Pub Date : 2024-07-05DOI: 10.5194/egusphere-2024-2008
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, Ulla Wandinger
<strong>Abstract.</strong> The number of wildfire smoke layers in the upper troposphere per fire season increased at mid and high northern latitudes during the last years. To consider smoke in weather and climate models appropriately, the influence of smoke on a variety of atmospheric processes needs to be explored in detail. In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. The complex study is based on aerosol and ice cloud observations in the central Arctic during the one-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. For almost a year (from the summer of 2019 to the spring of 2020), aged Siberian wildfire smoke polluted the tropopause region over the central Arctic and many cirrus systems developed in the polluted upper troposphere. Goal of the data analysis (part 1) is to provide observational evidence for a dominating impact of aged wildfire smoke (organic aerosol particles) on cirrus formation in the central Arctic (over the MOSAiC research icebreaker Polarstern) during the winter half year of 2019–2020. Aim of the simulations in part 2 is to gain a deeper and more detailed insight into the potential smoke impact on ice nucleation as a function of observed aerosol and meteorological conditions (temperature, relative humidity) and by considering realistic gravity wave characteristics (updraft speed, wave amplitude). Vertical movements of air parcels are essential to initiate cloud formation. The measurements presented in part 1 were conducted during the winter half year (October to March), aboard the ice breaker Polarstern. The research vessel Polarstern drifted with the pack ice in the central Arctic mainly at latitudes >85 °N during the winter half year. The cirrus statistics show typical properties of ice clouds of the synoptic cirrus category (top-down generation of cirrus structures). The ice clouds mostly started to evolve at heights close to the tropopause. Cirrus top temperatures accumulated between −60 and −75 °C. The cirrus optical thickness (COT at 532 nm) of the ice clouds covered a wide range of values from < 0.03 (subvisible cirrus fraction, 25 % out of all cases) over 0.03–0.3 (visible thin cirrus, 40 %) to > 0.3 (opaque cirrus fraction, 35 %). In about 30 % out of all high altitude lidar observations, cirrus signatures were detected, much more than expected (10 %). This fact may be taken as a first hint that wildfire smoke was significantly involved in Arctic cirrus formation. The smoke particle surface area concentration around the tropopause was of the order of 5–15 µm<sup>2</sup> cm<sup>−3</sup> and indicated considerably enhanced levels of aerosol pollutio
{"title":"Impact of wildfire smoke on Arctic cirrus formation, part 1: analysis of MOSAiC 2019–2020 observations","authors":"Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, Ulla Wandinger","doi":"10.5194/egusphere-2024-2008","DOIUrl":"https://doi.org/10.5194/egusphere-2024-2008","url":null,"abstract":"<strong>Abstract.</strong> The number of wildfire smoke layers in the upper troposphere per fire season increased at mid and high northern latitudes during the last years. To consider smoke in weather and climate models appropriately, the influence of smoke on a variety of atmospheric processes needs to be explored in detail. In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. The complex study is based on aerosol and ice cloud observations in the central Arctic during the one-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. For almost a year (from the summer of 2019 to the spring of 2020), aged Siberian wildfire smoke polluted the tropopause region over the central Arctic and many cirrus systems developed in the polluted upper troposphere. Goal of the data analysis (part 1) is to provide observational evidence for a dominating impact of aged wildfire smoke (organic aerosol particles) on cirrus formation in the central Arctic (over the MOSAiC research icebreaker Polarstern) during the winter half year of 2019–2020. Aim of the simulations in part 2 is to gain a deeper and more detailed insight into the potential smoke impact on ice nucleation as a function of observed aerosol and meteorological conditions (temperature, relative humidity) and by considering