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The Impact of Aerosol on Cloud Water: A Heuristic Perspective 气溶胶对云水的影响:启发式视角
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-21 DOI: 10.5194/egusphere-2024-1725
Fabian Hoffmann, Franziska Glassmeier, Graham Feingold
Abstract. Aerosol-cloud interactions modulate the role of clouds in Earth's climate. We derive, evaluate, and apply a simple model to understand aerosol-mediated cloud water adjustments in stratocumulus based on only two prognostic equations for the integrated cloud water L and droplet number concentration N. The model is solved numerically and analytically, and agrees well with documented large-eddy simulation data and satellite retrievals. A tight relationship between adjustments at low and high N is found, revealing the influence of non-precipitation processes (primarily entrainment) on adjustments in precipitating clouds. Furthermore, it is shown that adjustments in non-precipitating clouds tend to be positively biased by external L or N perturbations, while adjustments in precipitating clouds are barely susceptible. By deliberately reducing the complexity of the underlying system, this study constitutes a way forward to facilitate process-level understanding of cloud water adjustments.
摘要气溶胶与云的相互作用调节着云在地球气候中的作用。我们推导、评估并应用了一个简单的模型来理解气溶胶介导的层积云云水调整,该模型仅基于综合云水 L 和水滴数浓度 N 的两个预报方程。研究发现,低 N 值和高 N 值的调整之间关系密切,揭示了非沉降过程(主要是夹带)对降水云调整的影响。此外,研究还表明,非沉降云的调整往往会受到外部L或N扰动的正偏影响,而沉降云的调整则几乎不受影响。通过有意降低基本系统的复杂性,本研究为促进对云水调节过程的理解提供了一条前进的道路。
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引用次数: 0
AERO-MAP: A data compilation and modelling approach to understand spatial variability in fine and coarse mode aerosol composition AERO-MAP:数据汇编和建模方法,用于了解细粒和粗粒模式气溶胶成分的空间变异性
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-21 DOI: 10.5194/egusphere-2024-1617
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, Xi Zhao
Abstract. Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, change the surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. High particulate matter concentrations at the surface represent an important public health hazard. There are substantial datasets describing aerosol particles in the literature or in public health databases, but they have not been compiled for easy use by the climate and air quality modelling community. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output. Overall, most of the planet or even the land fraction does not have sufficient observations of surface concentrations, and especially particle composition to understand the current distribution of particles. Most climate models exclude 10–30 % of the aerosol particles in both PM2.5 and PM10 size fractions across large swaths of the globe in their current configurations, with ammonium nitrate and agricultural dust aerosol being the most important omitted aerosol types.
摘要气溶胶粒子是地球系统的重要组成部分,但其浓度在空间和时间上都是不均匀的,在大小和成分上也是多变的。颗粒物可与进入的太阳辐射和流出的长波辐射相互作用,改变云的性质,影响光化学,影响地表空气质量,改变冰雪的表面反照率,并调节陆地和海洋对二氧化碳的吸收。地表颗粒物浓度过高对公众健康造成严重危害。文献或公共卫生数据库中有大量描述气溶胶粒子的数据集,但这些数据集尚未汇编成册,以方便气候和空气质量建模界使用。在此,我们对 PM2.5 和 PM10 气溶胶观测数据进行了新的汇编,重点关注不同观测站的空间变化,包括成分,并展示了一种将数据集与模型输出进行比较的方法。总体而言,地球上大部分地区甚至陆地部分都没有足够的表面浓度观测数据,尤其是颗粒物成分观测数据,因此无法了解颗粒物目前的分布情况。大多数气候模式在其当前配置中排除了全球大部分地区 PM2.5 和 PM10 尺寸分数中 10-30% 的气溶胶粒子,硝酸铵和农业尘埃气溶胶是被忽略的最重要的气溶胶类型。
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引用次数: 0
Microphysical characteristics of precipitation within convective overshooting over East China observed by GPM DPR and ERA5 GPM DPR 和 ERA5 观测到的华东上空对流凌空降水的微物理特征
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-21 DOI: 10.5194/acp-24-7123-2024
Nan Sun, Gaopeng Lu, Yunfei Fu
Abstract. We examine the geographical distribution and microphysical three-dimensional structure of convective overshooting over East China by matching the Global Precipitation Measurement Dual-frequency Precipitation Radar (GPM DPR) instrument with the European Centre for Medium-Range Weather Forecasts Fifth-Generation Reanalysis (ERA5). Convective overshooting mainly occurs over Northeast China (NC) and northern Middle and East China (MEC), and its frequency varies from 4×10-4 to 5.4×10-3. Radar reflectivity of convective overshooting over NC accounts for a higher proportion below the freezing level, while MEC and South China (SC) account for a higher proportion above the freezing level, indicating stronger upward motion and more ice crystal particles. The microphysical processes within convective overshooting are unique, leading to various properties of the droplets in precipitation. Droplets of convective overshooting are large but sparse, with an effective droplet radius of nearly 2.5 mm below 10 km, which is about twice that of non-overshooting precipitation. The findings of this study may have important implications for the microphysical evolution associated with convective overshooting and provide more accurate precipitation microphysical parameters as input for model simulations.
