Atmospheric Chemistry and Physics

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ISSN / EISSN : 1680-7316 / 1680-7324
Published by: Copernicus GmbH (10.5194)
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Zhixiong Chen, , , Xugeng Cheng, Yukun Shen, Mengmiao Yang, Rubin Jiang, Xiangke Liu
Atmospheric Chemistry and Physics Discussions, Volume 22, pp 8221-8240; https://doi.org/10.5194/acp-22-8221-2022

Abstract:
Stratospheric ozone transported to the troposphere is estimated to account for 5 %–15 % of the tropospheric ozone sources. However, the chances of intruded stratospheric ozone reaching the surface are low. Here, we report an event of a strong surface ozone surge of stratospheric origin in the North China Plain (NCP, 34–40 N, 114–121 E) during the night of 31 July 2021. The hourly measurements reveal surface ozone concentrations of up to 80–90 ppbv at several cities over the NCP from 23:00 LST (Local Standard time, = UTC +8 h) on 31 July to 06:00 LST on 1 August 2021. The ozone enhancement was 40–50 ppbv higher than the corresponding monthly mean. A high-frequency surface measurement indicates that this ozone surge occurred abruptly, with an increase reaching 40–50 ppbv within 10 min. A concurrent decline in surface carbon monoxide (CO) concentrations suggests that this surface ozone surge might have resulted from the downward transport of a stratospheric ozone-rich and CO-poor air mass. This is further confirmed by the vertical evolutions of humidity and ozone profiles based on radiosonde and satellite data respectively. Such an event of stratospheric impact on surface ozone is rarely documented in view of its magnitude, coverage, and duration. We find that this surface ozone surge was induced by a combined effect of dying Typhoon In-fa and shallow local mesoscale convective systems (MCSs) that facilitated transport of stratospheric ozone to the surface. This finding is based on analysis of meteorological reanalysis and radiosonde data, combined with high-resolution Weather Research and Forecasting (WRF) simulation and backward trajectory analysis using the FLEXible PARTicle (FLEXPART) particle dispersion model. Although Typhoon In-fa on the synoptic scale was at its dissipation stage when it passed through the NCP, it could still bring down a stratospheric dry and ozone-rich air mass. As a result, the stratospheric air mass descended to the middle-to-low troposphere over the NCP before the MCSs formed. With the pre-existing stratospheric air mass, the convective downdrafts of the MCSs facilitated the final descent of stratospheric air mass to the surface. Significant surface ozone enhancement occurred in the convective downdraft regions during the development and propagation of the MCSs. This study underscores the substantial roles of weak convection in transporting stratospheric ozone to the lower troposphere and even to the surface, which has important implications for air quality and climate change.
, , Duane E. Waliser, Arlindo M. da Silva
Atmospheric Chemistry and Physics, Volume 22, pp 8175-8195; https://doi.org/10.5194/acp-22-8175-2022

Abstract:
Leveraging the concept of atmospheric rivers (ARs), a detection technique based on a widely utilized global algorithm to detect ARs (Guan and Waliser, 2019, 2015; Guan et al., 2018) was recently developed to detect aerosol atmospheric rivers (AARs) using the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis (Chakraborty et al., 2021a). The current study further characterizes and quantifies various details of AARs that were not provided in that study, such as the AARs' seasonality, event characteristics, vertical profiles of aerosol mass mixing ratio and wind speed, and the fraction of total annual aerosol transport conducted by AARs. Analysis is also performed to quantify the sensitivity of AAR detection to the criteria and thresholds used by the algorithm. AARs occur more frequently over, and typically extend from, regions with higher aerosol emission. For a number of planetary-scale pathways that exhibit large climatological aerosol transport, AARs contribute up to a maximum of 80 % to the total annual transport, depending on the species of aerosols. Dust (DU) AARs are more frequent in boreal spring, sea salt AARs are often more frequent during the boreal winter (summer) in the Northern (Southern) Hemisphere, carbonaceous (CA) AARs are more frequent during dry seasons, and often originate from the global rainforests and industrial areas, and sulfate AARs are present in the Northern Hemisphere during all seasons. For most aerosol types, the mass mixing ratio within AARs is highest near the surface. However, DU and CA AARs over or near the African continent exhibit peaks in their aerosol mixing ratio profiles around 700 hPa. AAR event characteristics are mostly independent of species with the mean length, width, and length / width ratio around 4000 km, 600 km, and 7–8, respectively.
, , Ryan Eastman, Mark Smalley,
Atmospheric Chemistry and Physics, Volume 22, pp 8197-8219; https://doi.org/10.5194/acp-22-8197-2022

