Aerosol Composition Research Articles

Balancing water conservation and health: do water-saving showerheads impact the microbes we breathe in during showering?

Low-flow showerheads offer consumers economic and water-saving benefits, yet their use may inadvertently affect the microbial content of produced water and water-associated aerosols. This study aimed to compare the abundance and microbial composition of bacteria in shower water and associated respirable aerosols produced by various low flow rate (1, 1.5, and 1.8 gpm) showerheads. Our findings indicate that the lowest-flow showerhead produces water with lower total microbial and opportunistic bacterial pathogen densities compared to higher low flow rate counterparts. However, microbiome analysis revealed that 1.8 gpm flow rate showerheads exhibit reduced abundance of Gram-negative organisms and common biofilm-forming organisms, suggesting potentially lower pathogenicity compared to 1 and 1.5 gpm low-flow showerheads. Additionally, the number of respirable aerosols produced by showerheads as well as the partitioning of certain microorganisms from the water to aerosol phases was negatively correlated with flow rate, suggesting that there may be increasing exposure potential to pathogenic bioaerosols when using a 1gpm showerhead compared to a 1.8 gpm showerhead. However, the 1.5 gpm showerhead seemed to balance microbial partitioning, aerosol generation, and water conservation. Moreover, the microbial composition of aerosols produced from shower water was more influenced by the age of the showerhead than the flow rate, highlighting the significance of biofilm formation on the microbial community. Overall, our findings underscore the importance of evaluating the microbial risk associated with low-flow showerheads using multiple metrics in both water and aerosols, and dynamically assessing this over time, to ensure accurate future risk assessment.

Temporal variation characteristics of microbial aerosols in the goose house environment

ABSTRACT 1. Preventing disease is important in poultry production systems, but this has mainly been studied in chickens. The aim of this study is to explore the impact of microbial aerosols in intensive goose house environments. 2. To evaluate the environmental quality of geese housing, fine particulate matter (PM2.5) was collected using an ambient air particulate matter sampler. High-throughput sequencing was used to analyse bacterial diversity and relative abundance. Results showed that the number of general and operational taxonomic units (OTUs) were 1,578 and 19 112 in all PM2.5 samples. Firmicutes, Bacteroidota, Proteobacteria, Acidobacterota were the four most abundant phyla in PM2.5. 3. Compared with bacterial phyla in the PM2.5 from chicken houses, those in the genus Acidobacterota were increased in goose housing. There are various genera of bacteria present in PM2.5, and their composition was similar across different samples. No significant change was observed in the diversity of microbiota in the PM2.5, although multiple pathogenic bacteria were detected. 4. A prediction function showed that a variety of bacterial phyla correlated positively with the human diseases. 5. In summary, the microbial aerosols in the goose shed pose significant risks to the health of the geese. Regular monitoring of the composition of microbial aerosols is important for the healthy growth of geese and disease prevention and control.

Reaction Kinetics and Secondary Organic Aerosol Composition Analysis of 2-Cyclohexen-1-one with NO3 Radicals

Reaction Kinetics and Secondary Organic Aerosol Composition Analysis of 2-Cyclohexen-1-one with NO3 Radicals

Validation of aerosol chemical composition and optical properties provided by Copernicus Atmosphere Monitoring Service (CAMS) using ground-based global data