摘要通过全球降水测量双频降水雷达(GPM DPR)与欧洲中期天气预报中心第五代再分析(ERA5)的匹配,研究了华东地区对流过冲的地理分布和微物理三维结构。对流过冲主要发生在中国东北(NC)和中国中东部北部(MEC),其频率在 4×10-4 到 5.4×10-3 之间。东北地区对流凌空的雷达反射率在冰面以下的比例较高,而华中和华南地区对流凌空的雷达反射率在冰面以上的比例较高,这表明对流凌空的上升运动较强,冰晶颗粒较多。对流凌空的微物理过程是独特的,导致降水中的水滴具有不同的性质。对流过冲的水滴大而稀疏,10 公里以下的有效水滴半径接近 2.5 毫米,约为非过冲降水的两倍。这项研究的结果可能对与对流过冲相关的微物理演变产生重要影响,并为模式模拟提供更准确的降水微物理参数输入。
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引用次数: 0
On the dynamics of ozone depletion events at Villum Research Station in the High Arctic 北极高纬度地区 Villum 研究站臭氧消耗事件的动态变化
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-21 DOI: 10.5194/egusphere-2024-1676
Jakob Boyd Pernov, Jens Liengaard Hjorth, Lise Lotte Sørensen, Henrik Skov
Abstract. Ozone depletion events (ODEs) occur every spring in the Arctic and have implications for the atmospheric oxidizing capacity, radiative balance, and mercury oxidation. Here we comprehensively analyze ozone, ODEs, and their connection to meteorological and air mass history variables through statistical analyses, back-trajectories, and machine learning (ML) from observations at Villum Research Station, Station Nord, Greenland. We show that the ODE frequency and duration peak in May followed by April and March, which is likely related to air masses spending more time over sea ice and increases in radiation from March to May. Back-trajectories indicate that, as spring progresses, ODE air masses spend more time within the mixed layer and the geographic origins move closer to Villum. ODE frequency and duration are increasing during May (low confidence) and April (high confidence), respectively. Our analysis revealed that ODEs are favorable under sunny, calm conditions with air masses arriving from northerly wind directions with sea ice contact. The ML model was able to reproduce the ODE occurrence and illuminated that radiation, time over sea ice, and temperature were the most important variables for modeling ODEs during March, April, and May, respectively. Several variables displayed threshold ranges for contributing to the positive prediction of ODEs vs Non-ODEs, notably temperature, radiation, wind direction, time spent over sea ice, and snow. Our ML methodology provides a framework for investigating and comparing the environmental drivers of ODEs between different Arctic sites and can be applied to other atmospheric phenomena (e.g., atmospheric mercury depletion events).
