Biomass Burning Plumes Research Articles

Intensive aerosol properties of boreal and regional biomass burning aerosol at Mt. Bachelor Observatory: larger and black carbon (BC)-dominant particles transported from Siberian wildfires

Abstract. We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8–14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σscat), aerosol light-absorbing coefficients (σabs), fine particulate matter (PM1), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσscat/ΔPM1), and a bimodal aerosol size distribution with a higher geometric mean diameter (Dg). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region.

Effects of transport on a biomass burning plume from Indochina during EMeRGe-Asia identified by WRF-Chem

Abstract. The Indochina biomass burning (BB) season in springtime has a substantial environmental impact on the surrounding areas in Asia. In this study, we evaluated the environmental impact of a major long-range BB transport event on 19 March 2018 (a flight of the High Altitude and Long Range Research Aircraft (HALO; https://www.halo-spp.de, last access: 14 February 2023) research aircraft, flight F0319) preceded by a minor event on 17 March 2018 (flight F0317). Aircraft data obtained during the campaign in Asia of the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales (EMeRGe) were available between 12 March and 7 April 2018. In F0319, results of 1 min mean carbon monoxide (CO), ozone (O3), acetone (ACE), acetonitrile (ACN), organic aerosol (OA), and black carbon aerosol (BC) concentrations were up to 312.0, 79.0, 3.0, and 0.6 ppb and 6.4 and 2.5 µg m−3, respectively, during the flight, which passed through the BB plume transport layer (BPTL) between the elevation of 2000–4000 m over the East China Sea (ECS). During F0319, the CO, O3, ACE, ACN, OA, and BC maximum of the 1 min average concentrations were higher in the BPTL by 109.0, 8.0, 1.0, and 0.3 ppb and 3.0 and 1.3 µg m−3 compared to flight F0317, respectively. Sulfate aerosol, rather than OA, showed the highest concentration at low altitudes (<1000 m) in both flights F0317 and F0319 resulting from the continental outflow in the ECS. The transport of BB aerosols from Indochina and its impacts on the downstream area were evaluated using a Weather Research Forecasting with Chemistry (WRF-Chem) model. The modeling results tended to overestimate the concentration of the species, with examples being CO (64 ppb), OA (0.3 µg m−3), BC (0.2 µg m−3), and O3 (12.5 ppb) in the BPTL. Over the ECS, the simulated BB contribution demonstrated an increasing trend from the lowest values on 17 March 2018 to the highest values on 18 and 19 March 2018 for CO, fine particulate matter (PM2.5), OA, BC, hydroxyl radicals (OH), nitrogen oxides (NOx), total reactive nitrogen (NOy), and O3; by contrast, the variation of J(O1D) decreased as the BB plume's contribution increased over the ECS. In the lower boundary layer (<1000 m), the BB plume's contribution to most species in the remote downstream areas was <20 %. However, at the BPTL, the contribution of the long-range transported BB plume was as high as 30 %–80 % for most of the species (NOy, NOx, PM2.5, BC, OH, O3, and CO) over southern China (SC), Taiwan, and the ECS. BB aerosols were identified as a potential source of cloud condensation nuclei, and the simulation results indicated that the transported BB plume had an effect on cloud water formation over SC and the ECS on 19 March 2018. The combination of BB aerosol enhancement with cloud water resulted in a reduction of incoming shortwave radiation at the surface in SC and the ECS by 5 %–7 % and 2 %–4 %, respectively, which potentially has significant regional climate implications.

