首页 > 最新文献

Atmospheric Chemistry and Physics最新文献

英文 中文
Impact of Asian aerosols on the summer monsoon strongly modulated by regional precipitation biases 亚洲气溶胶对夏季季风的影响受区域降水偏差的强烈调节
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-25 DOI: 10.5194/acp-24-7227-2024
Zhen Liu, Massimo A. Bollasina, Laura J. Wilcox
Abstract. Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models that suffer from long-standing biases, undermining their reliability in attributing anthropogenically forced changes. We analyze a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols and associated physical mechanisms, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatio-temporal variability in the climatological monsoon winds, clouds, and precipitation across Asia, which modulates the magnitude and efficacy of aerosol–cloud–precipitation interactions, an important component of the total aerosol response. There is a strong interplay between South Asia and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early- and late-summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realize the full extent of the aerosol impact over Asia. These findings provide important implications for better understanding and constraining the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections.
摘要。将亚洲夏季季风的变化可靠地归因于气溶胶的作用,对于减少未来区域水供应预测的不确定性至关重要,而这对这一人口稠密地区的风险管理和适应规划至关重要。然而,模拟季风对于气候模型来说仍然是一个挑战,因为气候模型长期以来存在偏差,这削弱了它们归因于人为强迫变化的可靠性。我们分析了一系列气候模式实验,以确定模式偏差与季风对亚洲气溶胶的响应及相关物理机制之间的联系,包括大尺度环流变化的作用。气溶胶对季风降水和环流的影响深受模型模拟亚洲各地气候学季风风、云和降水时空变化能力的影响,这种能力会调节气溶胶-云-降水相互作用的程度和效果,而这是气溶胶总响应的一个重要组成部分。南亚和东亚季风降水偏差及其在驱动整体季风响应中的相对主导地位之间存在着强烈的相互作用。我们发现,气溶胶驱动的初夏和夏末变化之间形成了鲜明对比,这是因为这两个地区的偏差具有相反的符号和季节演变。大尺度大气环流演变的真实模拟对于全面了解气溶胶对亚洲的影响至关重要。这些发现对更好地理解和制约历史模拟和未来预测中模式对亚洲上空气溶胶变化的反应的多样性和不一致性具有重要意义。
{"title":"Impact of Asian aerosols on the summer monsoon strongly modulated by regional precipitation biases","authors":"Zhen Liu, Massimo A. Bollasina, Laura J. Wilcox","doi":"10.5194/acp-24-7227-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7227-2024","url":null,"abstract":"Abstract. Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models that suffer from long-standing biases, undermining their reliability in attributing anthropogenically forced changes. We analyze a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols and associated physical mechanisms, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatio-temporal variability in the climatological monsoon winds, clouds, and precipitation across Asia, which modulates the magnitude and efficacy of aerosol–cloud–precipitation interactions, an important component of the total aerosol response. There is a strong interplay between South Asia and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early- and late-summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realize the full extent of the aerosol impact over Asia. These findings provide important implications for better understanding and constraining the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452951","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}
引用次数: 0
Unheralded contributions of biogenic volatile organic compounds from urban greening to ozone pollution: a high-resolution modeling study 城市绿化产生的生物挥发性有机化合物对臭氧污染的贡献未被察觉:一项高分辨率模型研究
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-25 DOI: 10.5194/egusphere-2024-1163
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Tianhang Zhang, Chong Shen
Abstract. Urban Green Spaces (UGS) are widely advocated for mitigating urban atmospheric environment. However, this study reveals that it can exacerbate urban ozone (O3) levels under certain conditions, as demonstrated by a September 2017 study in Guangzhou, China. Utilizing the Weather Research and Forecasting Model with the Model of Emissions of Gases and Aerosols from Nature (WRF-MEGAN) and the Community Multiscale Air Quality (CMAQ) model with a high horizontal resolution (1 km), we assessed the impact of UGS-related biogenic volatile organic compound (BVOC) emissions on urban O3. Our findings indicate that UGS-BVOC emissions in Guangzhou amounted to 666.49 Gg, primarily from isoprene (ISOP) and terpenes (TERP). These emissions contribute ~30 % of urban ISOP concentrations and their incorporations to the model significantly reduce the underestimation against observations. The study shows improvements in simulation biases for NO2, from 7.01 µg/m3 to 6.03 µg/m3, and for O3, from 7.77 µg/m3 to -1.60 µg/m3. UGS-BVOC and UGS-LUCC (land use cover changes) integration in air quality models notably enhances surface monthly mean O3 predictions by 3.6–8.0 µg/m3 (+3.8–8.5 %) and contributes up to 18.7 µg/m3 (+10.0 %) to MDA8 O3 during O3 pollution episodes. Additionally, UGS-BVOC emissions alone increase the monthly mean O3 levels by 2.2–3.0 µg/m3 (+2.3–3.2 %) in urban areas and contribute up to 6.3 µg/m3 (+3.3 %) to MDA8 O3 levels during O3 pollution episodes. These impacts can extend to surrounding suburban and rural areas through regional transport, highlighting the need for selecting low-emission vegetation and refining vegetation classification in urban planning.