摘要北极地区每年春季都会发生臭氧耗损事件(ODEs),对大气氧化能力、辐射平衡和汞氧化都有影响。在此,我们通过统计分析、回溯轨迹和机器学习(ML),利用格陵兰岛北站 Villum 研究站的观测数据,全面分析了臭氧、ODEs 及其与气象和气团历史变量的联系。我们发现,ODE 的频率和持续时间在 5 月达到峰值,随后是 4 月和 3 月,这可能与气团在海冰上空停留时间更长以及 3 月至 5 月辐射增加有关。回溯轨迹表明,随着春季的到来,ODE 气团在混合层中停留的时间越来越长,地理起源也越来越靠近 Villum。在五月(低置信度)和四月(高置信度)期间,ODE 的频率和持续时间分别在增加。我们的分析表明,在天气晴朗、风平浪静的条件下,气团从与海冰接触的偏北风向到达,有利于 ODE。ML 模式能够再现 ODE 的发生,并表明辐射、海冰上空时间和温度分别是 3 月、4 月和 5 月 ODE 模拟的最重要变量。有几个变量显示了对 ODEs 与非 ODEs 正预测的阈值范围,特别是温度、辐射、风向、海冰上空时间和积雪。我们的 ML 方法为研究和比较不同北极地点的 ODEs 环境驱动因素提供了一个框架,并可应用于其他大气现象(如大气汞耗竭事件)。
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引用次数: 0
Emission characteristics of reactive organic gases (ROGs) from industrial volatile chemical products (VCPs) in the Pearl River Delta (PRD), China 中国珠江三角洲(PRD)工业挥发性化学产品(VCP)产生的活性有机气体(ROGs)的排放特征
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-20 DOI: 10.5194/acp-24-7101-2024
Sihang Wang, Bin Yuan, Xianjun He, Ru Cui, Xin Song, Yubin Chen, Caihong Wu, Chaomin Wang, Yibo Huangfu, Xiao-Bing Li, Boguang Wang, Min Shao
Abstract. Volatile chemical products (VCPs) have become an important source of reactive organic gases (ROGs) in urban areas worldwide. Industrial activities can also utilize a large number of VCPs and emit many organic gases into the atmosphere. Due to multiple sampling and measurement challenges, only a subset of ROG species is usually measured for many industrial VCP sources. This study aims to investigate the emissions of ROGs from five industrial VCP sources in the Pearl River Delta (PRD) region of China, including the shoemaking, plastic surface coating, furniture coating, printing, and ship coating industries. A more comprehensive speciation of ROG emissions from these industrial VCP sources was developed by the combination of proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) and the gas chromatography–mass spectrometer/flame ionization detector (GC–MS/FID). Our study identified oxygenated ROG species (OVOCs) as representative ROGs emitted from these sources, which are highly related to specific chemicals used during industrial activities. Moreover, mass spectra similarity analysis revealed significant dissimilarities among the ROG emissions from industrial activities, indicating substantial variations between different industrial VCP sources. Except for the ship coating industry utilizing solvent-borne coatings, the proportions of OVOCs range from 67 % to 96 % in total ROG emissions and 72 % to 97 % in total OH reactivity (OHR) for different industrial sources, while the corresponding contributions of OVOCs in the ship coating industry are only 16 ± 3.5 % and 15 ± 3.6 %. The industrial VCP sources associated with solvent-borne coatings exhibited a higher ozone formation potential (OFP), reaching as high as 5.5 and 2.7 g O3 g−1 ROGs for the ship coating and furniture coating industries, primarily due to contributions from aromatics. We find that a few species can contribute the majority of the ROG emissions and also their OHR and OFP from various industrial VCP sources. Our results suggest that ROG treatment devices may have limited effectiveness for all ROGs, with treatment efficiencies ranging from −12 % to 68 %. Furthermore, we found that ambient measurements in industrial areas have been significantly impacted by industrial VCP sources, and ROG pairs (e.g., methyl ethyl ketone (MEK) / C8 aromatics ratio) can be utilized as reliable evidence by using high-time-resolution ROG measurements from PTR-ToF-MS. Our study demonstrated the importance of measuring a large number of ROGs using PTR-ToF-MS for characterizing ROG emissions from industrial VCP sources.