Airborne glyoxal measurements in the marine and continental atmosphere: comparison with TROPOMI observations and EMAC simulations

Abstract. We report on airborne limb and nadir measurements of vertical profiles and total vertical column densities (VCDs) of glyoxal (C2H2O2) in the troposphere, which were performed aboard the German research aircraft HALO (High Altitude and LOng Range) in different regions and seasons around the globe between 2014 and 2019. The airborne nadir and integrated limb profiles agree excellently among each other. Our airborne observations are further compared to collocated glyoxal measurements of the TROPOspheric Monitoring Instrument (TROPOMI), with good agreement between both data sets for glyoxal observations in (1) pristine terrestrial, (2) pristine marine, (3) mixed polluted, and (4) biomass-burning-affected air masses with high glyoxal concentrations. Exceptions to the overall good agreement are observations of (1) faint and aged biomass burning plumes over the oceans and (2) of low-lying biomass burning or anthropogenic plumes in the terrestrial or marine boundary layer, both of which contain elevated glyoxal that is mostly not captured by TROPOMI. These differences in airborne and satellite-detected glyoxal are most likely caused by the overall small contribution of plumes of a limited extent to the total glyoxal absorption in the atmosphere and the difficulty in remotely detecting weak absorbers located close to low reflective surfaces (e.g. the ocean in the visible wavelength range) or within dense aerosol layers. Observations of glyoxal in aged biomass burning plumes (e.g. observed over the tropical Atlantic off the coast of West Africa in summer 2018, off the coast of Brazil by the end of the dry season 2019, and the East China Sea in spring 2018) could be traced back to related wildfires, such as a plume crossing over the Drake Passage that originated from the Australian bushfires in late 2019. Our observations of glyoxal in such aged biomass burning plumes confirm recent findings of enhanced glyoxal and presumably secondary organic aerosol (SOA) formation in aged wildfire plumes from yet-to-be-identified, longer-lived organic precursor molecules (e.g. aromatics, acetylene, or aliphatic compounds) co-emitted in the fires. Furthermore, elevated glyoxal (median 44 ppt – parts per trillion), as compared to other marine regions (median 10–19 ppt), is observed in the boundary layer over the tropical oceans, which is well in agreement with previous reports. The airborne data sets are further compared to glyoxal simulations performed with the global atmosphere chemistry model EMAC (ECHAM/MESSy Atmospheric Chemistry). When using an EMAC set up that resembles recent EMAC studies focusing on complex chemistry, reasonable agreement is found for pristine air masses (e.g. the unperturbed free and upper troposphere), but a notable glyoxal overestimation of the model exists for regions with high emissions of glyoxal and glyoxal-producing volatile organic compounds (VOCs) from the biosphere (e.g. the Amazon). In all other investigated regions, the model underpredicts glyoxal to varying degrees, in particular when probing mixed emissions from anthropogenic activities (e.g. over continental Europe, the Mediterranean, and East China Sea) and potentially from the sea (e.g. the tropical oceans). Also, the model tends to largely underpredict glyoxal in city plumes and aged biomass burning plumes. The potential causes for these differences are likely to be multifaceted, but they all point to missing glyoxal sources from the degradation of the mixture of potentially longer-chained organic compounds emitted from anthropogenic activities, biomass burning, and from the organic microlayer of the sea surface.

Impacts of biomass burning in Southeast Asia on aerosols over the low-latitude plateau in China: An analysis of a typical pollution event

From March to April, widespread forest fires and agro-residue burning frequently occur in Southeast Asia, which release large amounts of gas species and aerosols and impact air quality over the wide source and downwind regions. In this study, we investigated the impact of biomass burning (BB) over Southeast Asia on particulate matter concentrations and aerosol properties in downwind areas of the low-latitude plateau from 1 March to 30 April 2019, with a focus on a typical pollution event in Kunming (KM), the capital of Yunnan Province, by using a wide variety of observations from the Chenggong ground monitoring station in Yunnan University, an air quality network in China, satellite retrievals and ERA-5 reanalysis data and numerical simulation. A regional pollution event contributed by BB pollutants from Southeast Asia and the India-Myanmar trough occurred in Yunnan Province on 31 March to 1 April 2019, which was the only typical pollution event that pollution transmission ran through central Yunnan Province from south to north since 2013, when the Airborne Pollution Action Plan was unveiled by China government. The daily mean PM2.5, PM1, and black carbon concentrations increased by 73.3 μg m−3(78%), 70.5 μg m−3 (80%), and 7.7 μg m−3 (83%), respectively, and the scattering and absorbing coefficients increased by 471.6 Mm−1 and 63.5 Mm−1, respectively, at the Chenggong station. The southwest winds exceeding 2 km vertically thick appeared in front of the India-Myanmar trough over the fire regions, pushing BB plumes northward into Yunnan Province. The model results show that 59.5% of PM2.5 mass produced by BB in Yunnan Province was sourced from the Myanmar-Thailand border, and 29.3% was from western Myanmar at a lower altitude (<4.9 km), which indicated that BB in the Myanmar-Thailand border was the dominant contributor.