realistic gravity wave characteristics (updraft speed, wave amplitude). Vertical movements of air parcels are essential to initiate cloud formation. The measurements presented in part 1 were conducted during the winter half year (October to March), aboard the ice breaker Polarstern. The research vessel Polarstern drifted with the pack ice in the central Arctic mainly at latitudes >85 °N during the winter half year. The cirrus statistics show typical properties of ice clouds of the synoptic cirrus category (top-down generation of cirrus structures). The ice clouds mostly started to evolve at heights close to the tropopause. Cirrus top temperatures accumulated between −60 and −75 °C. The cirrus optical thickness (COT at 532 nm) of the ice clouds covered a wide range of values from < 0.03 (subvisible cirrus fraction, 25 % out of all cases) over 0.03–0.3 (visible thin cirrus, 40 %) to > 0.3 (opaque cirrus fraction, 35 %). In about 30 % out of all high altitude lidar observations, cirrus signatures were detected, much more than expected (10 %). This fact may be taken as a first hint that wildfire smoke was significantly involved in Arctic cirrus formation. The smoke particle surface area concentration around the tropopause was of the order of 5–15 µm<sup>2</sup> cm<sup>−3</sup> and indicated considerably enhanced levels of aerosol pollutio","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"17 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-05DOI: 10.5194/acp-24-7609-2024
Oliver Schneising, Michael Buchwitz, Maximilian Reuter, Michael Weimer, Heinrich Bovensmann, John P. Burrows, Hartmut Bösch
Abstract. Global crude steel production is expected to continue to increase in the coming decades to meet the demands of the growing world population. Currently, the dominant steelmaking technology worldwide is the conventional highly CO2-intensive blast furnace–basic oxygen furnace production route (also known as the Linz–Donawitz process), which uses iron ore as raw material and coke as a reducing agent. As a result, large quantities of special gases that are rich in carbon monoxide (CO) are by-products of the various stages of the steelmaking process. Given the challenges associated with satellite-based estimates of carbon dioxide (CO2) emissions at the scale of emitting installations due to significant background levels, co-emitted CO may serve as a valuable indicator of the carbon footprint of steel plants. We show that regional CO release from steel production sites can be monitored from space using 5 years of measurements (2018–2022) from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite, benefiting from its relatively high spatial resolution and daily global coverage. We analyse all German steel plants with blast furnaces and basic oxygen furnaces and obtain associated CO emissions in the range of 50–400 kt yr−1 per site. A comparison with the respective CO2 emissions on the level of emitting installations available from emissions trading data of the European Union Emissions Trading System yields a linear relationship with a sector-specific CO/CO2 emission ratio for the analysed steelworks of 3.24 % [2.73–3.89; 1σ], suggesting the feasibility of using CO as a proxy for CO2 emissions from comparable steel production sites. An evaluation at other steel production sites indicates that the derived CO/CO2 emission ratio is also representative of other highly optimised state-of-the-art Linz–Donawitz steelworks outside Germany and that the emission ratio is potentially valuable for estimating sector-specific CO2 emissions from remotely sensed CO emissions, provided that the underlying CO emission estimate is not affected by other sources.
摘要未来几十年，全球粗钢产量预计将继续增加，以满足不断增长的世界人口的需求。目前，全球最主要的炼钢技术是传统的高炉--碱性氧气炉生产工艺（又称林茨-多纳维茨工艺），该工艺以铁矿石为原料，焦炭为还原剂，是一种高度二氧化碳密集型工艺。因此，炼钢过程的各个阶段都会产生大量富含一氧化碳（CO）的特殊气体副产品。由于大量的背景水平，基于卫星的二氧化碳（CO2）排放量估算在排放装置的规模上面临挑战，因此共同排放的 CO 可以作为衡量钢铁厂碳足迹的重要指标。我们利用哨兵-5 号前兆卫星上的 TROPOspheric Monitoring Instrument（TROPOMI）进行了为期 5 年（2018-2022 年）的测量，结果表明，利用其相对较高的空间分辨率和每日全球覆盖范围，可以从太空监测钢铁生产基地的区域性二氧化碳排放。我们对德国所有拥有高炉和氧气炉的钢铁厂进行了分析，获得了每个钢铁厂每年 50-400 kt-1 的相关二氧化碳排放量。根据欧盟排放交易系统的排放交易数据，我们将排放装置的二氧化碳排放量与相应的二氧化碳排放量进行了比较，结果发现，在所分析的钢铁厂中，特定行业的二氧化碳/一氧化碳排放比为 3.24 % [2.73-3.89; 1σ]，这表明使用二氧化碳作为可比钢铁生产基地二氧化碳排放量的替代物是可行的。对其他钢铁生产基地的评估表明，推导出的 CO/CO2 排放比也能代表德国以外其他高度优化的林茨-多纳维茨（Linz-Donawitz）先进钢铁厂，并且只要基本的 CO 排放估算不受其他来源的影响，该排放比对于从遥感 CO 排放中估算特定行业的 CO2 排放量具有潜在价值。