摘要城市绿地(UGS)被广泛提倡用于缓解城市大气环境。然而,本研究发现,在某些条件下,城市绿地会加剧城市臭氧(O3)水平,2017 年 9 月在中国广州进行的一项研究就证明了这一点。利用气象研究和预报模型与自然界气体和气溶胶排放模型(WRF-MEGAN)以及高水平分辨率(1 千米)的社区多尺度空气质量(CMAQ)模型,我们评估了与 UGS 相关的生物挥发性有机化合物(BVOC)排放对城市臭氧(O3)的影响。研究结果表明,广州的 UGS-BVOC 排放量为 666.49 千兆克,主要来自异戊二烯(ISOP)和萜烯(TERP)。这些排放物占城市 ISOP 浓度的约 30%,将其纳入模型可显著减少对观测数据的低估。研究显示,二氧化氮的模拟偏差从 7.01 µg/m3 降至 6.03 µg/m3,臭氧的模拟偏差从 7.77 µg/m3 降至 -1.60 µg/m3。将 UGS-BVOC 和 UGS-LUCC(土地利用覆盖变化)集成到空气质量模型中,可显著提高地表月平均 O3 预测值 3.6-8.0 µg/m3 (+3.8-8.5 %),并在 O3 污染事件期间对 MDA8 O3 的贡献高达 18.7 µg/m3 (+10.0 %)。此外,仅 UGS-BVOC 排放就会使城市地区的月平均 O3 水平增加 2.2-3.0 µg/m3 (+2.3-3.2 %),并在 O3 污染事件期间使 MDA8 的 O3 水平增加高达 6.3 µg/m3 (+3.3 %)。这些影响可通过区域运输扩展到周围的郊区和农村地区,这突出表明了在城市规划中选择低排放植被和完善植被分类的必要性。
{"title":"Unheralded contributions of biogenic volatile organic compounds from urban greening to ozone pollution: a high-resolution modeling study","authors":"Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Tianhang Zhang, Chong Shen","doi":"10.5194/egusphere-2024-1163","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1163","url":null,"abstract":"<strong>Abstract.</strong> Urban Green Spaces (UGS) are widely advocated for mitigating urban atmospheric environment. However, this study reveals that it can exacerbate urban ozone (O<sub>3</sub>) levels under certain conditions, as demonstrated by a September 2017 study in Guangzhou, China. Utilizing the Weather Research and Forecasting Model with the Model of Emissions of Gases and Aerosols from Nature (WRF-MEGAN) and the Community Multiscale Air Quality (CMAQ) model with a high horizontal resolution (1 km), we assessed the impact of UGS-related biogenic volatile organic compound (BVOC) emissions on urban O<sub>3</sub>. Our findings indicate that UGS-BVOC emissions in Guangzhou amounted to 666.49 Gg, primarily from isoprene (ISOP) and terpenes (TERP). These emissions contribute ~30 % of urban ISOP concentrations and their incorporations to the model significantly reduce the underestimation against observations. The study shows improvements in simulation biases for NO<sub>2</sub>, from 7.01 µg/m<sup>3</sup> to 6.03 µg/m<sup>3</sup>, and for O<sub>3</sub>, from 7.77 µg/m<sup>3</sup> to -1.60 µg/m<sup>3</sup>. UGS-BVOC and UGS-LUCC (land use cover changes) integration in air quality models notably enhances surface monthly mean O<sub>3</sub> predictions by 3.6–8.0 µg/m<sup>3 </sup>(+3.8–8.5 %) and contributes up to 18.7 µg/m<sup>3 </sup>(+10.0 %) to MDA8 O<sub>3</sub> during O<sub>3</sub> pollution episodes. Additionally, UGS-BVOC emissions alone increase the monthly mean O<sub>3</sub> levels by 2.2–3.0 µg/m<sup>3 </sup>(+2.3–3.2 %) in urban areas and contribute up to 6.3 µg/m<sup>3 </sup>(+3.3 %) to MDA8 O<sub>3</sub> levels during O<sub>3</sub> pollution episodes. These impacts can extend to surrounding suburban and rural areas through regional transport, highlighting the need for selecting low-emission vegetation and refining vegetation classification in urban planning.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452995","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}
引用次数: 0
Quantification and characterization of primary biological aerosol particles and bacteria aerosolized from Baltic seawater 波罗的海海水中初级生物气溶胶颗粒和气溶胶细菌的定量与定性
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-25 DOI: 10.5194/egusphere-2024-1851
Julika Zinke, Gabriel Freitas, Rachel Ann Foster, Paul Zieger, Ernst Douglas Nilsson, Piotr Markuszewski, Matthew Edward Salter
Abstract. Primary biological aerosol particles (PBAP) can influence climate and affect human health. To investigate the aerosolization of PBAP with sea spray aerosol (SSA), we conducted ship-based campaigns in the central Baltic Sea near Östergarnsholm in May and August 2021. Using a plunging jet sea spray simulation chamber filled with local seawater, we performed controlled chamber experiments to collect filters and measure aerosols. We determined the abundance of bacteria in the chamber air and seawater by staining and fluorescence microscopy, normalizing these values to sodium concentration to calculate enrichment factors. Our results showed that bacteria were enriched in the aerosol by 13 to 488 times compared to the underlying seawater, with no significant enrichment observed in the sea surface microlayer. Bacterial abundances obtained through microscopy were compared with estimates of fluorescent PBAP (fPBAP) using a single-particle fluorescence spectrometer. We estimated bacterial emission fluxes using two independent approaches: (1) applying the enrichment factors derived from this study with mass flux estimates from previous SSA parameterizations, and (2) using a scaling approach from a companion study. Both methods produced bacterial emission flux estimates that were in good agreement and on the same order of magnitude as previous studies, while fPBAP emission flux estimates were significantly lower. Furthermore, 16S rRNA sequencing identified the diversity of bacteria enriched in the nascent SSA compared to the underlying seawater.
摘要原生生物气溶胶粒子(PBAP)可影响气候和人类健康。为了研究初级生物气溶胶粒子(PBAP)与海雾气溶胶(SSA)的气溶胶化,我们于 2021 年 5 月和 8 月在波罗的海中部厄斯特加恩肖尔姆附近开展了船基活动。我们使用一个装满当地海水的柱塞式喷射海雾模拟舱,进行了受控舱实验,以收集过滤器并测量气溶胶。我们通过染色和荧光显微镜测定了舱内空气和海水中的细菌丰度,并将这些值与钠浓度进行归一化,以计算富集因子。结果表明,与底层海水相比,气溶胶中的细菌富集了 13 到 488 倍,而在海面微层中没有观察到明显的富集。通过显微镜获得的细菌丰度与使用单粒子荧光光谱仪估算的荧光 PBAP(fPBAP)进行了比较。我们使用两种独立的方法估算了细菌排放通量:(1) 将本研究得出的富集因子与先前 SSA 参数化估算的质量通量相结合;(2) 使用一项配套研究中的缩放方法。这两种方法得出的细菌排放通量估算值与之前的研究结果一致,且数量级相同,而 fPBAP 排放通量估算值则明显偏低。此外,16S rRNA 测序确定了与底层海水相比,新生 SSA 中富含的细菌多样性。
{"title":"Quantification and characterization of primary biological aerosol particles and bacteria aerosolized from Baltic seawater","authors":"Julika Zinke, Gabriel Freitas, Rachel Ann Foster, Paul Zieger, Ernst Douglas Nilsson, Piotr Markuszewski, Matthew Edward Salter","doi":"10.5194/egusphere-2024-1851","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1851","url":null,"abstract":"<strong>Abstract.</strong> Primary biological aerosol particles (PBAP) can influence climate and affect human health. To investigate the aerosolization of PBAP with sea spray aerosol (SSA), we conducted ship-based campaigns in the central Baltic Sea near Östergarnsholm in May and August 2021. Using a plunging jet sea spray simulation chamber filled with local seawater, we performed controlled chamber experiments to collect filters and measure aerosols. We determined the abundance of bacteria in the chamber air and seawater by staining and fluorescence microscopy, normalizing these values to sodium concentration to calculate enrichment factors. Our results showed that bacteria were enriched in the aerosol by 13 to 488 times compared to the underlying seawater, with no significant enrichment observed in the sea surface microlayer. Bacterial abundances obtained through microscopy were compared with estimates of fluorescent PBAP (fPBAP) using a single-particle fluorescence spectrometer. We estimated bacterial emission fluxes using two independent approaches: (1) applying the enrichment factors derived from this study with mass flux estimates from previous SSA parameterizations, and (2) using a scaling approach from a companion study. Both methods produced bacterial emission flux estimates that were in good agreement and on the same order of magnitude as previous studies, while fPBAP emission flux estimates were significantly lower. Furthermore, 16S rRNA sequencing identified the diversity of bacteria enriched in the nascent SSA compared to the underlying seawater.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452996","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}
引用次数: 0
Present-day correlations are insufficient to predict cloud albedo change by anthropogenic aerosols in E3SM v2 目前的相关性不足以预测 E3SM v2 中人为气溶胶造成的云反照率变化
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-25 DOI: 10.5194/acp-24-7253-2024
Naser Mahfouz, Johannes Mülmenstädt, Susannah Burrows
Abstract. Cloud albedo susceptibility to droplet number perturbation remains a source of uncertainty in understanding aerosol–cloud interactions and thus both past and present climate states. Through the Energy Exascale Earth System Model (E3SM) v2 experiments, we probe the effects of competing processes on cloud albedo susceptibility of low-lying marine stratocumulus in the northeast Pacific. In present-day conditions, we find that increasing precipitation suppression by aerosols increases cloud albedo susceptibility, whereas increasing cloud sedimentation decreases it. By constructing a hypothetical model configuration exhibiting negative susceptibility under all conditions, we conclude that cloud albedo change due to aerosol perturbation cannot be predicted by present-day co-variabilities in E3SM v2. As such, our null result herein challenges the assumption that present-day climate observations are sufficient to constrain past states, at least in the context of cloud albedo changes to aerosol perturbation.