Monitoring particulate matter (PM) air pollution in terms of both concentration and composition, is very important due to its effects on human health and climate. In the PRIMARY project we aim at retrieving the aerosol composition from space using the hyperspectral observations from the Italian Space Agency's PRISMA mission. To this end, we are developing a machine learning algorithm trained with synthetic top-of-atmosphere reflectances and underlying aerosol fields. As part of this process, we plan to use the global forecasts from the Copernicus Atmosphere Monitoring Service (CAMS) as the core to generate this synthetic dataset. However, to proceed in this direction, a preliminary assessment of the reliability of this model-based dataset when compared to observations is necessary, also to bias correct the output if needed. With this aim, we assess the representation of the aerosol chemical composition and the related optical properties at selected globally distributed sites in CAMS, comparing the simulations with near-surface aerosol chemical analyses from the SPARTAN network and column sun-photometer observations from the AERONET network. We found that CAMS forecasts skills changed over time due to updates in the modelling system, with the latter two version cycles (46 and 47) being similar. Generally, they reproduce the aerosol composition within a factor of 2. We found a substantial overestimation of organic matter (OM) by a factor of 3. Applying a correcting factor to OM (constant at the global level) warrants a much more realistic representation of PM2.5 total mass and relative fraction of single species in CAMS. From the so derived CAMS aerosol-speciated profiles, we calculate aerosol optical properties, needed for subsequent use in a radiative transfer model. Comparison against AERONET indeed shows that OM bias correction resulted in improvements in Extinction Ångstrom Exponent (α440nm870nm). Aerosol Optical Depth (AOD), Single Scattering Albedo (SSA) and Asymmetry Parameter (g) simulations resulted slightly degraded, confirming the possibility of using CAMS as the base for a synthetic retrieval training dataset.

Experimental Study on Composition and Optic of Secondary Organic Aerosol Generated by Aqueous Photoxidation of Toluene in Presence of Copper Ions

Experimental Study on Composition and Optic of Secondary Organic Aerosol Generated by Aqueous Photoxidation of Toluene in Presence of Copper Ions

Multi-Decadal Trends in Aerosol Optical Depth of the Main Aerosol Species Based on MERRA-2 Reanalysis: A Case Study in the Baltic Sea Basin

This study analyses the trends of total aerosol and the main aerosol species over nine capitals in the Baltic Sea basin from 1989 to 2019 based on the Modern-Era Retrospective Analysis for Research and Applications, Version 2 Reanalysis. Aerosol speciation includes mineral dust, sea salt, sulphate (SO4), organic carbon (OC), and black carbon (BC). The mean total aerosol optical depth (AOD) values were the highest (up to 0.216) over the continental capitals (i.e., Warsaw, Berlin, and Vilnius). For each capital, the mean SO4 AOD was the main aerosol species, with a trend specular to total AOD. Apart from Warsaw, the mean BC AOD was the aerosol species with the lowest level. The composition of aerosols changed with respect to the species of anthropogenic origins (i.e., SO4, OC, and BC), with the percentage contribution to the total AOD decreasing for the SO4 AOD and increasing for the BC AOD. Also, the OC AOD showed an increase in the percentage contribution to total AOD for Copenhagen, Oslo, Stockholm, and the continental capitals. Anthropogenic aerosols contributed up to 90.3% of the total AOD, with the highest values over the continental capitals. For each capital, the minimum in the percentage contribution of anthropogenic AOD was between 2007 and 2008, likely due to the global financial crisis. Anthropogenic AOD as a percentage of the total AOD decreased from 1989 to 2008. Both the total and the SO4 AODs decreased over each capital. By contrast, the BC AOD increased over Stockholm, and both the OC and BC AODs increased over Berlin, Copenhagen, and Oslo. The decoupling of carbonaceous aerosols and the SO4 AOD trends was likely due to concurrent factors such as biomass burning and low-sulphur fuel policies. From 2000 to 2019, the inverse relationships between gross domestic products and SO4 AODs suggest a relative decoupling of economic growth from fossil fuels for Oslo, Stockholm, Tallinn, and Vilnius.