Aerosols on the Tropical Island of La Réunion (21°S, 55°E): Assessment of Climatology, Origin of Variability and Trend

Aerosols are essential climate variables that need to be observed at a global scale to monitor the evolution of the atmospheric composition and potential climate impacts. We used the measurements performed over the May 2007–December 2019 period by a ground-based sun photometer installed at the island of La Réunion (21°S, 55°E), together with a linear regression fitting model, to assess the climatology and types of aerosols reaching this observation site located in a sparsely documented pristine area, and the forcings responsible for the variability of the observed aerosol optical depth (AOD) and related trend. The climatology of the aerosol optical depth (AOD) at 440 nm (AOD440) and Ångström exponent between 500 and 870 nm (α) revealed that sea salts could be considered as the La Réunion AOD440 and α baselines (0.06 ± 0.03 and 0.61 ± 0.40, respectively, from December to August), which were mainly modulated by biomass burning (BB) plumes passing over La Réunion (causing a doubling of AOD440 and α up to 0.13 ± 0.07 and 1.06 ± 0.34, respectively, in October). This was confirmed by the retrieved aerosol volume size distributions showing that the coarse-mode (fine-mode) dominated the total volume concentration for AOD440 lower (higher) than 0.2 with a mean radius equal to 3 μm (0.15 μm). The main contribution to the AOD440 variability over La Réunion was evaluated to be the BB activity (67.4 ± 28.1%), followed by marine aerosols (16.3 ± 4.2%) and large-scale atmospheric structures (5.5 ± 1.7%). The calculated trend for AOD440 equaled 0.02 ± 0.01 per decade (2.6 ± 1.3% per year). These results provide a scientific reference base for upcoming studies dedicated to the quantification of the impact of wildfire emissions on the southwestern Indian Ocean’s atmospheric composition and radiative balance.

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

Abstract. The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancement ratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.

VLIDORT-QS: A quasi-spherical vector radiative transfer model

We present a new VLIDORT-based quasi-spherical vector radiative transfer (RT) model (VLIDORT-QS) that was developed for forward-model simulations of long-path measurements in limb- or nadir-viewing spherical-atmosphere configurations. This paper provides a theoretical description of the RT model, in which the single-scatter radiation field is treated accurately in spherical geometry, while the diffuse-scatter source terms at points along the line-of-sight are approximated locally through pseudo-spherical simulations based on the VLIDORT RT code; these multiple scatter source terms are then folded into the source function integration to yield the radiation field at any line-of-sight observation point in the atmosphere. In addition, the VLIDORT-QS model has a complete linearization facility (ability to generate analytic Jacobians of the radiation field with respect to any atmospheric or surface property). Validation of the model has been carried out against a fully-spherical Monte Carlo code, and also against the standard VLIDORT model for nadir-view scenarios with relatively low sphericity effects. A sample application of VLIDORT-QS for a biomass-burning plume scenario is demonstrated. A second paper will present a detailed analysis of the retrieval of ice-cloud properties from high-altitude aircraft measurements taken as part of the NASA Airborne Tropical Tropopause Experiment (ATTREX) campaign, with VLIDORT-QS providing forward-model simulations of the radiation fields and associated Jacobian functions.

Biomass burning and marine aerosol processing over the southeast Atlantic Ocean: a TEM single-particle analysis

Abstract. This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.