摘要。云反照率对液滴数量扰动的敏感性仍然是理解气溶胶-云相互作用以及过去和现在气候状态的不确定性来源。通过能源超大规模地球系统模式(E3SM)v2 实验,我们探究了竞争过程对东北太平洋低海平面层积云反照率的影响。我们发现,在当今条件下,气溶胶对降水的抑制增加会提高云反照率,而云沉积的增加则会降低云反照率。通过构建一个在所有条件下都表现出负易感性的假设模型配置,我们得出结论:气溶胶扰动导致的云反照率变化无法通过 E3SM v2 中的现今共变量进行预测。因此,至少在气溶胶扰动引起的云反照率变化方面,我们在此得出的无效结果对当今气候观测足以制约过去状态的假设提出了挑战。
{"title":"Present-day correlations are insufficient to predict cloud albedo change by anthropogenic aerosols in E3SM v2","authors":"Naser Mahfouz, Johannes Mülmenstädt, Susannah Burrows","doi":"10.5194/acp-24-7253-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7253-2024","url":null,"abstract":"Abstract. Cloud albedo susceptibility to droplet number perturbation remains a source of uncertainty in understanding aerosol–cloud interactions and thus both past and present climate states. Through the Energy Exascale Earth System Model (E3SM) v2 experiments, we probe the effects of competing processes on cloud albedo susceptibility of low-lying marine stratocumulus in the northeast Pacific. In present-day conditions, we find that increasing precipitation suppression by aerosols increases cloud albedo susceptibility, whereas increasing cloud sedimentation decreases it. By constructing a hypothetical model configuration exhibiting negative susceptibility under all conditions, we conclude that cloud albedo change due to aerosol perturbation cannot be predicted by present-day co-variabilities in E3SM v2. As such, our null result herein challenges the assumption that present-day climate observations are sufficient to constrain past states, at least in the context of cloud albedo changes to aerosol perturbation.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453111","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}
引用次数: 0
The Impact of Aqueous Phase Replacement Reaction on the Phase State of Internally Mixed Organic/ammonium Aerosols 水相置换反应对内部混合有机物/铵气溶胶相态的影响
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/egusphere-2024-1556
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, Yunhong Zhang
Abstract. Aerosol phase state is crucial for air quality, climate, and human health. Atmospheric secondary aerosols are often internally mixed with organic and inorganic components, particularly dicarboxylic acids, ammonium, sulfate, nitrate, and chloride. These complex compositions enable aqueous reaction between organic and inorganic species, significantly complicating aerosol phase behaviour during aging and making phase predictions challenging. We investigated carboxylate/ammonium salt mixtures using in-situ infrared spectroscopy. The di- and tri- carboxylates included sodium pyruvate (SP), sodium tartrate (ST), and sodium citrate (SC), while the ammonium salts included NH4NO3, NH4Cl, and (NH4)2SO4. Our results demonstrated that aqueous replacement reactions between carboxylates and ammonium salts was promoted by the formation and depletion of NH3 as relative humidity (RH) changed. Solid NaNO3, SP, and Na2SO4 formed in SP/ammonium aerosol at 35.7 %~12.7 %, 64 % and 65.5 %~60.1 % RH, respectively. In contrast, reactions between ST or SC and (NH4)2SO4 was incomplete due to the gel structure of SC or ST at low RH. Upon hydration, the deliquescence RH of Na2SO4 in SP/(NH4)2SO4 (88.8 %–95.2 %) and NaNO3 in SP/NH4NO3 (76.5–81.9 %) are higher than those of pure inorganic aerosols. Unexpectedly, aqueous Na2SO4 crystallized upon humidification in ST/(NH4)2SO4 particles at 43.6 % RH and then deliquesced with increasing RH. This is attributed to decreased viscosity and increased ion mobility, which overcome the kinetic inhibition of ion movement, leading to nucleation and growth of Na2SO4 crystal. Our findings highlight the intricate interplay between chemical components within organic/inorganic aerosol, the impact of replacement reactions on aerosol aging and phase state, and subsequently on atmospheric processes.
摘要气溶胶相态对空气质量、气候和人类健康至关重要。大气中的二次气溶胶通常内部混合了有机和无机成分,特别是二羧酸、铵、硫酸盐、硝酸盐和氯化物。这些复杂的成分使得有机物和无机物之间能够发生水反应,从而使气溶胶在老化过程中的相态表现变得非常复杂,并使相态预测变得具有挑战性。我们利用原位红外光谱对羧酸盐/铵盐混合物进行了研究。二元和三元羧酸盐包括丙酮酸钠(SP)、酒石酸钠(ST)和柠檬酸钠(SC),而铵盐包括 NH4NO3、NH4Cl 和 (NH4)2SO4。我们的研究结果表明,随着相对湿度(RH)的变化,NH3 的形成和消耗促进了羧酸盐和铵盐之间的水置换反应。在相对湿度分别为 35.7 %~12.7 %、64 % 和 65.5 %~60.1 % 时,SP/铵气溶胶中会形成固体 NaNO3、SP 和 Na2SO4。相反,在低相对湿度条件下,由于 SC 或 ST 的凝胶结构,ST 或 SC 与 (NH4)2SO4 之间的反应不完全。水合时,SP/(NH4)2SO4 中 Na2SO4 的潮解相对湿度(88.8%-95.2%)和 SP/NH4NO3 中 NaNO3 的潮解相对湿度(76.5%-81.9%)均高于纯无机气溶胶。意想不到的是,ST/(NH4)2SO4 颗粒中的 Na2SO4 水溶液在相对湿度为 43.6% 时加湿后会结晶,然后随着相对湿度的增加而潮解。这归因于粘度降低和离子流动性增加,从而克服了离子运动的动力学抑制,导致 Na2SO4 晶体的成核和生长。我们的研究结果突显了有机/无机气溶胶中化学成分之间错综复杂的相互作用、置换反应对气溶胶老化和相态的影响以及随后对大气过程的影响。
{"title":"The Impact of Aqueous Phase Replacement Reaction on the Phase State of Internally Mixed Organic/ammonium Aerosols","authors":"Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, Yunhong Zhang","doi":"10.5194/egusphere-2024-1556","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1556","url":null,"abstract":"<strong>Abstract.</strong> Aerosol phase state is crucial for air quality, climate, and human health. Atmospheric secondary aerosols are often internally mixed with organic and inorganic components, particularly dicarboxylic acids, ammonium, sulfate, nitrate, and chloride. These complex compositions enable aqueous reaction between organic and inorganic species, significantly complicating aerosol phase behaviour during aging and making phase predictions challenging. We investigated carboxylate/ammonium salt mixtures using in-situ infrared spectroscopy. The di- and tri- carboxylates included sodium pyruvate (SP), sodium tartrate (ST), and sodium citrate (SC), while the ammonium salts included NH<sub>4</sub>NO<sub>3</sub>, NH<sub>4</sub>Cl, and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>. Our results demonstrated that aqueous replacement reactions between carboxylates and ammonium salts was promoted by the formation and depletion of NH<sub>3</sub> as relative humidity (RH) changed. Solid NaNO<sub>3</sub>, SP, and Na<sub>2</sub>SO<sub>4</sub> formed in SP/ammonium aerosol at 35.7 %~12.7 %, 64 % and 65.5 %~60.1 % RH, respectively. In contrast, reactions between ST or SC and (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> was incomplete due to the gel structure of SC or ST at low RH. Upon hydration, the deliquescence RH of Na<sub>2</sub>SO<sub>4</sub> in SP/(NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> (88.8 %–95.2 %) and NaNO<sub>3</sub> in SP/NH<sub>4</sub>NO<sub>3</sub> (76.5–81.9 %) are higher than those of pure inorganic aerosols. Unexpectedly, aqueous Na<sub>2</sub>SO<sub>4</sub> crystallized upon humidification in ST/(NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> particles at 43.6 % RH and then deliquesced with increasing RH. This is attributed to decreased viscosity and increased ion mobility, which overcome the kinetic inhibition of ion movement, leading to nucleation and growth of Na<sub>2</sub>SO<sub>4</sub> crystal. Our findings highlight the intricate interplay between chemical components within organic/inorganic aerosol, the impact of replacement reactions on aerosol aging and phase state, and subsequently on atmospheric processes.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444759","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}
