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- ItemIce-nucleating particle concentrations unaffected by urban air pollution in Beijing, China(Katlenburg-Lindau : EGU, 2018) Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, HeikeExceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
- ItemChemical composition and droplet size distribution of cloud at the summit of Mount Tai, China(Katlenburg-Lindau : EGU, 2017) Li, Jiarong; Wang, Xinfeng; Chen, Jianmin; Zhu, Chao; Li, Weijun; Li, Chengbao; Liu, Lu; Xu, Caihong; Wen, Liang; Xue, Likun; Wang, Wenxing; Ding, Aijun; Herrmann, HartmutThe chemical composition of 39 cloud samples and droplet size distributions in 24 cloud events were investigated at the summit of Mt. Tai from July to October 2014. Inorganic ions, organic acids, metals, HCHO, H2O2, sulfur( IV), organic carbon, and elemental carbon as well as pH and electrical conductivity were analyzed. The acidity of the cloud water significantly decreased from a reported value of pH 3.86 during 2007-2008 (Guo et al., 2012) to pH 5.87 in the present study. The concentrations of nitrate and ammonium were both increased since 2007-2008, but the overcompensation of ammonium led to an increase in the mean pH value. The microphysical properties showed that cloud droplets were smaller than 26.0 μm and most were in the range of 6.0-9.0 μm at Mt. Tai. The maximum droplet number concentration (Nd) was associated with a droplet size of 7.0 μm. High liquid water content (LWC) values could facilitate the formation of larger cloud droplets and broadened the droplet size distribution. Cloud droplets exhibited a strong interaction with atmospheric aerosols. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions and smaller sizes with increased numbers of cloud droplets. The lower pH values were likely to occur at higher PM2.5 concentrations. Clouds were an important sink for soluble materials in the atmosphere. The dilution effect of cloud water should be considered when estimating concentrations of soluble components in the cloud phase.
- ItemContinuous vertical aerosol profiling with a multi-wavelength Raman polarization lidar over the Pearl River Delta, China(Katlenburg-Lindau : EGU, 2017) Heese, Birgit; Baars, Holger; Bohlmann, Stephanie; Althausen, Dietrich; Deng, RuruA dataset of particle optical properties of the highly polluted atmosphere over the Pearl River Delta (PRD), Guangzhou, China, is presented in this paper. The data were derived from the measurements of a multiwavelength Raman and depolarization lidar PollyXT and a co-located AERONET sun photometer. The measurement campaign was conducted from November 2011 to mid-June 2012. These are the first Raman lidar measurements in the PRD that lasted for several months. A mean value of aerosol optical depth (AOD) of 0.54±0.33 was observed by the sun photometer at 500 nm in the polluted atmosphere over this megacity for the whole measurement period. The lidar profiles frequently show lofted aerosol layers, which reach altitudes of up to 2 to 3 km and, especially during the spring season, up to 5 km. These layers contain between 12 and 56% of the total AOD, with the highest values in spring. The aerosol types in these lofted layers are classified by their optical properties. The observed lidar ratio values range from 30 to 80 sr with a mean value of 48.0±10.7 sr at 532 nm. The linear particle depolarization ratio at 532 nm lies mostly below 5 %, with a mean value of 3.6±3.7 %. The majority of the Ångström exponents lie between 0.5 and 1.5, indicating a mixture of fine- and coarsemode aerosols. These results reveal that mostly urban pollution particles mixed with particles produced from biomass and industrial burning are present in the atmosphere above the Pearl River Delta. Trajectory analyses show that these pollution mixtures arise mainly from local and regional sources.