Radiative impacts of the Australian bushfires 2019–2020 – Part 1: Large-scale radiative forcing

Abstract. As a consequence of extreme heat and drought, record-breaking wildfires developed and ravaged south-eastern Australia during the fire season 2019–2020. The fire strength reached its paroxysmal phase at the turn of the year 2019–2020. During this phase, pyrocumulonimbus clouds (pyroCb) developed and injected biomass burning aerosols and gases into the upper troposphere and lower stratosphere (UTLS). The UTLS aerosol layer was massively perturbed by these fires, with aerosol extinction increased by a factor of 3 in the visible spectral range in the Southern Hemisphere, with respect to a background atmosphere, and stratospheric aerosol optical depth reaching values as large as 0.015 in February 2020. Using the best available description of this event by observations, we estimate the radiative forcing (RF) of such perturbations of the Southern Hemispheric aerosol layer. We use offline radiative transfer modelling driven by observed information of the aerosol extinction perturbation and its spectral variability obtained from limb satellite measurements. Based on hypotheses on the absorptivity and the angular scattering properties of the aerosol layer, the regional (at three latitude bands in the Southern Hemisphere) clear-sky TOA (top-of-atmosphere) RF is found varying from small positive values to relatively large negative values (up to −2.0 W m−2), and the regional clear-sky surface RF is found to be consistently negative and reaching large values (up to −4.5 W m−2). We argue that clear-sky positive values are unlikely for this event, if the ageing/mixing of the biomass burning plume is mirrored by the evolution of its optical properties. Our best estimate for the area-weighted global-equivalent clear-sky RF is -0.35±0.21 (TOA RF) and -0.94±0.26 W m−2 (surface RF), thus the strongest documented for a fire event and of comparable magnitude with the strongest volcanic eruptions of the post-Pinatubo era. The surplus of RF at the surface, with respect to TOA, is due to absorption within the plume that has contributed to the generation of ascending smoke vortices in the stratosphere. Highly reflective underlying surfaces, like clouds, can nevertheless swap negative to positive TOA RF, with global average RF as high as +1.0 W m−2 assuming highly absorbing particles.

Development and evaluation of the Aerosol Forecast Member in the National Center for Environment Prediction (NCEP)'s Global Ensemble Forecast System (GEFS-Aerosols v1)

Abstract. The National Oceanic and Atmospheric Administration (NOAA)'s National Weather Service (NWS) is on its way to deploying various operational prediction applications using the Unified Forecast System (https://ufscommunity.org/, last access: 18 June 2022), a community-based coupled, comprehensive Earth modeling system. An aerosol model component developed in collaboration between the Global Systems Laboratory, Chemical Science Laboratory, Air Resources Laboratory, and Environmental Modeling Center (GSL, CSL, ARL, EMC) was coupled online with the FV3 Global Forecast System (FV3GFS) using the National Unified Operational Prediction Capability (NUOPC)-based NOAA Environmental Modeling System (NEMS) software framework. This aerosol prediction system replaced the NEMS GFS Aerosol Component version 2 (NGACv2) system in the National Center for Environment Prediction (NCEP) production suite in September 2020 as one of the ensemble members of the Global Ensemble Forecast System (GEFS), dubbed GEFS-Aerosols v1. The aerosol component of atmospheric composition in the GEFS is based on the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). GEFS-Aerosols includes bulk modules from the Goddard Chemistry Aerosol Radiation and Transport model (GOCART). Additionally, the biomass burning plume rise module from High-Resolution Rapid Refresh (HRRR)-Smoke based on WRF-Chem was implemented. The GOCART dust scheme was replaced by the FENGSHA dust scheme (developed by ARL). The Blended Global Biomass Burning Emissions Product (GBBEPx version 3) provides biomass burning emission and fire radiative power (FRP) data. The global anthropogenic emission inventories are derived from the Community Emissions Data System (CEDS). All sub-grid-scale transport and deposition are handled inside the atmospheric physics routines, which required consistent implementation of positive definite tracer transport and wet scavenging in the physics parameterizations used by the NCEP's operational FV3GFS. This paper describes the details of GEFS-Aerosols model development and evaluation of real-time and retrospective runs using different observations from in situ measurement and satellite and aircraft data. GEFS-Aerosols predictions demonstrate substantial improvements for both composition and variability of aerosol distributions over those from the former operational NGACv2 system with the fundamental updates (e.g., dust and fire emission) in the atmospheric and chemical transport model.