引用次数: 0
Why does stratospheric aerosol forcing strongly cool the warm pool? 为什么平流层气溶胶迫使暖池强烈降温?
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/acp-24-7203-2024
Moritz Günther, Hauke Schmidt, Claudia Timmreck, Matthew Toohey
Abstract. Previous research has shown that stratospheric aerosol causes only a small temperature change per unit forcing because they produce stronger cooling in the tropical Indian Ocean and the western Pacific Ocean than in the global mean. The enhanced temperature change in this so-called “warm-pool” region activates strongly negative local and remote feedbacks, which dampen the global mean temperature response. This paper addresses the question of why stratospheric aerosol forcing affects warm-pool temperatures more strongly than CO2 forcing, using idealized MPI-ESM simulations. We show that the aerosol's enhanced effective forcing at the top of the atmosphere (TOA) over the warm pool contributes to the warm-pool-intensified temperature change but is not sufficient to explain the effect. Instead, the pattern of surface effective forcing, which is substantially different from the effective forcing at the TOA, is more closely linked to the temperature pattern. Independent of surface temperature changes, the aerosol heats the tropical stratosphere, accelerating the Brewer–Dobson circulation. The intensified Brewer–Dobson circulation exports additional energy from the tropics to the extratropics, which leads to a particularly strong negative forcing at the tropical surface. These results show how forced circulation changes can affect the climate response by altering the surface forcing pattern. Furthermore, they indicate that the established approach of diagnosing effective forcing at the TOA is useful for global means, but a surface perspective on the forcing must be adopted to understand the evolution of temperature patterns.
摘要以往的研究表明,平流层气溶胶每单位强迫只引起很小的温度变化,因为它们在热带印度洋和西太平洋产生的降温比在全球平均温度产生的降温更强。在这个所谓的 "暖池 "区域,温度变化的增强激活了强烈的本地和远程负反馈,从而抑制了全球平均温度响应。本文利用理想化的 MPI-ESM 模拟,探讨了为什么平流层气溶胶强迫对暖池温度的影响比二氧化碳强迫更强。我们的研究表明,气溶胶在暖池上空大气顶部(TOA)增强的有效作用力是暖池温度变化加剧的原因之一,但不足以解释这种效应。相反,地表有效作用力的模式与 TOA 上的有效作用力有很大不同,与温度模式的关系更为密切。与地表温度变化无关,气溶胶会加热热带平流层,加速布鲁尔-多布森环流。增强的布鲁尔-多布森环流将额外的能量从热带地区输出到外热带地区,从而在热带地表产生特别强的负强迫。这些结果表明了强迫环流变化如何通过改变地表强迫模式来影响气候响应。此外,这些结果还表明,诊断 TOA 有效强迫的既定方法对全球手段是有用的,但必须从表面强迫的角度来理解温度模式的演变。
{"title":"Why does stratospheric aerosol forcing strongly cool the warm pool?","authors":"Moritz Günther, Hauke Schmidt, Claudia Timmreck, Matthew Toohey","doi":"10.5194/acp-24-7203-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7203-2024","url":null,"abstract":"Abstract. Previous research has shown that stratospheric aerosol causes only a small temperature change per unit forcing because they produce stronger cooling in the tropical Indian Ocean and the western Pacific Ocean than in the global mean. The enhanced temperature change in this so-called “warm-pool” region activates strongly negative local and remote feedbacks, which dampen the global mean temperature response. This paper addresses the question of why stratospheric aerosol forcing affects warm-pool temperatures more strongly than CO2 forcing, using idealized MPI-ESM simulations. We show that the aerosol's enhanced effective forcing at the top of the atmosphere (TOA) over the warm pool contributes to the warm-pool-intensified temperature change but is not sufficient to explain the effect. Instead, the pattern of surface effective forcing, which is substantially different from the effective forcing at the TOA, is more closely linked to the temperature pattern. Independent of surface temperature changes, the aerosol heats the tropical stratosphere, accelerating the Brewer–Dobson circulation. The intensified Brewer–Dobson circulation exports additional energy from the tropics to the extratropics, which leads to a particularly strong negative forcing at the tropical surface. These results show how forced circulation changes can affect the climate response by altering the surface forcing pattern. Furthermore, they indicate that the established approach of diagnosing effective forcing at the TOA is useful for global means, but a surface perspective on the forcing must be adopted to understand the evolution of temperature patterns.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444762","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}
引用次数: 0
Simulations of primary and secondary ice production during an Arctic mixed-phase cloud case from the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) campaign 尼-埃勒松德气溶胶云实验(NASCENT)活动中北极混合相云情况下的初级和次级冰生产模拟
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/acp-24-7179-2024
Britta Schäfer, Robert Oscar David, Paraskevi Georgakaki, Julie Thérèse Pasquier, Georgia Sotiropoulou, Trude Storelvmo
Abstract. The representation of Arctic clouds and their phase distributions, i.e., the amount of ice and supercooled water, influences predictions of future Arctic warming. Therefore, it is essential that cloud phase is correctly captured by models in order to accurately predict the future Arctic climate. Ice crystal formation in clouds happens through ice nucleation (primary ice production) and ice multiplication (secondary ice production). In common weather and climate models, rime splintering is the only secondary ice production process included. In addition, prescribed number concentrations of cloud condensation nuclei or cloud droplets and ice-nucleating particles are often overestimated in Arctic environments by standard model configurations. This can lead to a misrepresentation of the phase distribution and precipitation formation in Arctic mixed-phase clouds, with important implications for the Arctic surface energy budget. During the Ny-Ålesund Aerosol Cloud Experiment (NASCENT), a holographic probe mounted on a tethered balloon took in situ measurements of number and mass concentrations of ice crystals and cloud droplets in Svalbard, Norway, during fall 2019 and spring 2020. In this study, we choose one case study from this campaign that shows evidence of strong secondary ice production and use the Weather Research and Forecasting (WRF) model to simulate it at a high vertical and spatial resolution. We test the performance of different microphysical parametrizations and apply a new state-of-the-art secondary ice parametrization. We find that agreement with observations highly depends on the prescribed cloud condensation nuclei/cloud droplet and ice-nucleating particle concentrations and requires an enhancement of secondary ice production processes. Lowering mass mixing ratio thresholds for rime splintering inside the Morrison microphysics scheme is crucial to enable secondary ice production and thereby match observations for the right reasons. In our case, rime splintering is required to initiate collisional breakup. The simulated contribution from collisional breakup is larger than that from droplet shattering. Simulating ice production correctly for the right reasons is a prerequisite for reliable simulations of Arctic mixed-phase cloud responses to future temperature or aerosol perturbations.