{"title":"Towards a sector-specific CO∕CO2 emission ratio: satellite-based observations of CO release from steel production in Germany","authors":"Oliver Schneising, Michael Buchwitz, Maximilian Reuter, Michael Weimer, Heinrich Bovensmann, John P. Burrows, Hartmut Bösch","doi":"10.5194/acp-24-7609-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7609-2024","url":null,"abstract":"Abstract. Global crude steel production is expected to continue to increase in the coming decades to meet the demands of the growing world population. Currently, the dominant steelmaking technology worldwide is the conventional highly CO2-intensive blast furnace–basic oxygen furnace production route (also known as the Linz–Donawitz process), which uses iron ore as raw material and coke as a reducing agent. As a result, large quantities of special gases that are rich in carbon monoxide (CO) are by-products of the various stages of the steelmaking process. Given the challenges associated with satellite-based estimates of carbon dioxide (CO2) emissions at the scale of emitting installations due to significant background levels, co-emitted CO may serve as a valuable indicator of the carbon footprint of steel plants. We show that regional CO release from steel production sites can be monitored from space using 5 years of measurements (2018–2022) from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite, benefiting from its relatively high spatial resolution and daily global coverage. We analyse all German steel plants with blast furnaces and basic oxygen furnaces and obtain associated CO emissions in the range of 50–400 kt yr−1 per site. A comparison with the respective CO2 emissions on the level of emitting installations available from emissions trading data of the European Union Emissions Trading System yields a linear relationship with a sector-specific CO/CO2 emission ratio for the analysed steelworks of 3.24 % [2.73–3.89; 1σ], suggesting the feasibility of using CO as a proxy for CO2 emissions from comparable steel production sites. An evaluation at other steel production sites indicates that the derived CO/CO2 emission ratio is also representative of other highly optimised state-of-the-art Linz–Donawitz steelworks outside Germany and that the emission ratio is potentially valuable for estimating sector-specific CO2 emissions from remotely sensed CO emissions, provided that the underlying CO emission estimate is not affected by other sources.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"31 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553347","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.5194/acp-24-7591-2024
Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, Stephen Donnelly
Abstract. Tropopause-overshooting convection in the midlatitudes provides a rapid transport pathway for air from the lower troposphere to reach the upper troposphere and lower stratosphere (UTLS) and can result in the formation of above-anvil cirrus plumes (AACPs) that significantly hydrate the stratosphere. Such UTLS composition changes alter the radiation budget and impact climate. Novel in situ observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are used in this study to examine UTLS impacts from AACP-generating overshooting convection. Namely, a research flight on 31 May 2022 sampled active convection over the state of Oklahoma for more than 3 h with the NASA ER-2 high-altitude research aircraft. An AACP was bisected during this flight, providing the first such extensive in situ sampling of this phenomenon. The convective observations reveal pronounced changes in air mass composition and stratospheric hydration up to altitudes of 2.3 km above the tropopause and concentrations more than double background levels. Unique dynamic and trace gas signatures were found within the AACP, including enhanced vertical mixing near the AACP edge and a positive correlation between water vapor and ozone. Moreover, the water vapor enhancement within the AACP was found to be limited to the saturation mixing ratio of the low temperature overshoot and AACP air. Comparison with all remaining DCOTSS flights demonstrates that the 31 May 2022 flight had some of the largest tropospheric tracer and water vapor perturbations in the stratosphere and within the AACP.