Abstract:
Pockets of open cells (POCs) have been shown to develop within closed-cell stratocumulus (StCu), and a large body of evidence suggests that the development of POCs result from changes in small-scale processes internal to the boundary layer rather than large-scale forcings. Precipitation is widely viewed as a key process important to POC development and maintenance. In this study, GOES-16 satellite observations are used in conjunction with MERRA-2 winds to track and compare the microphysical and environmental evolution of two populations of closed-cell StCu selected by visual inspection over the southeastern Pacific Ocean: one group that transitions to POCs and another comparison group (CLOSED) that does not. The high spatiotemporal resolution of the new GOES-16 data allows for a detailed examination of the temporal evolution of POCs in this region. We find that POCs tend to develop near the coast, last tens of hours, are larger than 104 km2, and often (88 % of cases) do not re-close before they exit the StCu deck. Most POCs are observed to form at night and tend to exit the StCu during the day when the StCu is contracting in area. Relative to the CLOSED trajectories, POCs have systematically larger effective radii, lower cloud drop number concentrations, a comparable conditional in-cloud liquid water path, and a higher frequency of more intense precipitation. Meanwhile, no systematic environmental differences other than boundary layer height are observed between POC and CLOSED trajectories. Interestingly, there are no differences in reanalysis aerosol optical depth between both sets of trajectories, which may lead one to the interpretation that differences in aerosol concentrations are not influencing POC development or resulting in a large number that re-close. However, this largely depends on the reanalysis treatment of aerosol–cloud interactions, and the product used in this study has no explicit handling of these important processes. These results support the consensus view regarding the importance of precipitation on the formation and maintenance of POCs and demonstrate the utility of modern geostationary remote sensing data in evaluating the POC life cycle.
Atmospheric Chemistry and Physics Discussions, Volume 22, pp 8137-8149; https://doi.org/10.5194/acp-22-8137-2022

Abstract:
Chlorofluorocarbon (CFC) emissions in the latter part of the 20th century reduced stratospheric ozone abundance substantially, especially in the Antarctic region. Simultaneously, polar stratospheric ozone is also destroyed catalytically by nitrogen oxides (NOx = NO + NO2) descending from the mesosphere and the lower thermosphere during winter. These are produced by energetic particle precipitation (EPP) linked to solar activity and space weather. Active chlorine (ClOx = Cl + ClO) can also react mutually with EPP-produced NOx or hydrogen oxides (HOx) and transform both reactive agents into reservoir gases, chlorine nitrate or hydrogen chloride, which buffer ozone destruction by all these agents. We study the interaction between EPP-produced NOx, ClO and ozone over the 20th century by using free-running climate simulations of the chemistry–climate model SOCOL3-MPIOM. A substantial increase of NOx descending to the polar stratosphere is found during winter, which causes ozone depletion in the upper and mid-stratosphere. However, in the Antarctic mid-stratosphere, the EPP-induced ozone depletion became less efficient after the 1960s, especially during springtime. Simultaneously, a significant decrease in stratospheric ClO and an increase in hydrogen chloride – and partly chlorine nitrate between 10–30 hPa – can be ascribed to EPP forcing. Hence, the interaction between EPP-produced NOx/HOx and ClO likely suppressed the ozone depletion, due to both EPP and ClO at these altitudes. Furthermore, at the end of the century, a significant ClO increase and ozone decrease were obtained at 100 hPa altitude during winter and spring. This lower stratosphere response shows that EPP can influence the activation of chlorine from reservoir gases on polar stratospheric clouds, thus modulating chemical processes important for ozone hole formation. Our results show that EPP has been a significant modulator of reactive chlorine in the Antarctic stratosphere during the CFC era. With the implementation of the Montreal Protocol, stratospheric chlorine is estimated to return to pre-CFC era levels after 2050. Thus, we expect increased efficiency of chemical ozone destruction by EPP-NOx in the Antarctic upper and mid-stratosphere over coming decades. The future lower stratosphere ozone response by EPP is more uncertain.
Atmospheric Chemistry and Physics Discussions, Volume 22, pp 8151-8173; https://doi.org/10.5194/acp-22-8151-2022