摘要北极云及其云相分布(即冰和过冷却水的数量)的表示影响对未来北极变暖的预测。因此,模型必须正确捕捉云相,以准确预测未来北极气候。云中冰晶的形成是通过冰核化(一次产冰)和冰增殖(二次产冰)进行的。在常见的天气和气候模型中,冰渣分裂是唯一包含的二次产冰过程。此外,标准模式配置通常会高估北极环境中云凝结核或云滴和成冰粒子的规定数量浓度。这可能导致北极混合相云中的相分布和降水形成被错误地描述,从而对北极地表能量预算产生重要影响。在 Ny-Ålesund 气溶胶云实验(NASCENT)期间,一个安装在系留气球上的全息探测器于 2019 年秋季和 2020 年春季在挪威斯瓦尔巴群岛对冰晶和云滴的数量和质量浓度进行了实地测量。在本研究中,我们从这次活动中选择了一个案例研究,该案例显示了强烈的二次产冰现象,并使用天气研究与预报(WRF)模型以较高的垂直和空间分辨率对其进行了模拟。我们测试了不同微物理参数的性能,并应用了最新的二次结冰参数。我们发现,与观测结果的一致性在很大程度上取决于规定的云凝结核/云滴和成冰粒子浓度,并且需要增强二次冰生成过程。在莫里森微物理方案中,降低云泥分裂的质量混合比阈值对于实现二次产冰至关重要,从而以正确的理由与观测结果相吻合。在我们的研究中,石灰劈裂是引发碰撞破裂的必要条件。碰撞破裂的模拟贡献大于液滴破碎的模拟贡献。以正确的理由正确模拟冰的生成是可靠模拟北极混合相云对未来温度或气溶胶扰动响应的前提条件。
{"title":"Simulations of primary and secondary ice production during an Arctic mixed-phase cloud case from the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) campaign","authors":"Britta Schäfer, Robert Oscar David, Paraskevi Georgakaki, Julie Thérèse Pasquier, Georgia Sotiropoulou, Trude Storelvmo","doi":"10.5194/acp-24-7179-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7179-2024","url":null,"abstract":"Abstract. The representation of Arctic clouds and their phase distributions, i.e., the amount of ice and supercooled water, influences predictions of future Arctic warming. Therefore, it is essential that cloud phase is correctly captured by models in order to accurately predict the future Arctic climate. Ice crystal formation in clouds happens through ice nucleation (primary ice production) and ice multiplication (secondary ice production). In common weather and climate models, rime splintering is the only secondary ice production process included. In addition, prescribed number concentrations of cloud condensation nuclei or cloud droplets and ice-nucleating particles are often overestimated in Arctic environments by standard model configurations. This can lead to a misrepresentation of the phase distribution and precipitation formation in Arctic mixed-phase clouds, with important implications for the Arctic surface energy budget. During the Ny-Ålesund Aerosol Cloud Experiment (NASCENT), a holographic probe mounted on a tethered balloon took in situ measurements of number and mass concentrations of ice crystals and cloud droplets in Svalbard, Norway, during fall 2019 and spring 2020. In this study, we choose one case study from this campaign that shows evidence of strong secondary ice production and use the Weather Research and Forecasting (WRF) model to simulate it at a high vertical and spatial resolution. We test the performance of different microphysical parametrizations and apply a new state-of-the-art secondary ice parametrization. We find that agreement with observations highly depends on the prescribed cloud condensation nuclei/cloud droplet and ice-nucleating particle concentrations and requires an enhancement of secondary ice production processes. Lowering mass mixing ratio thresholds for rime splintering inside the Morrison microphysics scheme is crucial to enable secondary ice production and thereby match observations for the right reasons. In our case, rime splintering is required to initiate collisional breakup. The simulated contribution from collisional breakup is larger than that from droplet shattering. Simulating ice production correctly for the right reasons is a prerequisite for reliable simulations of Arctic mixed-phase cloud responses to future temperature or aerosol perturbations.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444767","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}
引用次数: 0
Surface Observation Constrained High Frequency Coal Mine Methane Emissions in Shanxi China Reveal More Emissions than Inventories, Consistency with Satellite Inversion 地表观测制约的山西煤矿甲烷高频排放显示排放量多于清单,与卫星反演一致
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/egusphere-2024-1784
Fan Lu, Kai Qin, Jason Blake Cohen, Qin He, Pravash Tiwari, Wei Hu, Chang Ye, Yanan Shan, Qing Xu, Shuo Wang, Qiansi Tu
Abstract. This work focuses on Changzhi, Shanxi China, a city and surrounding rural region with one of the highest atmospheric concentrations of methane (CH4) world-wide (campaign-wide minimum/mean/standard deviation/max observations: 2.0, 2.9, 1.3, and 16 ppm) due to a rapid increase in the mining, production, and use of coal over the past decade. An intensive 15-day surface observation campaign of CH4 is used to drive a new analytical, mass-conserving method to compute and attribute CH4 emissions. Observations made in concentric circles at 1 km, 3 km, and 5 km around a high production high gas coal mine yielded emissions of 0.73, 0.28, and 0.15 ppm min-1 respectively. Attribution used a 2-box mass conserving model to identify the known mine’s emissions from 0.042–5.3 ppm min-1, and a previously unidentified mine’s emission from 0.22–7.9 ppm min-1. These results demonstrate the importance of simultaneously quantifying both the spatial and temporal distribution of CH4 to better control regional-scale CH4 emissions. Results of the attribution are used in tandem with observations of boundary layer height to quantify policy-relevant emissions from the two coal mines as 13670±7400 kg h-1 and 5070±2270 kg h-1 respectively. Both mines display a fat tail distribution, with respective 25th, median, and 75th percentile values of [870, 7500, 38700] kg h-1 and [431, 1590, 7000] kg h-1. These findings are demonstrated to be higher than CH4 emissions from equivalent oil and gas operations in the USA, with one about double and the other similar to day-to-day emissions inverted over 5-years using TROPOMI over the same region.