- ItemA novel method for deriving the aerosol hygroscopicity parameter based only on measurements from a humidified nephelometer system(Katlenburg-Lindau : EGU, 2017) Kuang, Ye; Zhao, Chunsheng; Tao, Jiangchuan; Bian, Yuxuan; Ma, Nan; Zhao, GangAerosol hygroscopicity is crucial for understanding roles of aerosol particles in atmospheric chemistry and aerosol climate effects. Light-scattering enhancement factor f (RH, λ) is one of the parameters describing aerosol hygroscopicity, which is defined as f (RH, λ) = δsp(RH, λ)=δsp(dry, λ), where δsp(RH, λ) or δsp(dry, λ) represents δsp at wavelength λ under certain relative humidity (RH) or dry conditions. Traditionally, an overall hygroscopicity parameter κ can be retrieved from measured f (RH, λ), hereinafter referred to as κf(RH), by combining concurrently measured particle number size distribution (PNSD) and mass concentration of black carbon. In this paper, a new method is proposed to directly derive κf(RH) based only on measurements from a three-wavelength humidified nephelometer system. The advantage of this newly proposed approach is that κf(RH) can be estimated without any additional information about PNSD and black carbon. This method is verified with measurements from two different field campaigns. Values of κf(RH) estimated from this new method agree very well with those retrieved by using the traditional method: all points lie near the 1 : 1 line and the square of correlation coefficient between them is 0.99. The verification results demonstrate that this newly proposed method of deriving κf(RH) is applicable at different sites and in seasons of the North China Plain and might also be applicable in other regions around the world.
- ItemImpact of water uptake and mixing state on submicron particle deposition in the human respiratory tract (HRT) based on explicit hygroscopicity measurements at HRT-like conditions(Katlenburg-Lindau : EGU, 2022) Man, Ruiqi; Wu, Zhijun; Zong, Taomou; Voliotis, Aristeidis; Qiu, Yanting; Größ, Johannes; van Pinxteren, Dominik; Zeng, Limin; Herrmann, Hartmut; Wiedensohler, Alfred; Hu, MinParticle hygroscopicity plays a key role in determining the particle deposition in the human respiratory tract (HRT). In this study, the effects of hygroscopicity and mixing state on regional and total deposition doses on the basis of the particle number concentration for children, adults, and the elderly were quantified using the Multiple-Path Particle Dosimetry model, based on the size-resolved particle hygroscopicity measurements at HRT-like conditions (relative humidity = 98 %) performed in the North China Plain. The measured particle population with an external mixing state was dominated by hygroscopic particles (number fraction = (91.5 ± 5.7) %, mean ± standard deviation (SD); the same below). Particle hygroscopic growth in the HRT led to a reduction by around 24 % in the total doses of submicron particles for all age groups. Such a reduction was mainly caused by the growth of hygroscopic particles and was more pronounced in the pulmonary and tracheobronchial regions. Regardless of hygroscopicity, the elderly group of people had the highest total dose among three age groups, while children received the maximum total deposition rate. With 270 nm in diameter as the boundary, the total deposition doses of particles smaller than this diameter were overestimated, and those of larger particles were underestimated, assuming no particle hygroscopic growth in the HRT. From the perspective of the daily variation, the deposition rates of hygroscopic particles with an average of (2.88 ± 0.81) × 109 particles h-1 during the daytime were larger than those at night ((2.32 ± 0.24) × 109 particles h-1). On the contrary, hydrophobic particles interpreted as freshly emitted soot and primary organic aerosols exhibited higher deposition rates at nighttime ((3.39 ± 1.34) × 108 particles h-1) than those in the day ((2.58 ± 0.76) × 108 particles h-1). The traffic emissions during the rush hours enhanced the deposition rate of hydrophobic particles. This work provides a more explicit assessment of the impact of hygroscopicity and mixing state on the deposition pattern of submicron particles in the HRT. Copyright:
- ItemTeleconnections among tipping elements in the Earth system(London : Nature Publ. Group, 2023) Liu, Teng; Chen, Dean; Yang, Lan; Meng, Jun; Wang, Zanchenling; Ludescher, Josef; Fan, Jingfang; Yang, Saini; Chen, Deliang; Kurths, Jürgen; Chen, Xiaosong; Havlin, Shlomo; Schellnhuber, Hans JoachimTipping elements are components of the Earth system that may shift abruptly and irreversibly from one state to another at specific thresholds. It is not well understood to what degree tipping of one system can influence other regions or tipping elements. Here, we propose a climate network approach to analyse the global impacts of a prominent tipping element, the Amazon Rainforest Area (ARA). We find that the ARA exhibits strong correlations with regions such as the Tibetan Plateau (TP) and West Antarctic ice sheet. Models show that the identified teleconnection propagation path between the ARA and the TP is robust under climate change. In addition, we detect that TP snow cover extent has been losing stability since 2008. We further uncover that various climate extremes between the ARA and the TP are synchronized under climate change. Our framework highlights that tipping elements can be linked and also the potential predictability of cascading tipping dynamics.