摘要挥发性化学产品(VCPs)已成为全球城市地区活性有机气体(ROGs)的重要来源。工业活动也会利用大量的挥发性化学产品,并向大气排放多种有机气体。由于取样和测量方面的多重挑战,通常只能测量许多工业 VCP 来源的一部分 ROG 种类。本研究旨在调查中国珠江三角洲(PRD)地区五个工业 VCP 源的 ROG 排放情况,包括制鞋、塑料表面涂层、家具涂层、印刷和船舶涂层行业。通过质子转移反应飞行时间质谱仪(PTR-ToF-MS)和气相色谱-质谱联用仪/火焰离子化检测器(GC-MS/FID)的联用,对这些工业 VCP 源排放的 ROG 进行了更全面的标样。我们的研究发现,含氧 ROG 物种(OVOCs)是这些来源排放的代表性 ROGs,它们与工业活动中使用的特定化学品高度相关。此外,质谱相似性分析表明,工业活动排放的 ROG 之间存在显著差异,这表明不同工业 VCP 来源之间存在很大差异。除使用溶剂型涂料的船舶涂装业外,不同工业源的 OVOC 在 ROG 排放总量中所占比例为 67% 至 96%,在 OH 反应活性总量中所占比例为 72% 至 97%,而船舶涂装业中 OVOC 的相应比例仅为 16 ± 3.5% 和 15 ± 3.6%。与溶剂型涂料相关的工业 VCP 源表现出更高的臭氧形成潜势 (OFP),船舶涂料和家具涂料行业的 ROGs 分别高达 5.5 和 2.7 g O3 g-1,这主要是由于芳烃的贡献。我们发现,在各种工业 VCP 源的 ROG 排放中,少数几种物质可能占绝大部分,它们的 OHR 和 OFP 也占绝大部分。我们的研究结果表明,ROG 处理设备对所有 ROG 的处理效果可能有限,处理效率从 -12 % 到 68 % 不等。此外,我们还发现,工业区的环境测量受到工业 VCP 源的严重影响,而 ROG 对(例如,甲乙酮 (MEK) / C8 芳烃比率)可通过使用 PTR-ToF-MS 的高时间分辨率 ROG 测量值作为可靠证据。我们的研究表明,使用 PTR-ToF-MS 测量大量 ROG 对描述工业 VCP 源的 ROG 排放特征非常重要。
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引用次数: 0
Deciphering anthropogenic and biogenic contributions to selected non-methane volatile organic compound emissions in an urban area 解密城市地区某些非甲烷挥发性有机化合物排放的人为和生物贡献
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-20 DOI: 10.5194/acp-24-7063-2024
Arianna Peron, Martin Graus, Marcus Striednig, Christian Lamprecht, Georg Wohlfahrt, Thomas Karl
Abstract. The anthropogenic and biogenic contributions of isoprene, monoterpenes, sesquiterpenes and methanol in an urban area were estimated based on direct eddy covariance flux observations during four campaigns between 2018 and 2021. While these compounds are typically thought to be dominated by biogenic sources on regional and global scales, the role of potentially significant anthropogenic emissions in urban areas has been recently debated. Typical fluxes of isoprene, monoterpenes and sesquiterpenes were on the order of 0.07 ± 0.02, 0.09 and 0.003 nmol m−2 s−1 during spring. During summer, emission fluxes of isoprene, monoterpenes and sesquiterpenes were higher on the order of 0.85 ± 0.09, 0.11 and 0.004 nmol m−2 s−1. It was found that the contribution of the anthropogenic part is strongly seasonally dependent. For isoprene, the anthropogenic fraction can be as high as 64 % in spring but is typically very low < 18 % during the summer season. For monoterpenes, the anthropogenic fraction was estimated to be between 43 % in spring and less than 20 % in summer. With values of 2.8 nmol m−2 s−1 in spring and 3.2 nmol m−2 s−1 in summer, methanol did not exhibit a significant seasonal variation of observed surface fluxes. However, there was a difference in emissions between weekdays and weekends (about 2.3 times higher on weekdays in spring). This suggests that methanol emissions are likely influenced by anthropogenic activities during all seasons.