Characterization of aerosol composition: Insights from SEM-EDX analysis and CALIPSO overpasses

The effect of atmospheric aerosols on the earth’s radiation budget is primarily through their direct effects. Understanding aerosols’ morphology and elemental composition is crucial in this context. For two years, from January 2017 to December 2018, aerosol samples (PM10) were collected on quartz filter papers using a high-volume sampler (PM10) in Chennai, a semi-urban coastal environment located at 12.81°N, 80.03°E. These filter papers were stored under ambient laboratory conditions and were subsequently subjected to ultrasonication using ethanol as the solvent to separate the aerosols from the filters. The extracted samples were then analyzed using scanning electron microscopy (SEM) for the morphology and energy dispersive X-ray analysis (EDX) for elemental composition. The EDX analysis of the samples revealed the presence of various elements such as carbon (C), oxygen (O), aluminum (Al), silicon (Si), sulfur (S), potassium (K), iron (Fe), magnesium (Mg), calcium (Ca), vanadium (V), bismuth (Bi), sodium (Na), chlorine (Cl), phosphorus (P), and technetium (Tc). High concentrations of carbon, oxygen, and aluminum–silicate particles indicated the presence of carbonaceous aerosols and wind-blown dust particles. Concentration-weighted trajectory (CWT) analysis was carried out to assess the transport pathways of aerosols in the region. CALIPSO overpasses during the study period were selected, and the Vertical Feature Mask (VFM) identifiers for different aerosol types were compared with the local experimental results. The findings show that CALIPSO possess a reasonably effective capability in detecting and characterizing the local aerosol types. CALIPSO detected Dusty marine, Clean marine, Elevated smoke and Polluted dust in the study area across all four seasons. These findings closely match the characteristics of such aerosol types obtained from SEM/EDX analysis, HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) modeling, and the Angstrom exponent derived from sunphotometer readings.

Measurements of Water-Soluble Ions in Particulate Matter 2.5 in Polish Rural Areas: Identifying Possible Sources

Limited data on rural Poland's atmospheric ion concentrations exists, with no publicly available monitoring data in urban areas. These knowledge gaps hinder the comparison of concentrations across environments and the identification of their sources. This study examines water-soluble ions across five rural locations in Poland over four years to investigate their concentrations and sources in the atmosphere. This study explores aerosol origins, performing a four-year correlation analysis across five locations to reveal ion relationships. Notably, sulfate (SO₄2⁻), nitrate (NO₃⁻), and ammonium (NH₄⁺) exhibit significant correlations ranging from 0.3 to 0.8, suggesting a common pollution source in all analyzed rural locations. Interestingly, magnesium (Mg2⁺) and sodium (Na⁺) in two locations demonstrated a strong correlation, ranging between 0.4 and 0.9, suggesting the influence of sea spray on these sites. Principal component analysis is used to investigate the factors influencing ion concentrations, revealing distinctive patterns for each location and explaining the total variances ranging from 74.9% to 84.8%. This underscores the significance of geographical and environmental factors. The study's novelty lies in its thorough and long-term analysis of water-soluble ion concentrations across rural Poland, providing an extensive dataset for the region. The study fills a data gap on rural pollution sources and reveals consistent ion patterns across different sites and seasons. The findings emphasize geographical and environmental impacts on aerosol composition and suggest common pollution sources for all areas. This research encourages further investigations into the stability and origins of ions in rural environments, providing valuable insights for local and broader atmospheric studies.

Light Absorption and Chemical Composition of Brown Carbon Organic Aerosol Produced from Burning of Selected Biofuels

Light Absorption and Chemical Composition of Brown Carbon Organic Aerosol Produced from Burning of Selected Biofuels

Regime shift in secondary inorganic aerosol formation and nitrogen deposition in the rural United States

Secondary inorganic aerosols play an important role in air pollution and climate change, and their formation modulates the atmospheric deposition of reactive nitrogen (including oxidized and reduced nitrogen), thus impacting the nitrogen cycle. Large-scale and long-term analyses of secondary inorganic aerosol formation based on model simulations have substantial uncertainties. Here we improve constraints on secondary inorganic aerosol formation using decade-long in situ observations of aerosol composition and gaseous precursors from multiple monitoring networks across the United States. We reveal a shift in the secondary inorganic aerosol formation regime in the rural United States between 2011 and 2020, making rural areas less sensitive to changes in ammonia concentrations and shortening the effective atmospheric lifetime of reduced forms of reactive nitrogen. This leads to potential increases in reactive nitrogen deposition near ammonia emission hotspots, with ecosystem impacts warranting further investigation. Ammonia (NH3), a critical but not directly regulated precursor of fine particulate matter in the United States, has been increasingly scrutinized to improve air quality. Our findings, however, show that controlling NH3 became significantly less effective for mitigating fine particulate matter in the rural United States. We highlight the need for more collocated aerosol and precursor observations for better characterization of secondary inorganic aerosols formation in urban areas.