Abstract:
Previous studies revealed that satellites sensors with the best detection capability identify 25 %–40 % and 0 %–25 % fewer clouds below 0.5 and between 0.5–1.0 km, respectively, over the Arctic. Quantifying the impacts of cloud detection limitations on the radiation flux are critical especially over the Arctic Ocean considering the dramatic changes in Arctic sea ice. In this study, the proxies of the space-based radar, CloudSat, and lidar, CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations), cloud masks are derived based on simulated radar reflectivity with QuickBeam and cloud optical thickness using retrieved cloud properties from surface-based radar and lidar during the Surface Heat Budget of the Arctic Ocean (SHEBA) experiment. Limitations in low-level cloud detection by the space-based active sensors, and the impact of these limitations on the radiation fluxes at the surface and the top of the atmosphere (TOA), are estimated with radiative transfer model Streamer. The results show that the combined CloudSat and CALIPSO product generally detects all clouds above 1 km, while detecting 25 % (9 %) fewer in absolute values below 600 m (600 m to 1 km) than surface observations. These detection limitations lead to uncertainties in the monthly mean cloud radiative forcing (CRF), with maximum absolute monthly mean values of 2.5 and 3.4 Wm−2 at the surface and TOA, respectively. Cloud information from only CALIPSO or CloudSat lead to larger cloud detection differences compared to the surface observations and larger CRF uncertainties with absolute monthly means larger than 10.0 Wm−2 at the surface and TOA. The uncertainties for individual cases are larger – up to 30 Wm−2. These uncertainties need to be considered when radiation flux products from CloudSat and CALIPSO are used in climate and weather studies.
Shijie Cui, Dan Dan Huang, Yangzhou Wu, Junfeng Wang, Fuzhen Shen, Jiukun Xian, , Hongli Wang, , Hong Liao, et al.
Atmospheric Chemistry and Physics, Volume 22, pp 8073-8096; https://doi.org/10.5194/acp-22-8073-2022