摘要。根据2018年至2021年期间四次活动的直接涡度协方差通量观测结果,估算了城市地区异戊二烯、单萜烯、倍半萜烯和甲醇的人为和生物贡献。虽然这些化合物通常被认为在区域和全球范围内以生物源为主,但城市地区潜在的大量人为排放所起的作用最近引起了争论。在春季,异戊二烯、单萜烯和倍半萜烯的典型通量依次为 0.07 ± 0.02、0.09 和 0.003 nmol m-2 s-1。在夏季,异戊二烯、单萜烯和倍半萜烯的排放通量较高,依次为 0.85 ± 0.09、0.11 和 0.004 nmol m-2 s-1。研究发现,人为部分的贡献与季节密切相关。异戊二烯的人为部分在春季可高达 64%,但在夏季通常很低,< 18%。据估计,单萜烯的人为部分在春季为 43%,而在夏季则低于 20%。甲醇的观测表面通量在春季为 2.8 nmol m-2 s-1,夏季为 3.2 nmol m-2 s-1,没有明显的季节性变化。不过,平日和周末的甲醇排放量存在差异(春季平日的甲醇排放量约为周末的 2.3 倍)。这表明,甲醇的排放在所有季节都可能受到人为活动的影响。
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引用次数: 0
In situ measurement of organic aerosol molecular markers in urban Hong Kong during a summer period: temporal variations and source apportionment 香港市区夏季有机气溶胶分子标记原位测量:时间变化和来源分配
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-20 DOI: 10.5194/acp-24-7085-2024
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, Hai Guo
Abstract. Organic aerosol (OA) is a significant constituent of urban particulate matter (PM), and molecular markers therein provide information on the sources and formation mechanisms. With the in situ measurement of over 70 OA molecular markers in a summer month at a bihourly resolution, this study focused on the temporal variations in representative markers and dynamic source contributions to OA at an urban site in Hong Kong SAR (HK). The levels of secondary OA (SOA) markers were markedly elevated (p < 0.05) in the short-duration cases with continental and coastal air relative to those in the most common marine air, and the primary markers primarily contained local characteristics. The troughs showed the enhancements of many SOA markers (p < 0.05), which appeared to be related to the high relative humidity. The diurnal patterns of 2-methyltetrols varied in differed cases, and their aqueous formation at night seemed plausible, particularly in the presence of troughs. Eight sources were identified for the organic matter in submicron PM (PM1-OM). Despite being an urban site, the mean SOA contribution (66.1 ± 10.5 %), primarily anthropogenic, was significant. Anthropogenic SOA dominated in the cases with continental and coastal air and in the early afternoon. Local cooking and vehicle emissions became predominant in the case of marine air without troughs. Even averaged over the study period in this summer month with the prevalence of marine air, primary cooking emissions contributed up to 44.2 % to PM1-OM in the early evening. The study highlighted the need to control regional anthropogenic SOA and local cooking emissions to mitigate PM pollution in HK.