{"title":"Airborne observations of upper troposphere and lower stratosphere composition change in active convection producing above-anvil cirrus plumes","authors":"Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, Stephen Donnelly","doi":"10.5194/acp-24-7591-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7591-2024","url":null,"abstract":"Abstract. Tropopause-overshooting convection in the midlatitudes provides a rapid transport pathway for air from the lower troposphere to reach the upper troposphere and lower stratosphere (UTLS) and can result in the formation of above-anvil cirrus plumes (AACPs) that significantly hydrate the stratosphere. Such UTLS composition changes alter the radiation budget and impact climate. Novel in situ observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are used in this study to examine UTLS impacts from AACP-generating overshooting convection. Namely, a research flight on 31 May 2022 sampled active convection over the state of Oklahoma for more than 3 h with the NASA ER-2 high-altitude research aircraft. An AACP was bisected during this flight, providing the first such extensive in situ sampling of this phenomenon. The convective observations reveal pronounced changes in air mass composition and stratospheric hydration up to altitudes of 2.3 km above the tropopause and concentrations more than double background levels. Unique dynamic and trace gas signatures were found within the AACP, including enhanced vertical mixing near the AACP edge and a positive correlation between water vapor and ozone. Moreover, the water vapor enhancement within the AACP was found to be limited to the saturation mixing ratio of the low temperature overshoot and AACP air. Comparison with all remaining DCOTSS flights demonstrates that the 31 May 2022 flight had some of the largest tropospheric tracer and water vapor perturbations in the stratosphere and within the AACP.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"32 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.5194/egusphere-2024-1222
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, Igor Ezau
Abstract. Within the TURBAN project, a "Legerova campaign" focusing on air quality and meteorology in the traffic-loaded part of the Prague city (Czech Republic) was carried out from 30 May 2022 to 28 March 2023. The network comprised of 20 combined low-cost sensor (LCS) stations for NO2, O3, PM10 and PM2.5 concentrations, along with a mobile meteorological mast, a single-channel microwave radiometer and Doppler LIDAR for measurement of vertical temperature and wind profiles. Significant individual deviations of LCSs were detected during the 165 day initial field test of all units at the urban background Prague 4-Libuš reference station (coefficient of variation 17–28 %). Implementing the Multivariate Adaptive Regression Splines method for correction reduced the LCS inter-individual variability and improved correlation with reference monitors in all pollutants (R2 0.88–0.97). The LCSs' data drifts and ageing were checked by the double mass curve method for the entire measurement period. During the Legerova campaign, the highest NO2 concentrations were in traffic-loaded street canyons with continuous building blocks and several traffic lights. Aerosol pollution showed very little variation between the monitored streets. The highest PM10 and PM2.5 concentrations were recorded during temperature inversions and an episode involving pollution transported from a large forest fire in northern Czech Republic in July 2022. This report provides valuable data to support the validation of various predictive models dealing with complex urban environment, such as microscale LES model PALM tested in the TURBAN project.
{"title":"Measurement report: TURBAN observation campaign combining street-level low-cost air quality sensors and meteorological profile measurements in Prague","authors":"Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, Igor Ezau","doi":"10.5194/egusphere-2024-1222","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1222","url":null,"abstract":"<strong>Abstract.</strong> Within the TURBAN project, a \"Legerova campaign\" focusing on air quality and meteorology in the traffic-loaded part of the Prague city (Czech Republic) was carried out from 30 May 2022 to 28 March 2023. The network comprised of 20 combined low-cost sensor (LCS) stations for NO<sub>2</sub>, O<sub>3</sub>, PM<sub>10</sub> and PM<sub>2.5 </sub>concentrations, along with a mobile meteorological mast, a single-channel microwave radiometer and Doppler LIDAR for measurement of vertical temperature and wind profiles. Significant individual deviations of LCSs were detected during the 165 day initial field test of all units at the urban background Prague 4-Libuš reference station (coefficient of variation 17–28 %). Implementing the Multivariate Adaptive Regression Splines method for correction reduced the LCS inter-individual variability and improved correlation with reference monitors in all pollutants (R<sup>2</sup> 0.88–0.97). The LCSs' data drifts and ageing were checked by the double mass curve method for the entire measurement period. During the Legerova campaign, the highest NO<sub>2</sub> concentrations were in traffic-loaded street canyons with continuous building blocks and several traffic lights. Aerosol pollution showed very little variation between the monitored streets. The highest PM<sub>10</sub> and PM<sub>2.5</sub> concentrations were recorded during temperature inversions and an episode involving pollution transported from a large forest fire in northern Czech Republic in July 2022. This report provides valuable data to support the validation of various predictive models dealing with complex urban environment, such as microscale LES model PALM tested in the TURBAN project.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"67 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abstract. The supercooled liquid fraction (SLF) in mixed-phase clouds (MPCs) is an essential variable of cloud microphysical processes and climate sensitivity. However, the SLF is currently calculated in spaceborne remote sensing only as the cloud phase–frequency ratio of adjacent pixels, which results in a loss of the original resolution in observations of cloud liquid or ice content within MPCs. Here, we present a novel method for retrieving the SLF in MPCs based on the differences in radiative properties of supercooled liquid droplets and ice particles at visible (VIS) and shortwave infrared (SWI) channels of the geostationary Himawari-8. Liquid and ice water paths are inferred by assuming that clouds are composed of only liquid or ice, with the real cloud water path (CWP) expressed as a combination of these two water paths (SLF and 1-SLF as coefficients), and the SLF is determined by referring to the CWP from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). The statistically relatively small cloud phase spatial inhomogeneity at a Himawari-8 pixel level indicates an optimal scene for cloud retrieval. The SLF results are comparable to global SLF distributions observed by active instruments, particularly for single-layered cloud systems. While accessing the method's feasibility, SLF averages are estimated between 74 % and 78 % in Southern Ocean (SO) stratocumulus across seasons, contrasting with a range of 29 % to 32 % in northeastern Asia. The former exhibits a minimum SLF around midday in summer and a maximum in winter, while the latter trend differs. This novel algorithm will be valuable for research to track the evolution of MPCs and constrain the related climate impact.