- ItemWarming assessment of the bottom-up Paris Agreement emissions pledges([London] : Nature Publishing Group UK, 2018) Robiou du Pont, Yann; Meinshausen, MalteUnder the bottom-up architecture of the Paris Agreement, countries pledge Nationally Determined Contributions (NDCs). Current NDCs individually align, at best, with divergent concepts of equity and are collectively inconsistent with the Paris Agreement. We show that the global 2030-emissions of NDCs match the sum of each country adopting the least-stringent of five effort-sharing allocations of a well-below 2 °C-scenario. Extending such a self-interested bottom-up aggregation of equity might lead to a median 2100-warming of 2.3 °C. Tightening the warming goal of each country’s effort-sharing approach to aspirational levels of 1.1 °C and 1.3 °C could achieve the 1.5 °C and well-below 2 °C-thresholds, respectively. This new hybrid allocation reconciles the bottom-up nature of the Paris Agreement with its top-down warming thresholds and provides a temperature metric to assess NDCs. When taken as benchmark by other countries, the NDCs of India, the EU, the USA and China lead to 2.6 °C, 3.2 °C, 4 °C and over 5.1 °C warmings, respectively.
- ItemMolecular distributions of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in PM2.5 collected at the top of Mt. Tai, North China, during the wheat burning season of 2014(Katlenburg-Lindau : EGU, 2018) Zhu, Yanhong; Yang, Lingxiao; Chen, Jianmin; Kawamura, Kimitaka; Sato, Mamiko; Tilgner, Andreas; van Pinxteren, Dominik; Chen, Ying; Xue, Likun; Wang, Xinfeng; Simpson, Isobel J.; Herrmann, Hartmut; Blake, Donald R.; Wang, WenxingFine particulate matter (PM2.5) samples collected at Mount (Mt.) Tai in the North China Plain during summer 2014 were analyzed for dicarboxylic acids and related compounds (oxocarboxylic acids and α-dicarbonyls) (DCRCs). The total concentration of DCRCs was 1050±580 and 1040±490ng m-3 during the day and night, respectively. Although these concentrations were about 2 times lower than similar measurements in 2006, the concentrations reported here were about 1-13 times higher than previous measurements in other major cities in the world. Molecular distributions of DCRCs revealed that oxalic acid (C2) was the dominant species (50%), followed by succinic acid (C4) (12%) and malonic acid (C3) (8%). WRF modeling revealed that Mt. Tai was mostly in the free troposphere during the campaign and long-range transport was a major factor governing the distributions of the measured compounds at Mt. Tai. A majority of the samples (79%) had comparable concentrations during the day and night, with their day-night concentration ratios between 0.9 and 1.1. Multi-day transport was considered an important reason for the similar concentrations. Correlation analyses of DCRCs and their gas precursors and between C2 and sulfate indicated precursor emissions and aqueous-phase oxidations during long-range transport also likely play an important role, especially during the night. Source identification indicated that anthropogenic activities followed by photochemical aging accounted for about 60% of the total variance and were the dominant source at Mt. Tai. However, biomass burning was only important during the first half of the measurement period. Measurements of potassium (K+) and DCRCs were about 2 times higher than those from the second half of the measurement period. The concentration of levoglucosan, a biomass burning tracer, decreased by about 80% between 2006 and 2014, indicating that biomass burning may have decreased between 2006 and 2014.
- ItemHeterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: Roles of aerosol water content and chemical composition(Katlenburg-Lindau : EGU, 2018) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Wang, Weihao; Wang, Xinfeng; Lu, Keding; Ma, Nan; Yan, Chao; Kecorius, Simonas; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoHeterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (γ(N2O5)) and ClNO2 production yield (ϕ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined γ(N2O5) and ϕ values varied greatly, with an average of 0.022 for γ(N2O5) (±0.012, standard deviation) and 0.34 for ϕ (±0.28, standard deviation). The variations in γ(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived ϕ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for γ(N2O5) and ϕ to accurately assess photochemical and haze pollution.