Effects of photochemical aging on the molecular composition of organic aerosols derived from agricultural biomass burning in whole combustion process

Biomass burning organic aerosols (BBOA) are key components of atmospheric particulate matter, yet the effects of aging process on their chemical composition and related properties remain poorly understood. In this study, fresh smoke emissions from the combustion of three types of agricultural biomass residues (rice, maize, and wheat straws) were photochemically aged in an oxidation flow reactor. The changes in BBOA composition were characterized by offline analysis using ultrahigh performance liquid chromatography coupled with Orbitrap mass spectrometry. The BBOA molecular composition varied dramatically with biomass type and aging process. Fresh and aged BBOA were predominated by CHO and nitrogen-containing CHON, CHN, and CHONS species, while with very few CHOS and other non‑oxygen species. The signal peak area variations revealed that individual molecular species underwent dynamic changes, with 77–81 % of fresh species decreased or even disappeared and 33–46 % of aged species being newly formed. A notable increase was observed in the number and peak area of CxHyO≥6 compounds in aged BBOA, suggesting that photochemical process served as an important source of highly oxygenated species. Heterocyclic CxHyN2 compounds mostly dominated in fresh CHN species, whereas CxHyN1 were more abundant in aged ones. Fragmentation and homologs oxidation by addition of oxygen-containing functional groups were important pathways for the BBOA aging. The changes in BBOA composition with aging would have large impacts on particle optical properties and toxicity. This study highlights the significance of photochemical aging process in altering chemical composition and related properties of BBOA.

Selective molecular characterization of organic aerosols using in situ laser desorption ionization mass spectrometry.

The sources and chemical compositions of organic aerosol (OA) exert a significant influence on both regional and global atmospheric conditions, thereby having far-reaching implications on environmental chemistry. However, existing mass spectrometry (MS) methods have limitations in characterizing the detailed composition of OA due to selective ionization as well as fractionation during cold-water extraction and solid-phase extraction (SPE). A comprehensive MS study was conducted using aerosol samples collected on dusty, clean, and polluted days. To supplement the data obtained from electrospray ionization (ESI), a strategy for analyzing OAs collected using the quartz fiber filter directly utilizing laser desorption ionization (LDI) was employed. Additionally, the ESI method was conducted to explore suitable approaches for determining various OA compositions from samples collected on dusty, clean, and polluted days. In situ LDI has the advantages of significantly reducing the sample volume, simplifying sample preparation, and overcoming the problem of overestimating sulfur-containing compounds usually encountered in ESI. It is suitable for the characterization of highly unsaturated and hydrophobic aerosols, such as brown carbon-type compounds with low volatility and high stability, which is supplementary to ESI. Compared with other ionization methods, in situ LDI helps provide a complementary description of the molecular compositions of OAs, especially for analyzing OAs in polluted day samples. This method may contribute to a more comprehensive MS analysis of the elusive compositions and sources of OA in the atmosphere.

Investigating the convective transport possibilities of lower-atmospheric pollutants to the UTLS region using rainwater and aerosol chemical characterization