{"title":"Technical note: Retrieval of the supercooled liquid fraction in mixed-phase clouds from Himawari-8 observations","authors":"Ziming Wang, Husi Letu, Huazhe Shang, Luca Bugliaro","doi":"10.5194/acp-24-7559-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7559-2024","url":null,"abstract":"Abstract. The supercooled liquid fraction (SLF) in mixed-phase clouds (MPCs) is an essential variable of cloud microphysical processes and climate sensitivity. However, the SLF is currently calculated in spaceborne remote sensing only as the cloud phase–frequency ratio of adjacent pixels, which results in a loss of the original resolution in observations of cloud liquid or ice content within MPCs. Here, we present a novel method for retrieving the SLF in MPCs based on the differences in radiative properties of supercooled liquid droplets and ice particles at visible (VIS) and shortwave infrared (SWI) channels of the geostationary Himawari-8. Liquid and ice water paths are inferred by assuming that clouds are composed of only liquid or ice, with the real cloud water path (CWP) expressed as a combination of these two water paths (SLF and 1-SLF as coefficients), and the SLF is determined by referring to the CWP from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). The statistically relatively small cloud phase spatial inhomogeneity at a Himawari-8 pixel level indicates an optimal scene for cloud retrieval. The SLF results are comparable to global SLF distributions observed by active instruments, particularly for single-layered cloud systems. While accessing the method's feasibility, SLF averages are estimated between 74 % and 78 % in Southern Ocean (SO) stratocumulus across seasons, contrasting with a range of 29 % to 32 % in northeastern Asia. The former exhibits a minimum SLF around midday in summer and a maximum in winter, while the latter trend differs. This novel algorithm will be valuable for research to track the evolution of MPCs and constrain the related climate impact.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"16 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.5194/egusphere-2024-1633
Corina Wieber, Lasse Z. Jensen, Leendert Vergeynst, Lorenz Maire, Thomas Juul-Pedersen, Kai Finster, Tina Šantl-Temkiv
Abstract. The accelerated warming of the Arctic manifests in sea ice loss and melting glaciers, significantly altering the dynamics of marine biota. This disruption in marine ecosystems can lead to the emission of biological ice nucleating particles (INPs) from the ocean into the atmosphere. Once airborne, these INPs induce cloud droplet freezing, thereby affecting cloud lifetime and radiative properties. Despite the potential atmospheric impacts of marine INPs, their properties and sources remain poorly understood. Analysing sea bulk water and the sea surface microlayer in two southwest Greenlandic fjords, collected between June and September 2018, and investigating the INPs along with the microbial communities, we could demonstrate a clear seasonal variation in the number of INPs and a notable input from terrestrial runoff. We found the highest INP concentration in June during the late stage of the phytoplankton bloom and active melting processes causing enhanced terrestrial runoff. These highly active INPs were smaller in size and less heat-sensitive than those found later in the summer and those previously identified in Arctic marine systems. A negative correlation between salinity and INP abundance suggests freshwater input as sources of INPs. Stable oxygen isotope analysis, along with the strong correlation between INPs and the presence of the bacterium Aquaspirillum arcticum, highlighted meteoric water as the primary origin of the freshwater influx, suggesting that the notably active INPs originate from terrestrial sources such as glacial and soil runoff.