摘要。有机气溶胶(OA)是城市颗粒物(PM)的重要组成部分,其中的分子标记提供了有关其来源和形成机制的信息。这项研究以每两小时一次的分辨率,在一个夏季月份原位测量了超过 70 个有机气溶胶分子标记,重点研究了香港特别行政区(香港)一个市区地点的代表性标记的时间变化和有机气溶胶的动态来源贡献。与最常见的海洋空气相比,在大陆和沿海空气的短时情况下,二次 OA(SOA)标记物的水平明显升高(p < 0.05),而一次标记物主要包含本地特征。低谷显示了许多 SOA 标记的增强(p < 0.05),这似乎与高相对湿度有关。在不同的情况下,2-甲基四醇的昼夜模式各不相同,它们在夜间的水形成似乎是合理的,尤其是在出现低谷的情况下。亚微米级可吸入颗粒物(PM1-OM)中的有机物有八个来源。尽管这是一个城市站点,但 SOA 的平均贡献率(66.1 ± 10.5 %)非常高,主要是人为的。在有大陆和沿海空气的情况下,以及在下午早些时候,人为 SOA 占主导地位。在没有低谷的海洋空气中,本地烹饪和汽车尾气排放占主导地位。即使是在研究期间的平均值,在这个夏季海洋空气盛行的月份,一次烹饪排放对傍晚 PM1-OM 的影响高达 44.2%。这项研究强调有必要控制区域人为的 SOA 和本地烹饪排放,以减轻香港的 PM 污染。
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引用次数: 0
Upper tropospheric pollutants observed by MIPAS: geographic and seasonal variations MIPAS 观测到的对流层上层污染物:地理和季节变化
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-20 DOI: 10.5194/egusphere-2024-1793
Norbert Glatthor, Gabriele P. Stiller, Thomas von Clarmann, Bernd Funke, Sylvia Kellmann, Andrea Linden
Abstract. We present a global climatology of upper tropospheric hydrogen cyanide (HCN), carbon monoxide (CO), acetylene (C2H2), ethane (C2H6), peroxyacetyl nitrate (PAN) and formic acid (HCOOH), obtained from MIPAS/Envisat observations between 2002 and 2012. At northern mid- and high latitudes the biomass burning tracer HCN as well as CO, PAN and HCOOH exhibit maxima during spring and/or summer and minima during winter. On the contrary, maximum northern extra-tropical C2H2 and C2H6 amounts were measured during winter and spring and minimum values during summer and fall. In the tropics and subtropics, enhanced amounts of all pollutants were observed during all seasons, especially widespread and up to southern mid-latitudes during austral spring. Other characteristic features are eastward transport of anthropogenic C2H6 and of biogenic HCOOH from Central and North America in boreal summer, accumulation of pollutants in the Asian Monsoon Anticyclone and enhanced C2H2 over South-East Asia in boreal winter. Clear indication of biogenic release of HCOOH was also found above tropical South America and Africa. A global correlation analysis of the other pollutants with HCN corroborates common release by biomass burning as source of the widespread southern hemispheric pollution during austral spring. Further, high correlation with HCN points to biomass burning as major source of tropical and subtropical C2H2 and PAN during most of the year. In the northern extra-tropics there are generally low correlations with HCN during spring and early summer, indicating the influence of anthropogenic and biogenic sources. However, in August there are stronger correlations above Siberia and boreal North America, which points to common release by boreal fires. This is confirmed by the respective enhancement ratios (ERs). The ERs measured above North-East Africa fit well to the emission ratios of the dominant local fire type (savanna burning) for C2H2, while those for CO, C2H6 and HCOOH rather indicate tropical forest fires or additional anthropogenic or biogenic sources. The southern hemispheric ΔC2H6/ΔHCN ERs obtained during August to October are in good agreement with the emission ratio for savanna fires. The same applies for ΔC2H2/ΔHCN in August and for ΔHCN/ΔCO as well as for ΔHCOOH/ΔHCN in October.