Abstract:
Refractory black carbon (rBC) aerosols play an important role in air quality and climate change, yet highly time-resolved and detailed investigations on the physicochemical properties of rBC and its associated coating are still scarce. In this work, we used a laser-only Aerodyne soot particle aerosol mass spectrometer (SP-AMS) to exclusively measure rBC-containing (rBCc) particles, and we compared their properties with those of the total nonrefractory submicron particles (NR-PM1) measured in parallel by a high-resolution AMS (HR-AMS) in Shanghai. Observations showed that, overall, rBC was thickly coated, with an average mass ratio of coating to rBC core (RBC) of ∼5.0 (±1.7). However, the ratio of the mass of the rBC-coating species to the mass of those species in NR-PM1 was only 19.1 (±4.9) %; sulfate tended to condense preferentially on non-rBC particles, so the ratio of the sulfate on rBC to the NR-PM1 sulfate was only 7.4 (±2.2) %, while the majority (72.7±21.0 %) of the primary organic aerosols (POA) were associated with rBC. Positive matrix factorization revealed that organics emitted from cooking did not coat rBC, and a portion of the organics that coated rBC was from biomass burning; such organics were unidentifiable in NR-PM1. Small rBCc particles were predominantly from traffic, while large-sized ones were often mixed with secondary components and typically had a thick coating. Sulfate and secondary organic aerosol (SOA) species were generated mainly through daytime photochemical oxidation (SOA formation, likely associated with in situ chemical conversion of traffic-related POA to SOA), while nocturnal heterogeneous formation was dominant for nitrate; we also estimated an average time of 5–19 h for those secondary species to coat rBC. During a short period that was affected by ship emissions, particles were characterized as having a high vanadium concentration (on average 6.3±3.1 ng m−3) and a mean vanadium/nickel mass ratio of 2.0 (±0.6). Furthermore, the size-resolved hygroscopicity parameter (κrBCc) of rBCc particles was obtained based on their full chemical characterization, and was parameterized as κrBCc(x)=0.29–0.14 × exp⁡(-0.006×x) (where x ranges from 150 to 1000 nm). Under critical supersaturations (SSC) of 0.1 % and 0.2 %, the D50 values were 166 (±16) and 110 (±5) nm, respectively, and 16 (±3) % and 59 (±4) %, respectively, of the rBCc particles by number could be activated into cloud condensation nuclei (CCN). Our findings are valuable for advancing the understanding of BC chemistry as well as the effective control of atmospheric BC pollution.
, Magdalena Okuljar, , Joni Kalliokoski, Jiali Shen, , Markus Lampimäki, Yusheng Wu, , , et al.
Atmospheric Chemistry and Physics, Volume 22, pp 8097-8115; https://doi.org/10.5194/acp-22-8097-2022

Abstract:
The occurrence of new particle formation (NPF) events detected in a coastal agricultural site, at Qvidja, in Southwestern Finland, was investigated using the data measured with a nitrate ion-based chemical-ionization atmospheric-pressure-interface time-of-flight (CI-APi-TOF) mass spectrometer. The binned positive matrix factorization method (binPMF) was applied to the measured spectra. It resulted in eight factors describing the time series of ambient gas and cluster composition at Qvidja during spring 2019. The most interesting factors related to the observed NPF events were the two factors with the highest mass-to-charge ratios, numbered 7 and 8, both having profiles with patterns of highly oxygenated organic molecules with one nitrogen atom. It was observed that factor 7 had elevated intensities during the NPF events. A variable with an even better connection to the observed NPF events is fF7, which denotes the fraction of the total spectra within the studied mass-to-charge ratio range between 169 and 450 Th being in a form of factor 7. Values of fF7 higher than 0.50±0.05 were observed during the NPF events, of which durations also correlated with the duration of fF7 exceeding this critical value. It was also observed that factor 8 acts like a precursor for factor 7 with solar radiation and that the formation of factor 8 is associated with ozone levels.
Mingfu Cai, , Baoling Liang, Qibin Sun, , , Min Shao, , Wei Chen, Qicong Song, et al.
Atmospheric Chemistry and Physics Discussions, Volume 22, pp 8117-8136; https://doi.org/10.5194/acp-22-8117-2022