摘要这项工作的重点是中国山西长治市,该市及周边农村地区是世界上甲烷(CH4)大气浓度最高的地区之一(活动范围内的最小值/平均值/标准偏差/最大值观测值分别为 2.0、2.9、1.3 和 16 ppm):由于过去十年煤炭开采、生产和使用的快速增长,该地区的甲烷浓度分别为 2.0、2.9、1.3 和 16 ppm。通过对 CH4 进行为期 15 天的密集地表观测,采用了一种新的质量保证分析方法来计算和确定 CH4 排放量。在一个高产高瓦斯煤矿周围 1 千米、3 千米和 5 千米的同心圆范围内进行的观测得出的排放量分别为 0.73、0.28 和 0.15 ppm min-1。研究人员使用双箱质量守恒模型确定了已知煤矿的排放量为 0.042-5.3 ppm min-1,而之前未确定的煤矿的排放量为 0.22-7.9 ppm min-1。这些结果表明,同时量化 CH4 的空间和时间分布对于更好地控制区域尺度的 CH4 排放非常重要。归因结果与边界层高度观测结果结合使用,将两个煤矿与政策相关的排放量分别量化为 13670±7400 kg h-1 和 5070±2270 kg h-1。两个煤矿的排放量都呈肥尾分布,第 25 百分位数、中位数和第 75 百分位数分别为 [870, 7500, 38700] kg h-1 和 [431, 1590, 7000] kg h-1。这些研究结果表明,其甲烷排放量高于美国同等石油和天然气开采活动的甲烷排放量,一个约为后者的两倍,另一个则与使用 TROPOMI 对同一地区 5 年的日排放量进行反演后的结果相似。
{"title":"Surface Observation Constrained High Frequency Coal Mine Methane Emissions in Shanxi China Reveal More Emissions than Inventories, Consistency with Satellite Inversion","authors":"Fan Lu, Kai Qin, Jason Blake Cohen, Qin He, Pravash Tiwari, Wei Hu, Chang Ye, Yanan Shan, Qing Xu, Shuo Wang, Qiansi Tu","doi":"10.5194/egusphere-2024-1784","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1784","url":null,"abstract":"<strong>Abstract.</strong> This work focuses on Changzhi, Shanxi China, a city and surrounding rural region with one of the highest atmospheric concentrations of methane (CH<sub>4</sub>) world-wide (campaign-wide minimum/mean/standard deviation/max observations: 2.0, 2.9, 1.3, and 16 ppm) due to a rapid increase in the mining, production, and use of coal over the past decade. An intensive 15-day surface observation campaign of CH<sub>4</sub> is used to drive a new analytical, mass-conserving method to compute and attribute CH<sub>4</sub> emissions. Observations made in concentric circles at 1 km, 3 km, and 5 km around a high production high gas coal mine yielded emissions of 0.73, 0.28, and 0.15 ppm min<sup>-1</sup> respectively. Attribution used a 2-box mass conserving model to identify the known mine’s emissions from 0.042–5.3 ppm min<sup>-1</sup>, and a previously unidentified mine’s emission from 0.22–7.9 ppm min<sup>-1</sup>. These results demonstrate the importance of simultaneously quantifying both the spatial and temporal distribution of CH<sub>4</sub> to better control regional-scale CH<sub>4</sub> emissions. Results of the attribution are used in tandem with observations of boundary layer height to quantify policy-relevant emissions from the two coal mines as 13670±7400 kg h<sup>-1</sup> and 5070±2270 kg h<sup>-1 </sup>respectively. Both mines display a fat tail distribution, with respective 25<sup>th</sup>, median, and 75<sup>th</sup> percentile values of [870, 7500, 38700] kg h<sup>-1</sup> and [431, 1590, 7000] kg h<sup>-1</sup>. These findings are demonstrated to be higher than CH<sub>4</sub> emissions from equivalent oil and gas operations in the USA, with one about double and the other similar to day-to-day emissions inverted over 5-years using TROPOMI over the same region.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444753","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}
引用次数: 0
Measurement Report: Long-term Assessment of Primary and Secondary Organic Aerosols in Shanghai Megacity throughout China’s Clean Air Actions since 2010 测量报告:2010 年以来中国清洁空气行动期间上海特大城市一次和二次有机气溶胶的长期评估
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/egusphere-2024-1488
Haifeng Yu, Yunhua Chang, Lin Cheng, Yusen Duan, Jianlin Hu
Abstract. A growing body of research has demonstrated the effectiveness of China’s Air Pollution Prevention and Control Action Plan in controlling PM2.5 pollution. However, there is a lack of long-term studies investigating the impact of these abatement policies on carbonaceous aerosols in PM2.5, particularly secondary organic carbon (SOC). Shanghai, as China’s largest megacity and prominent industrial hub, serves as a crucial gateway to the nation’s rapid development with a population exceeding twenty million. In this study, we conducted hourly online measurements of organic carbon (OC) and elemental carbon (EC) in PM2.5 in Shanghai from July 2010 to July 2017. The results revealed that the annual concentrations (mean ± 1 σ) of OC and EC reached their peaks in 2013 (9.5 ± 6.4 and 2.7 ± 2.6 µg m-3 to 3.0 ± 2.3 µg m-3 and 2.7 ± 2.1 µg m-3). Subsequently, a consistent year-by-year decrease in both OC and EC concentrations was observed, mirroring the trend observed for PM2.5. Primary organic carbon (POC), the primary component of OC, accounted for an average of 65.6 %, displaying similar trends to OC. This finding indicates the effectiveness of primary emission control measures. However, the concentration of secondary organic carbon (SOC) did not decrease from 2013 to 2017, remaining relatively stable within the range of 2.7 ± 2.6 µg m-3 to 3.0 ± 2.3 µg m-3. When considering data from previous studies in Shanghai, concentrations of SOC did not exhibit a noticeable decline until 2018, coinciding with the implementation of measures targeting volatile organic compounds (VOCs) emissions. Seasonally, with the exception of 2011, OC and EC concentrations were highest during winter, likely influenced by unfavourable meteorological conditions and long-range transport. SOC displayed no distinct seasonal fluctuations, as its formation is influenced by both photochemical reactions and meteorological conditions. POC and SOC exhibited different diurnal patterns, but neither showed a significant weekend effect, suggesting limited reduction in anthropogenic activities during weekends. Furthermore, SOC concentrations exhibited simultaneous increases in summer, particularly when O3 concentrations exceeded 50 µg m-3, indicating that stronger oxidation reactions contribute to higher SOC concentrations. Our findings also revealed concentration gradients of SOC dependent on wind direction (WD) and wind speed (WS), with higher concentrations typically observed for winds originating from the southwest and northwest. Potential sources from distant regions were analyzed using the potential source contribution function (PSCF), indicating that the geographical potential source area is concentrated near the middle and lower Yangtze River.