{"title":"Terrestrial runoff is an important source of biological INPs in Arctic marine systems","authors":"Corina Wieber, Lasse Z. Jensen, Leendert Vergeynst, Lorenz Maire, Thomas Juul-Pedersen, Kai Finster, Tina Šantl-Temkiv","doi":"10.5194/egusphere-2024-1633","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1633","url":null,"abstract":"<strong>Abstract.</strong> The accelerated warming of the Arctic manifests in sea ice loss and melting glaciers, significantly altering the dynamics of marine biota. This disruption in marine ecosystems can lead to the emission of biological ice nucleating particles (INPs) from the ocean into the atmosphere. Once airborne, these INPs induce cloud droplet freezing, thereby affecting cloud lifetime and radiative properties. Despite the potential atmospheric impacts of marine INPs, their properties and sources remain poorly understood. Analysing sea bulk water and the sea surface microlayer in two southwest Greenlandic fjords, collected between June and September 2018, and investigating the INPs along with the microbial communities, we could demonstrate a clear seasonal variation in the number of INPs and a notable input from terrestrial runoff. We found the highest INP concentration in June during the late stage of the phytoplankton bloom and active melting processes causing enhanced terrestrial runoff. These highly active INPs were smaller in size and less heat-sensitive than those found later in the summer and those previously identified in Arctic marine systems. A negative correlation between salinity and INP abundance suggests freshwater input as sources of INPs. Stable oxygen isotope analysis, along with the strong correlation between INPs and the presence of the bacterium <em>Aquaspirillum arcticum</em>, highlighted meteoric water as the primary origin of the freshwater influx, suggesting that the notably active INPs originate from terrestrial sources such as glacial and soil runoff.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"39 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abstract. Humic-like substances (HULIS) are complex macromolecules in water-soluble organic compounds (WSOCs) containing multiple functional groups, and transition metal ions (TMs) are ubiquitous in atmospheric particles. In this study, potential physical and chemical interactions between HULIS and four TM species, including Cu2+, Mn2+, Ni2+, and Zn2+, were analyzed by optical method under acidic, weakly acidic, and neutral conditions. The results showed that Cu2+, Mn2+, and Zn2+ only slightly enhanced mass absorption efficiency (MAE365) of HULIS in winter and had indiscernible effects on the absorption Ångström exponent (AAE) of HULIS in both seasons under all acidity conditions. All four TMs had fluorescence quenching effects on winter HULIS, and only Cu2+ had similar effects on summer HULIS, with the highest quenching coefficients found under weakly acidic conditions in both seasons. The 1H-nuclear magnetic resonance (1H-NMR) and Fourier-transform infrared (FTIR) spectra revealed that Cu2+ mainly bound with aromatic species and tightened the molecule structures of HULIS. The parallel factor analysis (PARAFAC) results extracted four components of HULIS, including low-oxidized humic-like substances (C1), N-containing compounds (C2), highly oxidized humic-like substances (C3), and the mixing residuals (C4), from the fluorescence spectra in both winter and summer. The spectral characteristic of HULIS with Cu2+ additions under three acidity conditions indicated that electron-donating groups of HULIS mainly corresponded to C1 and C3, with Cu2+ binding with HULIS by replacing protons, while electron-withdrawing groups of HULIS could correspond to C2, with its connection with Cu2+ through electrostatic adsorption or colliding-induced energy transfer.
{"title":"Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China","authors":"Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, Xinming Wang","doi":"10.5194/acp-24-7575-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7575-2024","url":null,"abstract":"Abstract. Humic-like substances (HULIS) are complex macromolecules in water-soluble organic compounds (WSOCs) containing multiple functional groups, and transition metal ions (TMs) are ubiquitous in atmospheric particles. In this study, potential physical and chemical interactions between HULIS and four TM species, including Cu2+, Mn2+, Ni2+, and Zn2+, were analyzed by optical method under acidic, weakly acidic, and neutral conditions. The results showed that Cu2+, Mn2+, and Zn2+ only slightly enhanced mass absorption efficiency (MAE365) of HULIS in winter and had indiscernible effects on the absorption Ångström exponent (AAE) of HULIS in both seasons under all acidity conditions. All four TMs had fluorescence quenching effects on winter HULIS, and only Cu2+ had similar effects on summer HULIS, with the highest quenching coefficients found under weakly acidic conditions in both seasons. The 1H-nuclear magnetic resonance (1H-NMR) and Fourier-transform infrared (FTIR) spectra revealed that Cu2+ mainly bound with aromatic species and tightened the molecule structures of HULIS. The parallel factor analysis (PARAFAC) results extracted four components of HULIS, including low-oxidized humic-like substances (C1), N-containing compounds (C2), highly oxidized humic-like substances (C3), and the mixing residuals (C4), from the fluorescence spectra in both winter and summer. The spectral characteristic of HULIS with Cu2+ additions under three acidity conditions indicated that electron-donating groups of HULIS mainly corresponded to C1 and C3, with Cu2+ binding with HULIS by replacing protons, while electron-withdrawing groups of HULIS could correspond to C2, with its connection with Cu2+ through electrostatic adsorption or colliding-induced energy transfer.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"28 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546210","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.5194/egusphere-2024-1948
Mashiat Hossain, Rebecca M. Garland, Hannah M. Horowitz
Abstract. The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between −3.5 % (CLARIFY) and −7.5 % (ORACLES). At these altitudes, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during high DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting their overall importance. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations to better predict aerosol-cloud interactions and reduce uncertainties in aerosol radiative forcing over the southeast Atlantic.