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

Analysis of CO<sub>2</sub>, CH<sub>4</sub>, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations

Abstract. Réunion Island is situated in the Indian Ocean and holds one of the very few atmospheric observatories in the tropical Southern Hemisphere. Moreover, it hosts experiments providing both ground-based surface and column observations of CO2, CH4, and CO atmospheric concentrations. This work presents a comprehensive study of these observations made in the capital Saint-Denis and at the high-altitude Maïdo Observatory. We used simulations of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), in its passive tracer option (WRF-GHG), to gain more insight to the factors that determine the observed concentrations. Additionally, this study provides an evaluation of the WRF-GHG performance in a region of the globe where it has not yet been applied. A comparison of the basic meteorological fields near the surface and along atmospheric profiles showed that WRF-GHG has decent skill in reproducing these meteorological measurements, especially temperature. Furthermore, a distinct diurnal CO2 cycle with values up to 450 ppm was found near the surface in Saint-Denis, driven by local anthropogenic emissions, boundary layer dynamics, and accumulation due to low wind speed at night. Due to an overestimation of local wind speed, WRF-GHG underestimates this nocturnal buildup. At Maïdo, a similar diurnal cycle is found but with much smaller amplitude. There, surface CO2 is essentially driven by the surrounding vegetation. The hourly column-averaged mole fractions of CO2 (XCO2) of WRF-GHG and the corresponding TCCON observations were highly correlated with a Pearson correlation coefficient of 0.90. These observations represent different air masses to those near the surface; they are influenced by processes from Madagascar, Africa, and further away. The model shows contributions from fires during the Southern Hemisphere biomass burning season but also biogenic enhancements associated with the dry season. Due to a seasonal bias in the boundary conditions, WRF-GHG fails to accurately reproduce the CH4 observations at Réunion Island. Furthermore, local anthropogenic fluxes are the largest source influencing the surface CH4 observations. However, these are likely overestimated. Furthermore, WRF-GHG is capable of simulating CO levels on Réunion Island with a high precision. As to the observed CO column (XCO), we confirmed that biomass burning plumes from Africa and elsewhere are important for explaining the observed variability. The in situ observations at the Maïdo Observatory can characterize both anthropogenic signals from the coastal regions and biomass burning enhancements from afar. Finally, we found that a high model resolution of 2 km is needed to accurately represent the surface observations. At Maïdo an even higher resolution might be needed because of the complex topography and local wind patterns. To simulate the column Fourier transform infrared (FTIR) observations on the other hand, a model resolution of 50 km might already be sufficient.

Using Multi-Platform Satellite Observations to Study the Atmospheric Evolution of Brown Carbon in Siberian Biomass Burning Plumes

A bulk of evidence from in situ observations and lab experiments suggests that brown carbon (light-absorbing organic compounds in particles) can provide a significant yet highly variable contribution to the overall light absorption by aerosol particles from biomass burning (BB). Partly stemming from the complexity of the atmospheric evolution of organic aerosol (OA), the variability in brown carbon (BrC) absorption makes it difficult to partition the radiative effects of BrC and black carbon (BC) in atmospheric and climate models; as such, there are calls for satellite-based methods that could provide a statistical characterization of BrC absorption and its evolution in different regions of the world, especially in remote BB regions, such as Siberia. This study examined the feasibility of the statistical characterization of the evolution of BrC absorption and related parameters of BB aerosol in smoke plumes from intense wildfires in Siberia through the analysis of a combination of data from three satellite instruments: OMI (Ozone Monitoring Instrument), MISR (Multi-Angle Imaging SpectroRadiometer), and MODIS (Moderate Resolution Imaging Spectroradiometer). Using a Monte Carlo method, which related the satellite retrievals of the absorption and extinction aerosol optical depths to Mie theory calculations of the optical properties of BB aerosol, we found that the BrC absorption, as well as the imaginary refractive index for the OA, decreased significantly in Siberian BB smoke plumes during about 30 h of the daylight evolution, nevertheless remaining considerable until at least 70 h of the daylight evolution. Overall, the study indicated that the analysis of multi-platform satellite observations of BB plumes can provide useful insights into the atmospheric evolution of BrC absorption and the partitioning of BrC and BC contributions to the total light absorption by BB aerosol.

