phenoxy radicals to the chemical destruction of O3, which is predicted to be as large as 40 % of the total chemical O3 loss in the UTLS. In the months following the fires, this loss propagates into the lower stratosphere and potentially contributes to the variability of lower stratospheric O3 observed by satellite retrievals. The Indonesian peatland fires regularly occur during El Niño years, and the largest perturbations of radical concentrations in the lower stratosphere are predicted for particularly strong El Niño years. By activating the detailed in-cloud OVOC oxidation scheme Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC), we find that the predicted changes are dampened. Global models that neglect in-cloud OVOC oxidation tend to overestimate the impact of such extreme pollution events on the atmospheric composition.

Rapid transformation of ambient absorbing aerosols from West African biomass burning

Abstract. Seasonal biomass burning (BB) over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. Here, the evolution of smoke aerosols emitted from flaming-controlled burning of agricultural waste and wooded savannah in the Senegal region was characterized over a timescale of half-day advection from the source during the MOYA-2017 (Methane Observation Yearly Assessment-2017) aircraft campaign. Plumes from such fire types are rich in black carbon (BC) emissions. Concurrent measurements of chemical composition, organic aerosol (OA) oxidation state, bulk aerosol size and BC mixing state reveal that emitted BB submicron aerosols changed dramatically with time. Various aerosol optical properties (e.g. absorption Ångström exponent – AAE – and mass absorption coefficients – MACs) also evolved with ageing. In this study, brown carbon (BrC) was a minor fractional component of the freshly emitted BB aerosols (&lt; 0.5 h), but the increasing AAE with particle age indicates that BrC formation dominated over any loss process over the first ∼ 12 h of plume transport. Using different methods, the fractional contribution of BrC to total aerosol absorption showed an increasing trend with time and was ∼ 18 %–31 % at the optical wavelength of 405 nm after half-day transport. The generated BrC was found to be positively correlated with oxygenated and low-volatility OA, likely from the oxidation of evaporated primary OA and secondary OA formation. We found that the evolution of BrC with particle age was different in this region compared with previous BB field studies that mainly focused on emissions from smouldering fires, which have shown a high contribution from BrC at the source and BrC net loss upon ageing. This study suggests an initial stage of BrC absorption enhancement during the evolution of BB smoke. Secondary processing is the dominant contributor to BrC production in this BB region, in contrast to the primary emission of BrC previously reported in other BB studies. The total aerosol absorption normalized to BC mass (MACmeas-BC) was also enhanced with ageing due to the lensing effect of increasingly thick coatings on BC and the absorption by BrC. The effect of ageing on aerosol absorption, represented by the absorption enhancement (EAbs-MAC), was estimated over timescales of hours. MOYA-2017 provides novel field results. The comparisons between MOYA-2017 and previous field studies imply that the evolution of absorbing aerosols (BC and BrC) after emission varies with source combustion conditions. Different treatments of absorbing aerosol properties from different types of fires and their downwind evolution should be considered when modelling regional radiative forcing. These observational results will be very important for predicting climate effects of BB aerosol in regions controlled by flaming burning of agricultural waste and savannah-like biomass fuels.

On the processes governing the variability of PTR-MS based VOCs and OVOCs in different seasons of a year over hillocky mega city of India

The rapidly increasing industrialization and urbanization, in combination with under representation of in-situ measurements, especially Volatile Organic Compounds (VOCs), has posed serious challenges in understanding air quality and atmospheric chemistry over India. Here we present yearlong measurements of VOCs, carried out during March 2014–February 2015 using a Proton Transfer Reaction Mass Spectrometer (PTR-MS) from an urban site Pune (18.58oN, 73.91°E, 559 m amsl) in western tropical India. The averaged diurnal variation in VOCs at Pune exhibited a characteristic bimodal pattern, with highly pronounced peak during morning hours and secondary enhancement during late evening/night, except for Isoprene. Isoprene mixing ratios were observed to be higher (1.30 ± 0.69 ppbv) during the daytime (0900–1800 h) and lower (0.89 ± 0.65 ppbv) during the nighttime (after 1900 h and before 0900 h). While, Methanol, Acetonitrile, and Acetaldehyde are observed to be the highest (14.3 ± 5.9, 0.9 ± 0.4, and 6.1 ± 2.6 ppbv respectively) during spring, Benzene and Toluene were highest (1.6 ± 1.1, 2.6 ± 2.2 ppbv respectively) during winter. Isoprene mixing ratios showed broader maxima during autumn and winter (1.3 ppbv). Nominally, all the VOCs were observed to be lowest during the monsoon season. The two peaks in the seasonal cycle of acetonitrile along with VIIRS retrieved fire counts indicated impact of the regional biomass burning during spring and winter. Analysis of air-mass residence time further revealed potential influences from the highly polluted Indo-Gangetic Plain during the autumn and winter, whereas local pollution supplemented with regional biomass burning found to be the dominant process during spring. These yearlong measurements are a step forward in filling a major gap of observational data of VOCs over the tropical Indian region, which would be invaluable for evaluation of chemistry transport models and understanding of regional tropospheric chemistry.