Various attempts using different platforms to understand the chemical composition of the Asian Tropopause Aerosol Layer (ATAL) have concluded that it primarily consists of nitrate (NO3−) aerosols. Recent in-situ measurements from aircraft flying through ATAL have suggested that ammonia (NH3) pollution from Asia could serve as the precursor for nitrate aerosols in ATAL through gas-to-particle formation after undergoing convective uplift to the Upper Troposphere and Lower Stratosphere (UTLS) regions. In this study, we aimed to investigate the potential pathways of convective transport of lower-atmospheric pollutants by analysing the chemical composition of rainwater and aerosols in a highly convective region, Kolkata (Head Bay of Bengal), India. We utilized the PILS-IC system established at Kolkata Camp Observatory of the National Atmospheric Research Laboratory (KCON). The analysis revealed a significant dominance of NH4+ and NO3− ions in both rainwater and aerosol samples during the monsoon and post-monsoon seasons, with the dominance increasing during the post-monsoon season. Air mass trajectories indicated a clear influence of the Indo-Gangetic Plain (IGP) region during the post-monsoon season, which is well-known for its dense agricultural activities and industries. High concentrations of NH3 even at higher altitudes, have been observed in Atmospheric Infrared Sounder (AIRS) measurements. Moreover, using Outgoing Longwave Radiation (OLR) and vertical wind as proxies for tropical deep convection and updrafts/downdrafts, respectively, we found evidence supporting the possibility of convective transport of these lower-atmospheric pollutants to the UTLS regions during the monsoon season. In conclusion, this study provides evidence for the potential convective transport of lower-atmospheric pollutants, including NH3 and other precursor gases, to higher levels. These pollutants could partially serve as the source of nitrate aerosols in the ATAL through gas-to-particle formation processes.

Aerosol sources and transport paths co-control the atmospheric bacterial diversity over the coastal East China Sea

Airborne bacteria along with chemical composition of aerosols were investigated during five sampling seasons at an offshore island of the East China Sea. Bacterial diversity was the lowest in spring, the highest in winter, and similar between the autumns of 2019 and 2020, suggesting remarkably seasonal variation but little interannual change. Geodermatophilus (Actinobacteria) was the indicator genus of mineral dust (MD) showed higher proportion in spring than in other seasons. Mastigocladopsis_PCC-10914 (Cyanobacteria) as the indicator of sea salt (SS) demonstrated the highest percentages in both autumns, when the air masses mainly passed over the ocean prior to the sampling site. The higher proportions of soil-derived genera Rubellimicrobium and Craurococcus (both Proteobacteria) and extremophile Chroococcidiopsis_SAG_2023 (Cyanobacteria) were found in summer and winter, respectively. Our study explores the linkage between aerosol source and transport path and bacterial composition, which has implication to understanding of land-sea transmission of bacterial taxa.

Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany

Abstract. The composition, sources and chemical transformation of volatile organic compounds (VOCs) and organic aerosol (OA) particles were investigated during July–August 2021 at a rural forested site in southwest Germany, 10 km north of the city of Karlsruhe. VOCs and semi-volatile OA particles were measured with a proton-transfer-reaction mass spectrometer coupled to the CHemical Analysis of aeRosols ONline particle inlet (CHARON–PTR-MS). The CHARON-measured OA mass accounted for 62 ± 18 % on average of the total OA mass (4.2 ± 2.8 µg m−3) measured concurrently with an aerosol mass spectrometer (AMS). The total concentrations of measured VOCs ranged from 7.6 to 88.9 ppb with an average of 31.2 ± 13.4 ppb. Positive matrix factorization (PMF) was used to identify major source factors of VOCs and OA particles. Three types of oxygenated VOC (OVOC), namely aromatic OVOCs, biogenic OVOCs and aged OVOCs, contributed on average 11 % ± 9 %, 37 % ± 29 % and 29 % ± 21 % of total VOC concentrations, respectively. The results of AMS–PMF indicated substantial contributions of oxygenated organic compounds to OA particle mass. Three secondary OA (SOA) factors determined by CHARON–PMF analysis, namely aromatic SOA (5 % ± 7 %), daytime biogenic SOA (17 % ± 17 %) and nighttime biogenic SOA (28 % ± 21 %), consistently showed high contributions to the total CHARON-measured OA mass. Nighttime particle growth was observed regularly in this area, which was mainly attributed to the semi-volatile organic compounds and organic nitrates formed from the oxidation of monoterpenes and sesquiterpenes. This study presents the major sources, real-time transformations of VOCs and OA particles, and nighttime particle formation characteristics for central European forested areas.