Evaluation of Cairpol and Aeroqual Air Sensors in Biomass Burning Plumes

Cairpol and Aeroqual air quality sensors measuring CO, CO2, NO2, and other species were tested in fresh biomass burning plumes in field and laboratory environments. We evaluated sensors by comparing 1-minute sensor measurements to collocated reference instrument measurements. Sensors were evaluated based on the coefficient of determination (r 2) between the sensor and reference measurements, by the accuracy, collocated precision, root mean square error (RMSE), and other metrics. In general, CO and CO2 sensors performed well (in terms of accuracy and r 2 values) compared to NO2 sensors. Cairpol CO and NO2 sensors had better sensor-versus-sensor agreement (e.g., collocated precision) than Aeroqual CO and NO2 sensors of the same species. Tests of other sensors (e.g., NH3, H2S, VOC, NMHC) provided more inconsistent results and need further study. Aeroqual NO2 sensors had an apparent O3 interference that was not observed in the Cairpol NO2 sensors. Although the sensor accuracy lags that of reference-level monitors, with location-specific calibrations they have the potential to provide useful data about community air quality and personal exposure to smoke impacts.

The characterization of long-range transported North American biomass burning plumes: what can a multi-wavelength Mie–Raman-polarization-fluorescence lidar provide?

Abstract. This article presents a study of long-range transported biomass burning aerosols (BBA) originated from the North American wildfires in September 2020. The BBA plumes presented in this study were in the troposphere and underwent 1–2 weeks of aging before arriving at the lidar station ATOLL (ATmospheric Observatory of LiLle) in northern France. A novel lidar-derived dataset, 2α+3β+3δ+ϕ (α: extinction coefficient; β: backscatter coefficient; δ: particle linear depolarization ratio, i.e., PLDR; ϕ: fluorescence capacity), is provided for the characterization of BBA. The fluorescence capacity is an intensive aerosol parameter describing the ability of aerosols in producing fluorescence when exposed to UV excitation. In our BBA observations, obvious variations in aerosol intensive parameters, reflecting the variability of BBA properties, were detected. The PLDRs varied from less than 0.03 at all wavelengths to 0.15–0.22 and 0.12–0.16, respectively, at 355 and 532 nm. The extinction related Angström exponent was within the range of −0.3 to 1.0 and the fluorescence capacity was 1.0 × 10−4–4.0 × 10−4. Lidar ratio as low as 24 ± 4 sr (50 ± 8 sr) was observed in the BBA plumes at 355 (532) nm on 17–18 September, which was lower than most previously observed aged BBAs. These variations are likely correlated with the combustion process, the lifting of BBA plumes and the conditions (temperature, humidities, etc.) in the aging process. In addition, our results indicate BBA could act as ice nucleating particles in tropospheric conditions. The lidar fluorescence channel proves to be an important added value in aerosol characterization and aerosol–cloud interactions studies, due to its high sensitivity. With the increase in wildfire occurrence and intensity, BBAs become a more and more important atmospheric component. In this context, we show the potential of our novel lidar-derived dataset for aged BBA particles' characterization and for the understanding of their role in cloud processes.

Ground-based investigation of HO<sub><i>x</i></sub> and ozone chemistry in biomass burning plumes in rural Idaho