摘要我们介绍了对流层上层氰化氢(HCN)、一氧化碳(CO)、乙炔(C2H2)、乙烷(C2H6)、过氧乙酰硝酸(PAN)和甲酸(HCOOH)的全球气候学数据,这些数据来自 2002 年至 2012 年期间的 MIPAS/Envisat 观测。在北部中高纬度地区,生物质燃烧示踪剂 HCN 以及 CO、PAN 和 HCOOH 在春季和/或夏季达到最大值,在冬季达到最小值。相反,北热带外的 C2H2 和 C2H6 量在冬季和春季达到最大值,在夏季和秋季达到最小值。在热带和亚热带地区,所有污染物的含量在各个季节都有所增加,尤其是在大范围内,直至南半球中纬度地区的春季。其他特征包括:在北方夏季,人为 C2H6 和生物源 HCOOH 从中美洲和北美洲向东迁移;在亚洲季风反气旋中污染物累积;在北方冬季,东南亚上空的 C2H2 增加。在热带南美洲和非洲上空也发现了 HCOOH 生物源释放的明显迹象。对其他污染物与 HCN 的全球相关性分析证实,生物质燃烧的共同释放是南半球春季大范围污染的来源。此外,与 HCN 的高度相关性表明,生物质燃烧是全年大部分时间热带和亚热带 C2H2 和 PAN 的主要来源。在北热带以外地区,春季和初夏与 HCN 的相关性普遍较低,表明人为和生物源的影响。然而,在八月份,西伯利亚和北美洲北部上空的相关性较强,这表明北半球的火星共同释放了HCN。各自的增强比(ER)证实了这一点。在非洲东北部上空测量到的增强比与当地主要火山类型(热带稀树草原燃烧)的 C2H2 排放比非常吻合,而 CO、C2H6 和 HCOOH 的增强比则表明是热带森林火山或其他人为或生物源造成的。8 月至 10 月期间获得的南半球 ΔC2H6/ΔHCN ER 与热带稀树草原焚烧的排放比率非常吻合。8 月份的 ΔC2H2/ΔHCN 和 10 月份的 ΔHCN/ΔCO 以及 ΔHCOOH/ΔHCN 也是如此。
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引用次数: 0
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) 共同体区域大气化学多相机制(CRACMM)中化学品生产和沉积损失对甲醛的作用
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-19 DOI: 10.5194/egusphere-2024-1680
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, Havala O. T. Pye
Abstract. Formaldehyde (HCHO) is an important air pollutant due to its direct health effects as an air toxic that contributes to elevated cancer risk, its role in ozone formation, and its role as a product from oxidation of most gas phase reactive organic carbon. We make several updates affecting secondary production of HCHO in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) in the Community Multiscale Air Quality (CMAQ) model. Secondary HCHO from isoprene and monoterpenes is increased, correcting an underestimate in the current version. Simulated 2019 June–August surface HCHO during peak photochemical production (11 am–3 pm) increased by 0.6 ppb (32 %) over the southeastern US and by 0.2 ppb (13 %) over the entire contiguous US. The increased HCHO compares more favorably with satellite-based observations from TROPOMI and observations from an aircraft campaign. Evaluation against hourly surface observations indicates a missing nighttime sink for HCHO which can be ameliorated by adding bidirectional exchange of HCHO and a leaf wetness dependent deposition process which increases nighttime deposition, decreasing 2019 June–August nocturnal (8 pm–4 am) surface HCHO by 1.1 ppb (36 %) over the southeastern US and 0.5 ppb (29 %) over the entire contiguous US. The ability of CRACMM to capture peak levels of HCHO at midday is improved, particularly at sites in the northeastern US, while peak levels at southeastern US sites are improved though still lower than observed. Using established risk assessment methods, lifetime exposure of the contiguous U.S. population (~320 million) to ambient HCHO levels predicted here may result in 6200 lifetime cancer cases, 40 % of which are from controllable anthropogenic emissions of nitrogen oxides and reactive organic compounds. Chemistry updates will be available in CRACMM version 2 (CRACMM2) in CMAQv5.5.
