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Rapid growth of new atmospheric particles by nitric acid and ammonia condensation

机译：通过硝酸和氨凝结的新型大气颗粒的快速生长

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A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog(1,2), but how it occurs in cities is often puzzling(3). If the growth rates of urban particles are similar to those found in cleaner environments (1-10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below -15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid-base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms(4,5).
机译：作者名单及其附属机构在纸质结束时出现新粒子的形成是城市烟雾的主要贡献者（1,2），但它在城市发生的是往往是令人费解的（3）。如果城市颗粒的增长率与在更清洁环境中发现的那些（每小时1-10纳米）类似，那么现有的理解表明新的城市颗粒应该被高浓度的预先存在的颗粒迅速清除。在这里，我们展示了在CERN的云室中的大气条件下进行的实验，低于约+ 5摄氏度，硝酸和氨蒸汽可以凝结在鲜成核的颗粒上，只有几纳米的直径。此外，当它冷却（低于-15摄氏度）时，硝酸和氨可以直接通过酸碱稳定机制直接成核，以形成硝酸铵颗粒。鉴于这些蒸气通常比硫酸更丰富的千倍，所得颗粒生长速率可以极高，达到每小时100纳米的良好。然而，这些高生长速率要求硝酸盐系统的气体颗粒铵系统超出平衡，以便维持气相过度饱和度。鉴于我们为气相过度衡量的强烈依赖性，我们预计在不均匀的城市环境中发生这种瞬态条件，特别是在冬季，由垂直混合驱动，并且通过交通等强大的本地来源驱动。尽管硝酸和氨凝结的快速增长可能持续几分钟，但尽管如此，它足以通过最小的尺寸范围捕获新鲜成核的颗粒，从而大大增加了它们的存活概率。我们还期望硝酸和氨成核和快速生长在相对清洁和寒冷的上部自由层中重要，其中氨可以与大陆边界层对象，硝酸从电风暴中丰富（4,5）。

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  • 来源
    《Nature》 |2020年第7807期|184-189|共6页
  • 作者

    Wang Mingyi; Kong Weimeng; Marten Ruby; He Xu-Cheng; Chen Dexian; Pfeifer Joschka; Heitto Arto; Kontkanen Jenni; Dada Lubna; Kuerten Andreas; Yli-Juuti Taina; Manninen Hanna E.; Amanatidis Stavros; Amorim Antonio; Baalbaki Rima; Baccarini Andrea; Bell David M.; Bertozzi Barbara; Braekling Steffen; Brilke Sophia; Murillo Lucia Caudillo; Chiu Randall; Chu Biwu; De Menezes Louis-Philippe; Duplissy Jonathan; Finkenzeller Henning; Carracedo Loic Gonzalez; Granzin Manuel; Guida Roberto; Hansel Armin; Hofbauer Victoria; Krechmer Jordan; Lehtipalo Katrianne; Lamkaddam Houssni; Lampimaki Markus; Lee Chuan Ping; Makhmutov Vladimir; Marie Guillaume; Mathot Serge; Mauldin Roy L.; Mentler Bernhard; Mueller Tatjana; Onnela Antti; Partoll Eva; Petaja Tuukka; Philippov Maxim; Pospisilova Veronika; Ranjithkumar Ananth; Rissanen Matti; Rorup Birte; Scholz Wiebke; Shen Jiali; Simon Mario; Sipila Mikko; Steiner Gerhard; Stolzenburg Dominik; Tham Yee Jun; Tome Antonio; Wagner Andrea C.; Wang Dongyu S.; Wang Yonghong; Weber Stefan K.; Winkler Paul M.; Wlasits Peter J.; Wu Yusheng; Xiao Mao; Ye Qing; Zauner-Wieczorek Marcel; Zhou Xueqin; Volkamer Rainer; Riipinen Ilona; Dommen Josef; Curtius Joachim; Baltensperger Urs; Kulmala Markku; Worsnop Douglas R.; Kirkby Jasper; Seinfeld John H.; El-Haddad Imad; Flagan Richard C.; Donahue Neil M.;

  • 作者单位

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem 4400 5th Ave Pittsburgh PA 15213 USA;

    CALTECH Div Chem & Chem Engn Pasadena CA 91125 USA;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem Engn Pittsburgh PA 15213 USA;

    CERN European Org Nucl Res Geneva Switzerland;