Abstract. Ozone (O3), a potent greenhouse gas that is detrimental to human health, is typically found in elevated concentrations within biomass burning (BB) smoke plumes. The radical species OH, HO2, and RO2 (known collectively as ROx) have central roles in the formation of secondary pollutants including O3 but are poorly characterized for BB plumes. We present measurements of total peroxy radical concentrations ([XO2] ≡ [HO2] + [RO2]) and additional trace-gas and particulate matter measurements from McCall, Idaho, during August 2018. There were five distinct periods in which BB smoke impacted this site. During BB events, O3 concentrations were enhanced, evident by ozone enhancement ratios (ΔO3/ΔCO) that ranged up to 0.06 ppbv ppbv−1. [XO2] was similarly elevated during some BB events. Overall, instantaneous ozone production rates (P(O3)) were minimally impacted by the presence of smoke as [NOx] enhancements were minimal. Measured XO2 concentrations were compared to zero-dimensional box modeling results to evaluate the Master Chemical Mechanism (MCM) and GEOS-Chem mechanisms overall and during periods of BB influence. The models consistently overestimated XO2 with the base MCM and GEOS-Chem XO2 predictions high by an average of 28 % and 20 %, respectively. One period of BB influence had distinct measured enhancements of 15 pptv XO2 that were not reflected in the model output, likely due to the presence of unmeasured HOx sources. To the best of our knowledge, this is the first BB study featuring peroxy radical measurements.

Atmospheric Reactivity of Methoxyphenols: A Review

Methoxyphenols emitted from lignin pyrolysis are widely used as potential tracers for biomass burning, especially for wood burning. In the past ten years, their atmospheric reactivity has attracted increasing attention from the academic community. Thus, this work provides an extensive review of the atmospheric reactivity of methoxyphenols, including their gas-phase, particle-phase, and aqueous-phase reactions, as well as secondary organic aerosol (SOA) formation. Emphasis was placed on kinetics, mechanisms, and SOA formation. The reactions of methoxyphenols with OH and NO3 radicals were the predominant degradation pathways, which also had significant SOA formation potentials. The reaction mechanism of methoxyphenols with O3 is the cycloaddition of O3 to the benzene ring or unsaturated C═C bond, while H-abstraction and radical adduct formation are the main degradation channels of methoxyphenols by OH and NO3 radicals. Based on the published studies, knowledge gaps were pointed out. Future studies including experimental simulations and theoretical calculations of other representative kinds of methoxyphenols should be systematically carried out under complex pollution conditions. In addition, the ecotoxicity of their degradation products and their contribution to SOA formation from the atmospheric aging of biomass-burning plumes should be seriously assessed.

NO<sub>3</sub> chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO<sub>3</sub> radical

Abstract. Furans are emitted to the atmosphere during biomass burning from the pyrolysis of cellulose. They are one of the major contributing volatile organic compound (VOC) classes to OH and NO3 reactivity in biomass burning plumes. The major removal process of furans from the atmosphere at night is reaction with the nitrate radical, NO3. Here, we report a series of relative rate experiments in the 7300 L indoor simulation chamber at Institut de Combustion Aérothermique Réactivité et Environnement, Centre national de la recherche scientifique (ICARE-CNRS), Orléans, using a number of different reference compounds to determine NO3 reaction rate coefficients for four furans, two furanones, and pyrrole. In the case of the two furanones, this is the first time that NO3 rate coefficients have been reported. The recommended values (cm3 molec.−1 s−1) are as follows: furan, (1.49 ± 0.23) × 10−12; 2-methylfuran, (2.26 ± 0.52) × 10−11; 2,5-dimethylfuran, (1.02 ± 0.31) × 10−10; furfural (furan-2-aldehyde), (9.07 ± 2.3) × 10−14; α-angelicalactone (5-methyl-2(3H)-furanone), (3.01 ± 0.45) × 10−12; γ-crotonolactone (2(5H)-furanone), <1.4 × 10−16; and pyrrole, (6.94 ± 1.9) × 10−11. The furfural + NO3 reaction rate coefficient is found to be an order of magnitude smaller than previously reported. These experiments show that for furan, alkyl-substituted furans, α-angelicalactone, and pyrrole, reaction with NO3 will be the dominant removal process at night and may also contribute during the day. For γ-crotonolactone, reaction with NO3 is not an important atmospheric sink.