Long-term quantification of springtime aerosols over Saudi Arabia using multi-satellite remotely sensed data.

A comprehensive analysis of aerosol characteristics over Saudi Arabia from 2005 to 2022, utilizing high-resolution satellite-based observations and reanalysis datasets, examining the distribution of aerosols and their subtypes across the three dimensions (temporal, spatial, and altitude based) for March, April, and May. This study focuses on the analysis of parameters such as aerosol optical depth (AOD), angstrom exponent (AE), absorption aerosol optical depth (AAOD), and Ultraviolet Aerosol Index (UVAI), revealing significant spatial disparities, with elevated aerosol concentrations in the central and eastern regions and comparatively lower concentrations along the western coastal areas. In this study, the spatial patterns and temporal trends are analyzed through trajectory modeling. The study also investigates the composition of aerosols in various Saudi cities. Aerosols prevailing in a dozen Saudi Arabian cities were systematically categorized into six sub-types, considering their particle size and UV-absorbing properties. Notably, two major aerosol sub-types, absorbing coarse (AC) aerosols (UVAI > 0.25, AE < 0.70) treated as mineral dust and absorbing mixed (AM) aerosols (0.70 < AE < 1.25) along with neutral fine (NF) particles (- 0.5 < UVAI < 0.25, AE > 1.25) treated as urban, predominate across the Kingdom of Saudi Arabia.

Chemical composition, source characteristics, and hygroscopic properties of organic-enriched aerosols in the high Arctic during summer

Arctic regions are extremely sensitive to global warming. Aerosols are one of the most important short-lived climate-forcing agents affecting the Arctic climate. The present study examines the summertime chemical characteristics and potential sources of various organic and inorganic aerosols at a Norwegian Arctic site, Ny-Ålesund (79°N). The results show that organic matter (OM) accounts for 60 % of the total PM10 mass, followed by sulfate (SO42−). Water-soluble organic carbon (WSOC) contributes 62 % of OC. Photochemical processes involving diverse anthropogenic and biogenic precursor compounds are identified as the major sources of WSOC, while water-insoluble organic carbon (WIOC) aerosols are predominantly linked to primary marine emissions. Despite being a remote pristine site, the aerosols show a sign of chemical aging, evidenced by a significant chloride depletion, which was about 82 % on average during the study period. Nitrogen-containing aerosols are likely stemming from migratory seabird colonies and local dust sources around the sampling site. While biogenic, crustal, and sea salt-derived SO42- account for 37%, 8%, and 5% respectively, the remaining 50% is attributed to anthropogenic SO42-. Through chemical tracers, Pearson correlation coefficient matrix, and Hierarchical Cluster Analysis (HCA), the present study identifies soil biota (terrestrial biogenic) and marine emissions, along with their photochemical oxidation processes, as potential sources of Arctic aerosols during summer, while biomass burning and combustion-related sources have a minor contribution. The chemical closure of hygroscopicity highlights that while organics predominantly control aerosol hygroscopicity in the Arctic summer, specific inorganic components like (NH4)2SO4 can significantly increase it on certain days, affecting aerosol-cloud interactions and climate processes over the Arctic during summer. The present study highlights the high abundance of organics and their vital role in the Arctic climate during summer when natural aerosols are conquered.