摘要越来越多的研究表明,中国的《大气污染防治行动计划》在控制 PM2.5 污染方面卓有成效。然而,目前还缺乏有关这些减排政策对 PM2.5 中碳质气溶胶,尤其是二次有机碳 (SOC) 影响的长期研究。上海是中国最大的特大城市和著名的工业中心,人口超过两千万,是中国快速发展的重要门户。在本研究中,我们对 2010 年 7 月至 2017 年 7 月期间上海 PM2.5 中的有机碳(OC)和元素碳(EC)进行了每小时在线测量。结果显示,有机碳和元素碳的年浓度(平均值±1 σ)在2013年达到峰值(9.5±6.4和2.7±2.6 µg m-3至3.0±2.3 µg m-3和2.7±2.1 µg m-3)。随后,OC 和 EC 浓度逐年下降,与 PM2.5 的下降趋势一致。OC 的主要成分原始有机碳 (POC) 平均占 65.6%,其变化趋势与 OC 相似。这一结果表明了一次排放控制措施的有效性。然而,从2013年到2017年,二次有机碳(SOC)的浓度并没有下降,保持在2.7±2.6 µg m-3到3.0±2.3 µg m-3的范围内相对稳定。考虑到上海以往研究的数据,SOC 的浓度直到 2018 年才出现明显下降,与针对挥发性有机化合物(VOC)排放的措施的实施时间相吻合。从季节上看,除 2011 年外,OC 和 EC 的浓度在冬季最高,这可能是受到不利气象条件和长程飘移的影响。SOC 没有明显的季节性波动,因为其形成受到光化学反应和气象条件的影响。POC 和 SOC 表现出不同的昼夜变化规律,但都没有表现出明显的周末效应,这表明周末人为活动减少有限。此外,SOC 浓度在夏季同时增加,尤其是当 O3 浓度超过 50 µg m-3 时,这表明较强的氧化反应导致 SOC 浓度升高。我们的研究结果还显示,SOC 的浓度梯度取决于风向(WD)和风速(WS),通常西南风和西北风的浓度较高。利用潜在污染源贡献函数(PSCF)分析了来自遥远地区的潜在污染源,结果表明地理上的潜在污染源区域集中在长江中下游附近。
{"title":"Measurement Report: Long-term Assessment of Primary and Secondary Organic Aerosols in Shanghai Megacity throughout China’s Clean Air Actions since 2010","authors":"Haifeng Yu, Yunhua Chang, Lin Cheng, Yusen Duan, Jianlin Hu","doi":"10.5194/egusphere-2024-1488","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1488","url":null,"abstract":"<strong>Abstract.</strong> A growing body of research has demonstrated the effectiveness of China’s Air Pollution Prevention and Control Action Plan in controlling PM<sub>2.5</sub> pollution. However, there is a lack of long-term studies investigating the impact of these abatement policies on carbonaceous aerosols in PM<sub>2.5</sub>, particularly secondary organic carbon (SOC). Shanghai, as China’s largest megacity and prominent industrial hub, serves as a crucial gateway to the nation’s rapid development with a population exceeding twenty million. In this study, we conducted hourly online measurements of organic carbon (OC) and elemental carbon (EC) in PM<sub>2.5</sub> in Shanghai from July 2010 to July 2017. The results revealed that the annual concentrations (mean ± 1 σ) of OC and EC reached their peaks in 2013 (9.5 ± 6.4 and 2.7 ± 2.6 µg m<sup>-3</sup> to 3.0 ± 2.3 µg m<sup>-3</sup> and 2.7 ± 2.1 µg m<sup>-3</sup>). Subsequently, a consistent year-by-year decrease in both OC and EC concentrations was observed, mirroring the trend observed for PM<sub>2.5</sub>. Primary organic carbon (POC), the primary component of OC, accounted for an average of 65.6 %, displaying similar trends to OC. This finding indicates the effectiveness of primary emission control measures. However, the concentration of secondary organic carbon (SOC) did not decrease from 2013 to 2017, remaining relatively stable within the range of 2.7 ± 2.6 µg m<sup>-3</sup> to 3.0 ± 2.3 µg m<sup>-3</sup>. When considering data from previous studies in Shanghai, concentrations of SOC did not exhibit a noticeable decline until 2018, coinciding with the implementation of measures targeting volatile organic compounds (VOCs) emissions. Seasonally, with the exception of 2011, OC and EC concentrations were highest during winter, likely influenced by unfavourable meteorological conditions and long-range transport. SOC displayed no distinct seasonal fluctuations, as its formation is influenced by both photochemical reactions and meteorological conditions. POC and SOC exhibited different diurnal patterns, but neither showed a significant weekend effect, suggesting limited reduction in anthropogenic activities during weekends. Furthermore, SOC concentrations exhibited simultaneous increases in summer, particularly when O<sub>3</sub> concentrations exceeded 50 µg m<sup>-3</sup>, indicating that stronger oxidation reactions contribute to higher SOC concentrations. Our findings also revealed concentration gradients of SOC dependent on wind direction (WD) and wind speed (WS), with higher concentrations typically observed for winds originating from the southwest and northwest. Potential sources from distant regions were analyzed using the potential source contribution function (PSCF), indicating that the geographical potential source area is concentrated near the middle and lower Yangtze River.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444764","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}
引用次数: 0
Modeling study of the snow darkening effect by black carbon deposition over the Arctic during the melting period 北极融雪期黑炭沉积造成雪变黑效应的模型研究
IF 6.3 1区 地球科学 Q1 Earth and Planetary Sciences Pub Date : 2024-06-24 DOI: 10.5194/egusphere-2024-1717
Zilu Zhang, Libo Zhou, Meigen Zhang
Abstract. The rapid warming of the Arctic, accompanied by glacier and sea ice melt, has significant consequences for the Earth's climate, ecosystems, and economy. Recent evidence suggests that the snow-darkening effect (SDE) induced by light-absorbing particles, such as black carbon (BC) deposition, could greatly influence rapid warming in the Arctic. However, there is still a lack of ensemble simulations using high-resolution models for investigating the impacts of the SDE resulting from BC deposition on the Arctic surface energy balance. By integrating the physically based Snow, Ice, Aerosol, and Radiation (SNICAR) model with a polar-optimized version of the Weather Research and Forecasting model (Polar-WRF), this study aimed to quantify the impacts of the SDE due to BC deposition and analyze the relationship between BC aerosol mass in snow (represented by snow depth) and snow albedo reduction. The simulation results indicate that BC deposition can directly affect the surface energy balance by decreasing snow albedo and its corresponding radiative forcing (RF). On average, BC deposition at 50 ng g-1 causes a radiative forcing (RF) of 1.6 W m-2 in off-line simulations (without surface feedbacks) and 1.4 W m-2 in on-line simulations (with surface feedbacks). The high RF caused by BC deposition reached 1–4 W m-2 and mainly occurred in Greenland, Baffin Island and East Siberia, where areas with deep snow depths and large snow densities are prevalent. The changes in snow albedo are indeed strongly