Abstract:
Organic aerosol (OA) has a significant contribution to cloud formation and hence climate change. However, high uncertainties still exist in its impact on global climate, owing to the varying physical properties affected by the complex formation and aging processes. In this study, the hygroscopicity, volatility, cloud condensation nuclei (CCN) activity, and chemical composition of particles were measured using a series of online instruments at a rural site in the Pearl River Delta (PRD) region of China in fall 2019. During the campaign, the average hygroscopicity of OA (κOA) increased from 0.058 at 30 nm to 0.09 at 200 nm, suggesting a higher oxidation state of OA at larger particle sizes, supported by a higher fraction of extremely low volatility OA (ELVOA) for larger size particles. Significantly different diurnal patterns of κOA were observed between Aitken mode particles and accumulation mode particles. For Aitken mode particles (30–100 nm), the κOA values showed daily minima (0.02–0.07) during daytime, while the accumulation mode exhibited a daytime peak (∼ 0.09). Coincidently, a daytime peak was observed for both aged biomass burning organic aerosol (aBBOA) and less oxygenated organic aerosol (LOOA) based on source apportionment, which was attributed to the aging processes and gas–particle partitioning through photochemical reactions. In addition, the fraction of semi-volatile OA (SVOA) was higher at all measured sizes during daytime than during nighttime. These results indicate that the formation of secondary OA (SOA) through gas–particle partitioning can generally occur at all diameters, while the aging processes of pre-existing particles are more dominated in the accumulation mode. Furthermore, we found that applying a fixed κOA value (0.1) could lead to an overestimation of the CCN number concentration (NCCN) up to 12 %–19 % at 0.1 %–0.7 % supersaturation (SS), which was more obvious at higher SS during daytime. Better prediction of NCCN could be achieved by using size-resolved diurnal κOA, which indicates that the size dependence and diurnal variations in κOA can strongly affect the NCCN at different SS values. Our results highlight the need for accurately evaluating the atmospheric evolution of OA at different size ranges and their impact on the physicochemical properties and hence climate effects.
, , Matthew C. Boyer, Jai Prakash Chaubey,
Atmospheric Chemistry and Physics Discussions, Volume 22, pp 8059-8071; https://doi.org/10.5194/acp-22-8059-2022

Abstract:
The impact of aerosols on clouds is a well-studied, although still poorly constrained, part of the atmospheric system. New particle formation (NPF) is thought to contribute 40 %–80 % of the global cloud droplet number concentration, although it is extremely difficult to observe an air mass from NPF to cloud formation. NPF and growth occurs frequently in the Canadian Arctic summer atmosphere, although only a few studies have characterized the source and properties of these aerosols. This study presents cloud condensation nuclei (CCN) concentrations measured on board the CCGS Amundsen in the eastern Canadian Arctic Archipelago from 23 July to 23 August 2016 as part of the Network on Climate and Aerosols: Addressing Uncertainties in Remote Canadian Environments (NETCARE). The study was dominated by frequent ultrafine particle and/or growth events, and particles smaller than 100 nm dominated the size distribution for 92 % of the study period. Using κ-Köhler theory and aerosol size distributions, the mean hygroscopicity parameter (κ) calculated for the entire study was 0.12 (0.06–0.12, 25th–75th percentile), suggesting that the condensable vapours that led to particle growth were primarily slightly hygroscopic, which we infer to be organic. Based on past measurement and modelling studies from NETCARE and the Canadian Arctic, it seems likely that the source of these slightly hygroscopic, organic, vapours is the ocean. Examining specific growth events suggests that the mode diameter (Dmax) had to exceed 40 nm before CCN concentrations at 0.99 % supersaturation (SS) started to increase, although a statistical analysis shows that CCN concentrations increased 13–274 cm−3 during all ultrafine particle and/or growth times (total particle concentrations >500 cm−3, Dmax<100 nm) compared with background times (total concentrations <500 cm−3) at SS of 0.26 %–0.99 %. This value increased to 25–425 cm−3 if the growth times were limited to times when Dmax was also larger than 40 nm. These results support past results from NETCARE by showing that the frequently observed ultrafine particle and growth events are dominated by a slightly hygroscopic fraction, which we interpret to be organic vapours originating from the ocean, and that these growing particles can increase the background CCN concentrations at SS as low as 0.26 %, thus pointing to their potential contribution to cloud properties and thus climate through the radiation balance.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, , , , Tom Ryerson, Carsten Warneke, , et al.
Atmospheric Chemistry and Physics, Volume 22, pp 8009-8036; https://doi.org/10.5194/acp-22-8009-2022

Abstract:
Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.
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