Inline coupling of simple and complex chemistry modules within the global weather forecast model FIM (FIM-Chem v1)

Abstract. The global Flow-following finite-volume Icosahedral Model (FIM), which was developed in the Global Systems Laboratory (GSL) of NOAA, has been coupled inline with aerosol and gas-phase chemistry schemes of different complexity using the chemistry and aerosol packages from WRF-Chem v3.7, named FIM-Chem v1. The three chemistry schemes include (1) the simple aerosol modules from the Goddard Chemistry Aerosol Radiation and Transport model that includes only simplified sulfur chemistry, black carbon (BC), organic carbon (OC), and sectional dust and sea salt modules (GOCART); (2) the photochemical gas phase of the Regional Atmospheric Chemistry Mechanism (RACM) coupled to GOCART to determine the impact of more realistic gas-phase chemistry on the GOCART aerosol simulations (RACM_GOCART); and (3) a further sophistication within the aerosol modules by replacing GOCART with a modal aerosol scheme that includes secondary organic aerosols (SOAs) based on the volatility basis set (VBS) approach (RACM_SOA_VBS). FIM-Chem is able to simulate aerosol, gas-phase chemical species, and SOA at various spatial resolutions with different levels of complexity and quantify the impact of aerosol on numerical weather prediction (NWP). We compare the results of RACM_GOCART and GOCART schemes which use the default climatological model fields for OH, H2O2, and NO3. We find significant reductions of sulfate that are on the order of 40 % to 80 % over the eastern US and are up to 40 % near the Beijing region over China when using the RACM_GOCART scheme. We also evaluate the model performance by comparing it with the Atmospheric Tomography Mission (ATom-1) aircraft measurements in the summer of 2016. FIM-Chem shows good performance in capturing the aerosol and gas-phase tracers. The model-predicted vertical profiles of biomass burning plumes and dust plumes off western Africa are also reproduced reasonably well.

Development of aerosol optical properties for improving the MESSy photolysis module in the GEM-MACH v2.4 air quality model and application for calculating photolysis rates in a biomass burning plume

Abstract. The photolysis module in Environment and Climate Change Canada's online chemical transport model GEM-MACH (GEM: Global Environmental Multi-scale – MACH: Modelling Air quality and Chemistry) was improved to make use of the online size and composition-resolved representation of atmospheric aerosols and relative humidity in GEM-MACH, to account for aerosol attenuation of radiation in the photolysis calculation. We coupled both the GEM-MACH aerosol module and the MESSy-JVAL (Modular Earth Submodel System) photolysis module, through the use of the online aerosol modeled data and a new Mie lookup table for the model-generated extinction efficiency, absorption and scattering cross sections of each aerosol type. The new algorithm applies a lensing correction factor to the black carbon absorption efficiency (core-shell parameterization) and calculates the scattering and absorption optical depth and asymmetry factor of black carbon, sea salt, dust and other internally mixed components. We carried out a series of simulations with the improved version of MESSy-JVAL and wildfire emission inputs from the Canadian Forest Fire Emissions Prediction System (CFFEPS) for 2 months, compared the model aerosol optical depth (AOD) output to the previous version of MESSy-JVAL, satellite data, ground-based measurements and reanalysis products, and evaluated the effects of AOD calculations and the interactive aerosol feedback on the performance of the GEM-MACH model. The comparison of the improved version of MESSy-JVAL with the previous version showed significant improvements in the model performance with the implementation of the new photolysis module and with adopting the online interactive aerosol concentrations in GEM-MACH. Incorporating these changes to the model resulted in an increase in the correlation coefficient from 0.17 to 0.37 between the GEM-MACH model AOD 1-month hourly output and AERONET (Aerosol Robotic Network) measurements across all the North American sites. Comparisons of the updated model AOD with AERONET measurements for selected Canadian urban and industrial sites, specifically, showed better correlation coefficients for urban AERONET sites and for stations located further south in the domain for both simulation periods (June and January 2018). The predicted monthly averaged AOD using the improved photolysis module followed the spatial patterns of MERRA-2 reanalysis (Modern-Era Retrospective analysis for Research and Applications – version 2), with an overall underprediction of AOD over the common domain for both seasons. Our study also suggests that the domain-wide impacts of direct and indirect effect aerosol feedbacks on the photolysis rates from meteorological changes are considerably greater (3 to 4 times) than the direct aerosol optical effect on the photolysis rate calculations.