{"title":"Quantifying the Impacts of Marine Aerosols over the Southeast Atlantic Ocean using a chemical transport model: Implications for aerosol-cloud interactions","authors":"Mashiat Hossain, Rebecca M. Garland, Hannah M. Horowitz","doi":"10.5194/egusphere-2024-1948","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1948","url":null,"abstract":"<strong>Abstract.</strong> The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between −3.5 % (CLARIFY) and −7.5 % (ORACLES). At these altitudes, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during high DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting their overall importance. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations to better predict aerosol-cloud interactions and reduce uncertainties in aerosol radiative forcing over the southeast Atlantic.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"39 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141546214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-03DOI: 10.5194/acp-24-7535-2024
Sandra Graßl, Christoph Ritter, Ines Tritscher, Bärbel Vogel
Abstract. The Asian summer monsoon has a strong convectional component with which aerosols are able to be lifted up into the lower stratosphere. Due to usually long lifetimes and long-range transport aerosols remain there much longer than in the troposphere and are also able to be advected around the globe. Our aim of this study is a synergy between simulations by Chemical Lagrangian Model of the Stratosphere (CLaMS) and KARL (Koldewey Aerosol Raman Lidar) at AWIPEV, Ny-Ålesund in the Arctic, by comparing CLaMS results with exemplary days of lidar measurements as well as analyzing the stratospheric aerosol background. We use global three-dimensional Lagrangian transport simulations including surface origin tracers as well as back trajectories to identify source regions of the aerosol particles measured over Ny-Ålesund. We analyzed lidar data for the year 2021 and found the stratosphere generally clear, without obvious aerosol layers from volcanic eruptions or biomass burnings. Still an obvious annual cycle of the backscatter coefficient with higher values in late summer to autumn and lower values in late winter has been found. Results from CLaMS model simulations indicate that from late summer to early autumn filaments with high fractions of air which originate in South Asia – one of the most polluted regions in the world – reach the Arctic at altitudes between 360 and 380 K potential temperature. We found a coinciding measurement between the overpass of such a filament and lidar observations, and we estimated that backscatter and depolarization increased by roughly 15 % during this event compared to the background aerosol concentration. Hence we demonstrate that the Asian summer monsoon is a weak but measurable source for Arctic stratospheric aerosol in late summer to early autumn.