摘要甲醛(HCHO)是一种重要的空气污染物,因为它作为一种空气有毒物质会直接影响健康,导致癌症风险升高,它在臭氧形成中的作用,以及它作为大多数气相活性有机碳氧化产物的作用。我们对共同体多尺度空气质量(CMAQ)模型中的共同体区域大气化学多相机制(CRACMM)中影响 HCHO 二次生成的部分进行了更新。增加了异戊二烯和单萜烯产生的二次 HCHO,纠正了当前版本中的低估。在光化学生成高峰期(上午 11 点至下午 3 点),模拟的 2019 年 6-8 月地表 HCHO 在美国东南部增加了 0.6 ppb(32%),在整个美国毗连地区增加了 0.2 ppb(13%)。增加的 HCHO 与 TROPOMI 卫星观测数据和飞机观测数据相比更为接近。根据每小时地表观测数据进行的评估表明,夜间缺少 HCHO 吸收汇,但可以通过增加 HCHO 的双向交换和叶片湿度依赖性沉积过程来改善,从而增加夜间沉积,使美国东南部地区 2019 年 6-8 月夜间(晚 8 点至早 4 点)地表 HCHO 减少 1.1 ppb(36%),整个美国毗连地区减少 0.5 ppb(29%)。CRACMM 捕获正午 HCHO 峰值水平的能力有所提高,尤其是在美国东北部的站点,而美国东南部站点的峰值水平有所提高,但仍低于观测值。使用既定的风险评估方法,美国毗连地区人口(约 3.2 亿)终生暴露于此处预测的环境 HCHO 水平可能会导致 6200 例癌症病例,其中 40% 来自可控的人为氮氧化物和活性有机化合物排放。化学更新将在 CMAQv5.5 中的 CRACMM 第 2 版 (CRACMM2) 中提供。
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引用次数: 0
Signs of climate variability in double tropopause global distribution from radio occultation data 从无线电掩星数据看双对流层顶全球分布的气候变异迹象
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-19 DOI: 10.5194/egusphere-2024-1654
Alejandro de la Torre, Peter Alexander, Torsten Schmidt, Andrea K. Steiner, Florian Ladstädter, Rodrigo Hierro, Pablo Llamedo
Abstract. In a standard atmosphere, there is a single lapse rate tropopause (in what follows, tropopause) that separates the troposphere below from the stratosphere above. However, in certain situations, such as in regions of strong vertical wind shear or associated with certain weather phenomena, a second tropopause layer may form above the standard tropopause. The presence of a double tropopause (DT) can have implications for atmospheric and climate studies, as it may be associated with dynamic and complex weather patterns. Based on 14 years of temperature profiles retrieved by GNSS radio occultation and the resulting DT, a possible relationship between the spatio-temporal distribution of the relative number of DT to simple tropopauses (NDT) (or dependent variable) and a set of monthly climate indices (or features) is explored with a focus on the methodological approach. A cluster analysis is applied to geographically associate the DT occurrences with the climate indices. Then a multivariate linear regression is constructed using a progression of different models to identify the relevant features for the occurrence of DTs. On a global scale, from a hierarchical cluster analysis six sub-regions with different location and spread characteristics are identified. In addition to the condition of linearity in the residuals, the performance of each model in the train and test populations is evaluated to discard possible overfitting. The required conditions of non-collinearity, stationarity and cross-correlation between the features and the relative number of NDT after the removal of the climatological mean for each month (NDT’) are checked. Mean squared errors, adjusted coefficient of determination (adjusted R2) and number of degrees of freedom (F-statistic) parameters are evaluated for each model obtained. Taking into account the constraints of the present analysis, the most relevant climatic indices for the distribution of NDT' are identified.
摘要在标准大气中,有一个单一的失效率对流层顶(以下简称 "对流层顶")将下面的对流层和上面的平流层分开。然而,在某些情况下,例如在强垂直风切变区域或与某些天气现象相关的区域,在标准对流层顶之上可能会形成第二个对流层顶层。双对流层顶(DT)的出现对大气和气候研究有影响,因为它可能与动态和复杂的天气模式有关。根据全球导航卫星系统无线电掩星检索到的 14 年温度剖面图和由此产生的双对流层顶,探讨了双对流层顶与简单对流层顶相对数量(或因变量)的时空分布与一系列月气候指数(或特征)之间可能存在的关系,重点是方法学方法。采用聚类分析将 DT 出现的地理位置与气候指数联系起来。然后,利用一系列不同的模型构建多元线性回归,以确定出现 DTs 的相关特征。在全球范围内,通过分层聚类分析,确定了六个具有不同位置和分布特征的子区域。除了残差的线性条件外,还对每个模型在训练群和测试群中的性能进行了评估,以排除可能的过拟合。对各特征之间的非共线性、静止性和交叉相关性以及去除各月气候平均值后的无损检测相对数量("无损检测")等必要条件进行检查。对获得的每个模型的均方误差、调整后的判定系数(调整后 R2)和自由度数(F 统计量)参数进行评估。考虑到本次分析的限制因素,确定了与 NDT'分布最相关的气候指数。
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Atmospheric Chemistry and Physics
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