PM2.5 sources affecting particle radioactivity in Boston, Massachusetts

Recent studies have found associations between particle radioactivity and various human health outcomes. The aim of this study is to identify sources contributing to PM2.5 (particulate matter with the aerodynamic diameter less than 2.5 μm) gross α- and β-activity levels. We used positive matrix factorization (PMF) to identify and apportion sources of PM2.5 in Boston during the period of one year in Boston. Toward this end, we used daily concentrations of elements, black carbon (BC), and PM2.5 mass. We identified six source types: regional pollution, motor vehicles, oil combustion, crustal, biomass burning, and sea salt. Subsequently, we performed multiple linear regression (MLR) analysis to examine the association between individual source contributions and PM2.5 gross α- and β-activities. Our analysis suggested that regional pollution had the highest impact on both PM2.5 α- and β-activities, followed by motor vehicles. Biomass burning and sea salt were not significantly associated with PM2.5 β-activity.

Direct radiative forcing of biomass burning aerosols from the extensive Australian wildfires in 2019–2020

In 2019, an unusually strong positive Indian Ocean Dipole spawned hot and dry weather in southeastern Australia, which promoted devastating wildfires in the period from September 2019 to February 2020. The fires produced large plumes of biomass burning aerosols that prevented sunlight from reaching the Earth’s surface, and in this way elicited regional radiative cooling. We estimated the direct aerosol radiative forcing (ARF) resulting from these wildfires, based on Moderate Resolution Imaging Spectroradiometer space-based data and an empirical relationship from AErosol RObotic NETwork ground-based data collected in biomass-burning regions. The wildfire-derived air pollution was associated with an aerosol optical thickness of >0.3 in Victoria and a strongly negative ARF of between −14.8 and −17.7 W m−2, which decreased the surface air temperature by about 3.7 °C–4.4 °C. This is of the same order of magnitude as the radiative cooling from volcanic eruptions. Although the atmospheric lifetime of biomass-burning aerosols is relatively short (about a week), the Australian wildfire pollution plumes extended across the Pacific Ocean to South America. Since climate change is expected to lead to more frequent and increasingly intense fires in many regions worldwide, the consequent biomass burning aerosols may become a significant radiative forcing factor, which will need to be accounted for in climate model projections for the future.

Photochemical environment over Southeast Asia primed for hazardous ozone levels with influx of nitrogen oxides from seasonal biomass burning

Abstract. Mainland and maritime Southeast Asia is home to more than 655 million people, representing nearly 10 % of the global population. The dry season in this region is typically associated with intense biomass burning activity, which leads to a significant increase in surface air pollutants that are harmful to human health, including ozone (O3). Latitude-based differences in the dry season and land use distinguish two regional biomass burning regimes: (1) burning on the peninsular mainland peaking in March and (2) burning across Indonesia peaking in September. The type and amount of material burned in each regime impact the emissions of nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs), which combine to produce ozone. Here, we use the nested GEOS-Chem atmospheric chemistry transport model (horizontal resolution of 0.25∘ × 0.3125∘), in combination with satellite observations from the Ozone Monitoring Instrument (OMI) and ground-based observations from Malaysia, to investigate ozone photochemistry over Southeast Asia in 2014. Seasonal cycles of tropospheric ozone columns from OMI and GEOS-Chem peak with biomass burning emissions. Compared to OMI, the model has a mean annual bias of −11 % but tends to overestimate tropospheric ozone near areas of seasonal fire activity. We find that outside these burning areas, the underlying photochemical environment is generally NOx-limited and dominated by anthropogenic NOx and biogenic non-methane VOC emissions. Pyrogenic emissions of NOx play a key role in photochemistry, shifting towards more VOC-limited ozone production and contributing about 30 % of the regional ozone formation potential during both biomass burning seasons. Using the GEOS-Chem model, we find that biomass burning activity coincides with widespread ozone exposure at levels that exceed world public health guidelines, resulting in about 260 premature deaths across Southeast Asia in March 2014 and another 160 deaths in September. Despite a positive model bias, hazardous ozone levels are confirmed by surface observations during both burning seasons.