    Carnegie Mellon Univ Dept Chem Engn Pittsburgh PA 15213 USA;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    Carnegie Mellon Univ Dept Chem Engn Pittsburgh PA 15213 USA;

    CERN European Org Nucl Res Geneva Switzerland;

    CALTECH Div Chem & Chem Engn Pasadena CA 91125 USA;

    Univ Lisbon CENTRA Lisbon Portugal|Univ Lisbon Fac Ciencias Lisbon Portugal;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Karlsruhe Inst Technol Inst Meteorol & Climate Res Karlsruhe Germany;

    Tofwerk Thun Switzerland;

    Univ Vienna Fac Phys Vienna Austria;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    Univ Colorado Dept Chem Boulder CO 80309 USA|Univ Colorado CIRES Boulder CO 80309 USA;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    CERN European Org Nucl Res Geneva Switzerland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Univ Helsinki Helsinki Inst Phys Helsinki Finland;

    Univ Colorado Dept Chem Boulder CO 80309 USA|Univ Colorado CIRES Boulder CO 80309 USA;

    Univ Vienna Fac Phys Vienna Austria;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    CERN European Org Nucl Res Geneva Switzerland;

    Univ Innsbruck Inst Ion Phys & Appl Phys Innsbruck Austria|Ionicon Analyt Innsbruck Austria;

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem 4400 5th Ave Pittsburgh PA 15213 USA;

    Aerodyne Res Billerica MA USA;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Finnish Meteorol Inst Helsinki Finland;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Russian Acad Sci PN Lebedev Phys Inst Moscow Russia;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    CERN European Org Nucl Res Geneva Switzerland;

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem 4400 5th Ave Pittsburgh PA 15213 USA|Univ Colorado Dept Atmospher & Ocean Sci Boulder CO 80309 USA;

    Univ Innsbruck Inst Ion Phys & Appl Phys Innsbruck Austria;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    CERN European Org Nucl Res Geneva Switzerland;

    Univ Innsbruck Inst Ion Phys & Appl Phys Innsbruck Austria;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Russian Acad Sci PN Lebedev Phys Inst Moscow Russia;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Leeds Sch Earth & Environm Leeds W Yorkshire England;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Tampere Univ Fac Engn & Nat Sci Aerosol Phys Lab Phys Unit Tampere Finland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Univ Innsbruck Inst Ion Phys & Appl Phys Innsbruck Austria|Ionicon Analyt Innsbruck Austria;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Univ Innsbruck Inst Ion Phys & Appl Phys Innsbruck Austria|Grimm Aerosol Techn Ainring Ainring Germany;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Univ Vienna Fac Phys Vienna Austria;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Univ Beira Interior Inst Infante Dom Luiz Covilha Portugal;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany|Univ Colorado Dept Chem Boulder CO 80309 USA|Univ Colorado CIRES Boulder CO 80309 USA;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    CERN European Org Nucl Res Geneva Switzerland;

    Univ Vienna Fac Phys Vienna Austria;

    Univ Vienna Fac Phys Vienna Austria;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem 4400 5th Ave Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Engn & Publ Policy Pittsburgh PA 15213 USA;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Colorado Dept Chem Boulder CO 80309 USA|Univ Colorado CIRES Boulder CO 80309 USA;

    Univ Stockholm Dept Appl Environm Sci Stockholm Sweden;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Univ Helsinki Helsinki Inst Phys Helsinki Finland|Nanjing Univ Joint Int Res Lab Atmospher & Earth Syst Sci Nanjing Peoples R China|Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci & Engn Aerosol & Haze Lab Beijing Peoples R China;

    Univ Helsinki Inst Atmospher & Earth Syst Res INAR Helsinki Finland|Aerodyne Res Billerica MA USA;

    CERN European Org Nucl Res Geneva Switzerland|Goethe Univ Frankfurt Inst Atmospher & Environm Sci Frankfurt Germany;

    CALTECH Div Chem & Chem Engn Pasadena CA 91125 USA;

    Paul Scherrer Inst Lab Atmospher Chem Villigen Switzerland;

    CALTECH Div Chem & Chem Engn Pasadena CA 91125 USA;

    Carnegie Mellon Univ Ctr Atmospher Particle Studies Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem 4400 5th Ave Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Chem Engn Pittsburgh PA 15213 USA|Carnegie Mellon Univ Dept Engn & Publ Policy Pittsburgh PA 15213 USA;

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