{"title":"Does the Asian summer monsoon play a role in the stratospheric aerosol budget of the Arctic?","authors":"Sandra Graßl, Christoph Ritter, Ines Tritscher, Bärbel Vogel","doi":"10.5194/acp-24-7535-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7535-2024","url":null,"abstract":"Abstract. The Asian summer monsoon has a strong convectional component with which aerosols are able to be lifted up into the lower stratosphere. Due to usually long lifetimes and long-range transport aerosols remain there much longer than in the troposphere and are also able to be advected around the globe. Our aim of this study is a synergy between simulations by Chemical Lagrangian Model of the Stratosphere (CLaMS) and KARL (Koldewey Aerosol Raman Lidar) at AWIPEV, Ny-Ålesund in the Arctic, by comparing CLaMS results with exemplary days of lidar measurements as well as analyzing the stratospheric aerosol background. We use global three-dimensional Lagrangian transport simulations including surface origin tracers as well as back trajectories to identify source regions of the aerosol particles measured over Ny-Ålesund. We analyzed lidar data for the year 2021 and found the stratosphere generally clear, without obvious aerosol layers from volcanic eruptions or biomass burnings. Still an obvious annual cycle of the backscatter coefficient with higher values in late summer to autumn and lower values in late winter has been found. Results from CLaMS model simulations indicate that from late summer to early autumn filaments with high fractions of air which originate in South Asia – one of the most polluted regions in the world – reach the Arctic at altitudes between 360 and 380 K potential temperature. We found a coinciding measurement between the overpass of such a filament and lidar observations, and we estimated that backscatter and depolarization increased by roughly 15 % during this event compared to the background aerosol concentration. Hence we demonstrate that the Asian summer monsoon is a weak but measurable source for Arctic stratospheric aerosol in late summer to early autumn.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"6 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495547","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-03DOI: 10.5194/acp-24-7499-2024
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, Stephan Borrmann
Abstract. The chemical composition of the upper troposphere/lower stratosphere region (UTLS) is influenced by horizontal transport of air masses, vertical transport within convective systems and warm conveyor belts, rapid turbulent mixing, as well as photochemical production or loss of species. This results in the formation of the extratropical transition layer (ExTL), which is defined by the vertical structure of CO and has been studied until now mostly by means of trace gas correlations. Here, we extend the analysis to include aerosol particles and derive the sulfate–ozone correlation in central Europe from aircraft in situ measurements during the CAFE-EU (Chemistry of the Atmosphere Field Experiment over Europe)/BLUESKY mission. The mission probed the UTLS during the COVID-19 period with significantly reduced anthropogenic emissions. We operated a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) to measure the chemical composition of non-refractory aerosol particles in the size range from about 40 to 800 nm. In our study, we find a correlation between the sulfate mass concentration and O3 in the lower stratosphere. The correlation exhibits some variability exceeding the mean sulfate–ozone correlation over the measurement period. Especially during one flight, we observed enhanced mixing ratios of sulfate aerosol in the lowermost stratosphere, where the analysis of trace gases shows tropospheric influence. However, back trajectories indicate that no recent mixing with tropospheric air occurred within the last 10 d. Therefore, we analyzed volcanic eruption databases and satellite SO2 retrievals from the TROPOspheric Monitoring Instrument (TROPOMI) for possible volcanic plumes and eruptions to explain the high amounts of sulfur compounds in the UTLS. From these analyses and the combination of precursor and particle measurements, we conclude that gas-to-particle conversion of volcanic SO2 leads to the observed enhanced sulfate aerosol mixing ratios.
{"title":"The influence of extratropical cross-tropopause mixing on the correlation between ozone and sulfate aerosol in the lowermost stratosphere","authors":"Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, Stephan Borrmann","doi":"10.5194/acp-24-7499-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7499-2024","url":null,"abstract":"Abstract. The chemical composition of the upper troposphere/lower stratosphere region (UTLS) is influenced by horizontal transport of air masses, vertical transport within convective systems and warm conveyor belts, rapid turbulent mixing, as well as photochemical production or loss of species. This results in the formation of the extratropical transition layer (ExTL), which is defined by the vertical structure of CO and has been studied until now mostly by means of trace gas correlations. Here, we extend the analysis to include aerosol particles and derive the sulfate–ozone correlation in central Europe from aircraft in situ measurements during the CAFE-EU (Chemistry of the Atmosphere Field Experiment over Europe)/BLUESKY mission. The mission probed the UTLS during the COVID-19 period with significantly reduced anthropogenic emissions. We operated a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) to measure the chemical composition of non-refractory aerosol particles in the size range from about 40 to 800 nm. In our study, we find a correlation between the sulfate mass concentration and O3 in the lower stratosphere. The correlation exhibits some variability exceeding the mean sulfate–ozone correlation over the measurement period. Especially during one flight, we observed enhanced mixing ratios of sulfate aerosol in the lowermost stratosphere, where the analysis of trace gases shows tropospheric influence. However, back trajectories indicate that no recent mixing with tropospheric air occurred within the last 10 d. Therefore, we analyzed volcanic eruption databases and satellite SO2 retrievals from the TROPOspheric Monitoring Instrument (TROPOMI) for possible volcanic plumes and eruptions to explain the high amounts of sulfur compounds in the UTLS. From these analyses and the combination of precursor and particle measurements, we conclude that gas-to-particle conversion of volcanic SO2 leads to the observed enhanced sulfate aerosol mixing ratios.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"50 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495801","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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