Reductions in NO2 burden over north equatorial Africa from decline in biomass burning in spite of growing fossil fuel use, 2005 to 2017

Socioeconomic development in low- and middle-income countries has been accompanied by increased emissions of air pollutants, such as nitrogen oxides [NOx: nitrogen dioxide (NO2) + nitric oxide (NO)], which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, landscape biomass burning-another important NOx source-has declined in north equatorial Africa, attributed to changes in climate and anthropogenic fire management. Here, we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs-home to hundreds of millions of people-mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the dry season of November through February. Reductions in burned area explained the majority of variation in NO2 VCDs, though changes in fossil fuel emissions also explained some variation. Over Africa's biomass burning regions, raising mean GDP density (USD⋅km-2) above its lowest levels is associated with lower NO2 VCDs during the dry season, suggesting that economic development mitigates net NO2 emissions during these highly polluted months. In contrast to the traditional notion that socioeconomic development increases air pollutant concentrations in low- and middle-income nations, our results suggest that countries in Africa's northern biomass-burning region are following a different pathway during the fire season, resulting in potential air quality benefits. However, these benefits may be lost with increasing fossil fuel use and are absent during the rainy season.

Year-long Concurrent MAX-DOAS Observations of Nitrogen Dioxide and Formaldehyde at Pune: Understanding Diurnal and Seasonal Variation Drivers

Year-long observations of nitrogen dioxide (NO2) and formaldehyde (HCHO) using the Multi-Axis Differential Absorption Spectroscopy (MAX-DOAS) technique are reported from Pune City, India. We studied the diurnal and seasonal variations, effect of biomass burning and the weekend effect on both species. NO2 diurnal profiles displayed a traffic induced peak at ~09:00 hrs. HCHO also showed a morning peak ~10:00 hrs due to production from oxidation of VOCs in the presence of solar radiation. Both NO2 and HCHO show the highest average concentrations during the winter (October, November, December, January and February—ONDJF), with mean mixing ratios of 2.0 ± 1.4 ppb and 3.0 ± 1.4 ppb, respectively. These observations suggest that a lower boundary layer (BL) height during ONDJF leads to higher concentrations of trace gases. During June, July, August, and September (JJAS), both trace gases show a minimum in their concentrations, with average mixing ratios for NO2 and HCHO being 0.9 ± 0.6 ppb and 1.1 ± 0.7 ppb, most likely due to removal by wet deposition. There was no significant difference in both the trace gases on weekdays and weekends. Using back-trajectory analysis, we conclude that air parcels coming from regions of biomass burning increased the concentrations in Pune. Emissions from nearby industrial areas of Bhosari and Pimpri-Chinchwad increased NO2 concentrations in Pune city. Finally, we compared the observations with previous reports over India and found that both HCHO and NO2 concentrations are lower in Pune compared to the other large cities in India.

Impacts of chlorine emissions on secondary pollutants in China

The identified components of fine particulate matter with dynamic diameters less than 2.5 μm (PM2.5) suggests the remarkable increase in Cl− in PM2.5 during autumn and winter over North China. Anthropogenic chlorine emissions, including those from biomass burning, coal combustion and biofuel burning, are the main sources of Cl−, which could potentially affect the formation of secondary pollutants in the troposphere. In this study, we resolve the effect of chlorine emissions on PM2.5 and O3 by using the Weather Research and Forecasting (WRF) model coupled with Chemistry (WRF-Chem model) with an updated chemistry mechanism that includes the gaseous chemistry of chlorine, N2O5 heterogeneous reactions and detailed aqueous chemistry. Additionally, the biomass burning emissions of chlorine are derived from the Fire Inventory of the National Center for Atmospheric Research (NCAR) (FINN), which are considered the main contributor to atmospheric chloride over inland areas. The improved model is able to simulate the atmospheric Cl− in PM2.5 with reasonable agreement with the available observations in China. In addition, this model reduces the mean bias of ground-level PM2.5 concentrations from −7.5% to 3.2% over the BTH area and from −11.6% to −0.4% over the Northeast China Plain (NEP). The model also slightly improves O3 simulations by reducing the mean bias from 25.3% to 23.9% over mainland China. The anthropogenic chlorine emissions are estimated to increase the monthly average PM2.5 by 7.5 μg/m3 (9.1%), whereas ozone decreases slightly by up to 2.1 ppbv (4.3%) in November 2014. The influence of ozone was more significant in summer, reaching 2–8 ppbv over the biomass burning regions in 2014. The increase in Cl− and NH4+ accounted for the impacts on PM2.5, and the decline in O3 could be explained by the cycle between chlorine radicals and gases and changes in precursor concentrations. Our results suggest the importance of chlorine emissions and their chemical processes in the formation of PM2.5 and O3 over high-emission regions in China.