Air Composition over the Russian Arctic–4: Atmospheric Aerosols

This work presents the analysis of the spatial distribution of number concentration, size distribution, and chemical composition of aerosol particles measured for the first time over the seas of the Russian Arctic. Various types of vertical distribution of the number concentration were recorded, characteristic of both coastal marine and continental areas. Most of them turned out to be of the continental type. Attention is also drawn to the almost complete absence of coarse particles above 2–3 km over all seas. The chemical composition of the Arctic aerosol at altitudes of both 200 m and 5000 m contains ions that can be referred to as both marine and continental. The identifiable carbon- and salt-free elemental part of the aerosol over the Arctic is 3–4 times larger than that of ions. Over all seas and at both altitudes, the Arctic aerosols mainly contain elements of terrigenous origin – Al, Cu, Fe, and Si. Over almost all seas, except the Barents Sea, Si is dominant in the elemental composition of the aerosol, its contribution over the Chukchi Sea reaching 85%. The analysis of backward trajectories showed that in all cases considered, whether the aerosol was formed over the continent or sea, air trajectories passed both over sea and over land. In this case, the formed particles could be enriched with additional ions and elements along their pathway. This work completes a cycle of the papers, devoted to studying air composition, which was carried out over the seas of the Russian Arctic in September 2020. Our results can be used to model the atmospheric processes occurring in the Arctic under the conditions of changing climate.

Reply to: “Comment on ‘Stratospheric Aerosol Composition Observed by the Atmospheric Chemistry Experiment Following the 2019 Raikoke Eruption’ by Boone et al.” by Ansmann et al.

AbstractThe question of stratospheric aerosol type following the Raikoke eruption is revisited. Raman lidar measurements suggest the aerosols are predominately smoke, while Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE‐FTS) results indicate the aerosols are predominately sulfate aerosols. The suggested mechanism of smoke particles self‐lofting into the stratosphere is inconsistent with observations in 2020, when more severe Siberian fires failed to invoke a response even vaguely similar to 2019. A side‐by side comparison of the Sarychev and Raikoke eruptions invalidates model calculations that suggest sulfate aerosols should be at levels too low to explain the observed aerosol loading. Structure in infrared absorption spectra provides conclusive evidence of composition, a unique fingerprint for identifying aerosol type. Such information cannot be misinterpreted so long as there is sufficient resolution and spectral coverage. ACE‐FTS infrared aerosol spectra often have an order of magnitude stronger absorption than that of background sulfate aerosols. These spectra can be accurately reproduced by laboratory measured sulfate aerosol spectroscopic information, providing unambiguous identification of the aerosols as sulfate. Visual inspection of thousands of infrared aerosol spectra from the period following the Raikoke eruption indicates the aerosols in the lower stratosphere are predominately sulfate, with no indication of smoke. The lidar study's identification of the aerosols as smoke was based primarily on observed lidar ratios that were more consistent with a material that absorbed significantly at the lidar wavelengths, inconsistent with expectations for sulfate aerosols. However, this could indicate the presence of a substance dissolved in the sulfate aerosols absorbing at those wavelengths rather than smoke particles.

Comment on “Stratospheric Aerosol Composition Observed by the Atmospheric Chemistry Experiment Following the 2019 Raikoke Eruption” by Boone et al.

AbstractBased on satellite observations in the Arctic stratosphere at latitudes from 61° to 66°N in the second half of 2019, Boone et al. (2022, https://doi.org/10.1029/2022jd036600) provide the impression that the aerosol in the upper troposphere and lower stratosphere (UTLS) over the entire Arctic consisted of sulfate aerosol originating from the Raikoke volcanic eruption in the summer of 2019. Here, we show that this was most probably not the case and the aerosol layering conditions were much more complex. By combining the stratospheric aerosol typing results of Boone et al. (2022, https://doi.org/10.1029/2022jd036600) with lidar observations at 85°–86°N of Ohneiser et al. (2021, https://doi.org/10.5194/acp‐21‐15783‐2021) of a dominating wildfire smoke layer in the UTLS height range, we demonstrate that the Arctic UTLS aerosol most likely consisted of Siberian wildfire smoke in the lower part and sulfate aerosol in the upper part of the aerosol layer which extended from 7 to 19 km height and was well observable until May 2020. The smoke‐ and sulfate‐related aerosol optical thickness (AOT) fractions were about 0.7–0.8 and 0.2–0.3, respectively, according to our analysis. The sulfate AOT is in good agreement with model‐based predictions of the Raikoke sulfate AOT.