linked to the mass of BC aerosols. Notably, a clear linear relationship was established between snow depth and the reduction in snow albedo, with a correlation coefficient exceeding 0.9 and an R-squared value greater than 0.85 when the snow depth is shallow. However, as snow depth increases, the impact of BC on snow albedo gradually diminishes until it reaches its maximum value when the snowpack becomes sufficiently optically thick. Regions with deep snowpack, such as Greenland, tend to exhibit greater sensitivity to BC deposition due to the higher absolute mass of BC and the longer duration of the SDE. For a given column-mean BC concentration in snow, the impacts of the SDE are approximately 25–41 % greater in deep snow-covered areas than in shallow snow-covered areas, leading to a 19–40 % increase in snowmelt. A comparison between off-line and on-line coupled simulations using Polar-WRF/Noah-MP and SNICAR has provided valuable insights into the critical mechanisms and key factors influencing changes in surface heat transfer due to the impacts of the SDE induced by BC deposition in the Arctic. It has been observed that various processes, such as snow melting and land‒atmosphere interactions, play significant roles in assessing changes in the surface energy balance caused by BC deposition. Notably, off-line simulations tend to overestimate the impacts of the SDE, sometimes by more than 50 %, due
摘要伴随着冰川和海冰融化,北极地区迅速变暖,对地球气候、生态系统和经济产生了重大影响。最近的证据表明,黑碳(BC)沉积等光吸收颗粒引起的雪变暗效应(SDE)可能会对北极地区的快速变暖产生重大影响。然而,目前仍缺乏利用高分辨率模型进行的集合模拟,来研究黑碳沉积导致的黑化效应对北极地表能量平衡的影响。本研究通过将基于物理的雪、冰、气溶胶和辐射(SNICAR)模型与极地优化版天气研究和预报模型(Polar-WRF)进行集成,旨在量化 BC 沉积导致的 SDE 的影响,并分析雪中 BC 气溶胶质量(以雪深表示)与雪反照率降低之间的关系。模拟结果表明,BC 沉积可通过降低雪反照率及其相应的辐射强迫(RF)直接影响地表能量平衡。平均而言,在离线模拟(无地表反馈)和在线模拟(有地表反馈)中,50 ng g-1 的 BC 沉积造成的辐射强迫(RF)分别为 1.6 W m-2 和 1.4 W m-2。由 BC 沉积引起的高 RF 达到 1-4 W m-2,主要发生在格陵兰岛、巴芬岛和东西伯利亚,这些地区普遍积雪深且雪密度大。雪地反照率的变化确实与 BC 气溶胶的质量密切相关。值得注意的是,积雪深度与雪反照率的降低之间存在明显的线性关系,当积雪深度较浅时,相关系数超过 0.9,R 平方值大于 0.85。然而,随着积雪深度的增加,BC 对雪反照率的影响逐渐减小,直到积雪厚度达到足够的光学厚度时才达到最大值。格陵兰岛等积雪较深的地区,由于 BC 的绝对质量较大,SDE 的持续时间较长,往往对 BC 沉积表现出更大的敏感性。对于给定的雪中 BC 柱均值浓度,SDE 对积雪较深地区的影响比积雪较浅地区大约 25-41%,导致融雪量增加 19-40%。利用极地-WRF/Noah-MP 和 SNICAR 进行的离线和在线耦合模拟比较,为了解北极 BC 沉积引起的 SDE 对地表传热变化的关键机制和主要影响因素提供了宝贵的见解。据观察,雪融化和陆地-大气相互作用等各种过程在评估 BC 沉积引起的地表能量平衡变化方面发挥了重要作用。值得注意的是,由于缺乏相关过程,离线模拟往往会高估 SDE 的影响,有时高估超过 50%。这项研究强调了积雪条件和陆地-大气相互作用对评估 BC 沉积造成的 SDE 影响的重要性。因此,有必要将包含详细物理过程的高分辨率建模研究列为优先事项,以提高我们对SDE对北极气候变化影响的认识。
{"title":"Modeling study of the snow darkening effect by black carbon deposition over the Arctic during the melting period","authors":"Zilu Zhang, Libo Zhou, Meigen Zhang","doi":"10.5194/egusphere-2024-1717","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1717","url":null,"abstract":"<strong>Abstract.</strong> The rapid warming of the Arctic, accompanied by glacier and sea ice melt, has significant consequences for the Earth's climate, ecosystems, and economy. Recent evidence suggests that the snow-darkening effect (SDE) induced by light-absorbing particles, such as black carbon (BC) deposition, could greatly influence rapid warming in the Arctic. However, there is still a lack of ensemble simulations using high-resolution models for investigating the impacts of the SDE resulting from BC deposition on the Arctic surface energy balance. By integrating the physically based Snow, Ice, Aerosol, and Radiation (SNICAR) model with a polar-optimized version of the Weather Research and Forecasting model (Polar-WRF), this study aimed to quantify the impacts of the SDE due to BC deposition and analyze the relationship between BC aerosol mass in snow (represented by snow depth) and snow albedo reduction. The simulation results indicate that BC deposition can directly affect the surface energy balance by decreasing snow albedo and its corresponding radiative forcing (RF). On average, BC deposition at 50 ng g<sup>-1</sup> causes a radiative forcing (RF) of 1.6 W m<sup>-2</sup> in off-line simulations (without surface feedbacks) and 1.4 W m<sup>-2</sup> in on-line simulations (with surface feedbacks). The high RF caused by BC deposition reached 1–4 W m<sup>-2</sup> and mainly occurred in Greenland, Baffin Island and East Siberia, where areas with deep snow depths and large snow densities are prevalent. The changes in snow albedo are indeed strongly linked to the mass of BC aerosols. Notably, a clear linear relationship was established between snow depth and the reduction in snow albedo, with a correlation coefficient exceeding 0.9 and an R-squared value greater than 0.85 when the snow depth is shallow. However, as snow depth increases, the impact of BC on snow albedo gradually diminishes until it reaches its maximum value when the snowpack becomes sufficiently optically thick. Regions with deep snowpack, such as Greenland, tend to exhibit greater sensitivity to BC deposition due to the higher absolute mass of BC and the longer duration of the SDE. For a given column-mean BC concentration in snow, the impacts of the SDE are approximately 25–41 % greater in deep snow-covered areas than in shallow snow-covered areas, leading to a 19–40 % increase in snowmelt. A comparison between off-line and on-line coupled simulations using Polar-WRF/Noah-MP and SNICAR has provided valuable insights into the critical mechanisms and key factors influencing changes in surface heat transfer due to the impacts of the SDE induced by BC deposition in the Arctic. It has been observed that various processes, such as snow melting and land‒atmosphere interactions, play significant roles in assessing changes in the surface energy balance caused by BC deposition. Notably, off-line simulations tend to overestimate the impacts of the SDE, sometimes by more than 50 %, due ","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":null,"pages":null},"PeriodicalIF":6.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141444768","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}
引用次数: 0
期刊
Atmospheric Chemistry and Physics
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1