Vertical Profiles of Atmospheric Species Concentrations and Nighttime Boundary Layer Structure in the Dry Season over an Urban Environment in Central Amazon Collected by an Unmanned Aerial Vehicle

Nighttime vertical profiles of ozone, PM2.5 and PM10 particulate matter, carbon monoxide, temperature, and humidity were collected by a copter-type unmanned aerial vehicle (UAV) over the city of Manaus, Brazil, in central Amazon during the dry season of 2018. The vertical profiles were analyzed to understand the structure of the urban nighttime boundary layer (NBL) and pollution within it. The ozone concentration, temperature, and humidity had an inflection between 225 and 350 m on most nights, representing the top of the urban NBL. The profile of carbon monoxide concentration correlated well with the local evening vehicular congestion of a modern transportation fleet, providing insight into the surface-atmosphere dynamics. In contrast, events of elevated PM2.5 and PM10 concentrations were not explained well by local urban emissions, but rather by back trajectories that intersected regional biomass burning. These results highlight the potential of the emerging technologies of sensor payloads on UAVs to provide new constraints and insights for understanding the pollution dynamics in nighttime boundary layers in urban regions.

Constraining the relationships between aerosol height, aerosol optical depth and total column trace gas measurements using remote sensing and models

Abstract. Proper quantification of the aerosol vertical height is essential to constrain the atmospheric distribution and lifetime of aerosols, as well as their impact on the environment. We use globally distributed, daily averaged measurements of aerosol stereo heights of fire aerosols from the Multi-angle Imaging SpectroRadiometer (MISR) to understand the aerosol distribution. We also connect these results with a simple plume rise model and a new multi-linear regression model approach based on daily measurements of NO2 from OMI and CO from MOPITT to understand and model the global aerosol vertical height profile over biomass burning regions. First, plumes associated with the local dry-burning season at midlatitudes to high latitudes frequently have a substantial fraction lofted into the free troposphere and in some cases even the stratosphere. Second, plumes mainly associated with less-polluted regions in developing countries and heavily forested areas tend to stay closer to the ground, although they are not always uniformly distributed throughout the boundary layer. Third, plumes associated with more serious loadings of pollution (such as in Africa, Southeast Asia and northeast China) tend to have a substantial amount of smoke transported uniformly through the planetary boundary layer and up to around 3 km. Fourth, the regression model approach yields a better ability to reproduce the measured heights compared to the plume rise model approach. This improvement is based on a removal of the negative bias observed from the plume model approach, as well as a better ability to work under more heavily polluted conditions. However, over many regions, both approaches fail, requiring deeper work to understand the physical, chemical and dynamical reasons underlying the failure over these regions.

New SOA Treatments Within the Energy Exascale Earth System Model (E3SM): Strong Production and Sinks Govern Atmospheric SOA Distributions and Radiative Forcing

AbstractSecondary organic aerosols (SOA) are large contributors to fine particle mass loading and number concentration and interact with clouds and radiation. Several processes affect the formation, chemical transformation, and removal of SOA in the atmosphere. For computational efficiency, global models use simplified SOA treatments, which often do not capture the dynamics of SOA formation. Here we test more complex SOA treatments within the global Energy Exascale Earth System Model (E3SM) to investigate how simulated SOA spatial distributions respond to some of the important but uncertain processes affecting SOA formation, removal, and lifetime. We evaluate model predictions with a suite of surface, aircraft, and satellite observations that span the globe and the full troposphere. Simulations indicate that both a strong production (achieved here by multigenerational aging of SOA precursors that includes moderate functionalization) and a strong sink of SOA (especially in the middle upper troposphere, achieved here by adding particle‐phase photolysis) are needed to reproduce the vertical distribution of organic aerosol (OA) measured during several aircraft field campaigns; without this sink, the simulated middle upper tropospheric OA is too large. Our results show that variations in SOA chemistry formulations change SOA wet removal lifetime by a factor of 3 due to changes in horizontal and vertical distributions of SOA. In all the SOA chemistry formulations tested here, an efficient chemical sink, that is, particle‐phase photolysis, was needed to reproduce the aircraft measurements of OA at high altitudes. Globally, SOA removal rates by photolysis are equal to the wet removal sink, and photolysis decreases SOA lifetimes from 10 to ~3 days. A recent review of multiple field studies found no increase in net OA formation over and downwind biomass burning regions, so we also tested an alternative, empirical SOA treatment that increases primary organic aerosol (POA) emissions near source region and converts POA to SOA with an aging time scale of 1 day. Although this empirical treatment performs surprisingly well in simulating OA loadings near the surface, it overestimates OA loadings in the middle and upper troposphere compared to aircraft measurements, likely due to strong convective transport to high altitudes where wet removal is weak. The default improved model formulation (multigenerational aging with moderate fragmentation and photolysis) performs much better than the empirical treatment in these regions. Differences in SOA treatments greatly affect the SOA direct radiative effect, which ranges from −0.65 (moderate fragmentation and photolysis) to −2 W m−2 (moderate fragmentation without photolysis). Notably, most SOA formulations predict similar global indirect forcing of SOA calculated as the difference in cloud forcing between present‐day and preindustrial simulations.