Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation
New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)(1-4). However, the precursorvapoursthat drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we showthat ni...
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Language: | English |
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Nature Publishing Group
2022
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Online Access: | http://hdl.handle.net/10138/347174 |
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HELDA – University of Helsinki Open Repository |
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114 Physical sciences |
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114 Physical sciences the MESSy Consortium Wang, Mingyi Xiao, Mao Rörup, Birte He, Xu-Cheng Shen, Jiali Dada, Lubna Baalbaki, Rima Manninen, Hanna E. Brasseur, Zoe Duplissy, Jonathan Korhonen, Kimmo Lehtipalo, Katrianne Onnela, Antti Petäjä, Tuukka Piedehierro, Ana A. Schobesberger, Siegfried Welti, Andre Wu, Yusheng Sipilä, Mikko Kulmala, Markku Riipinen, Ilona Worsnop, Douglas R. Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
topic_facet |
114 Physical sciences |
description |
New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)(1-4). However, the precursorvapoursthat drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we showthat nitric acid, sulfuric acid and ammonia form particles synergistically, at ratesthat are orders of magnitude faster than those from any two ofthe three components. The importance ofthis mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the uppertroposphere overthe Asian monsoon region(5,6). Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements showthat these CCN are also highly efficient ice nucleating particles-comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3-H2SO4-NH3 nucleation in the uppertroposphere and producing ice nucleating particles that spread acrossthe mid-latitude Northern Hemisphere. Peer reviewed |
author2 |
Institute for Atmospheric and Earth System Research (INAR) Polar and arctic atmospheric research (PANDA) Air quality research group Helsinki Institute of Physics Department of Physics |
format |
Article in Journal/Newspaper |
author |
the MESSy Consortium Wang, Mingyi Xiao, Mao Rörup, Birte He, Xu-Cheng Shen, Jiali Dada, Lubna Baalbaki, Rima Manninen, Hanna E. Brasseur, Zoe Duplissy, Jonathan Korhonen, Kimmo Lehtipalo, Katrianne Onnela, Antti Petäjä, Tuukka Piedehierro, Ana A. Schobesberger, Siegfried Welti, Andre Wu, Yusheng Sipilä, Mikko Kulmala, Markku Riipinen, Ilona Worsnop, Douglas R. |
author_facet |
the MESSy Consortium Wang, Mingyi Xiao, Mao Rörup, Birte He, Xu-Cheng Shen, Jiali Dada, Lubna Baalbaki, Rima Manninen, Hanna E. Brasseur, Zoe Duplissy, Jonathan Korhonen, Kimmo Lehtipalo, Katrianne Onnela, Antti Petäjä, Tuukka Piedehierro, Ana A. Schobesberger, Siegfried Welti, Andre Wu, Yusheng Sipilä, Mikko Kulmala, Markku Riipinen, Ilona Worsnop, Douglas R. |
author_sort |
the MESSy Consortium |
title |
Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
title_short |
Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
title_full |
Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
title_fullStr |
Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
title_full_unstemmed |
Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation |
title_sort |
synergistic hno3-h2so4-nh3 upper tropospheric particle formation |
publisher |
Nature Publishing Group |
publishDate |
2022 |
url |
http://hdl.handle.net/10138/347174 |
genre |
Arctic |
genre_facet |
Arctic |
op_relation |
10.1038/s41586-022-04605-4 We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources. This research has received funding from the US National Science Foundation (nos. AGS-1801574, AGS-1801897, AGS-1602086, AGS-1801329, AGS-2132089 and AGS-1801280), the European Union's Horizon 2020 programme (Marie Sklodowska-Curie ITN no. 764991 'CLOUD-MOTION'), the European Commission, H2020 Research Infrastructures (FORCeS, no. 821205), the European Union's Horizon 2020 research and innovation programme (Marie Sklodowska-Curie no. 895875 'NPF-PANDA'), a European Research Council (ERC) project ATM-GTP contract (no. 742206), an ERC-CoG grant INTEGRATE (no. 867599), the Swiss National Science Foundation (nos. 200021_169090, 200020_172602 and 20FI20_172622), the Academy of Finland ACCC Flagship (no. 337549), the Academy of Finland Academy professorship (no. 302958), the Academy of Finland (nos. 1325656, 316114 and 325647), Russian MegaGrant project 'Megapolis - heat and pollution island: interdisciplinary hydroclimatic, geochemical and ecological analysis' (application reference 2020-220-08-5835), Jane and Aatos Erkko Foundation 'Quantifying carbon sink, CarbonSink+ and their interaction with air quality' INAR project, Samsung PM2.5 SRP, Prince Albert Foundation 'the Arena for the gap analysis of the existing Arctic Science Co-Operations (AASCO)' (no. 2859), the German Federal Ministry of Education and Research (CLOUD-16 project nos. 01LK1601A and 01LK1601C), the Knut and Alice Wallenberg Foundation Wallenberg Academy Fellows project AtmoRemove (no. 2015.0162), the Portuguese Foundation for Science and Technology (no. CERN/FIS-COM/0014/2017) and the Technology Transfer Project N059 of the Karlsruhe Institute of Technology (KIT). The FIGAERO-CIMS was supported by a Major Research Instrumentation (MRI) grant for the US NSF AGS-1531284, as well as the Wallace Research Foundation. The computations by R.Bardakov were performed on resources provided by the Swedish National Infrastructure for Computing (SNIC) at the National Supercomputer Center (NSC). I.R. thanks the Max Planck Society for a sabbatical award. M.W. thanks Siebel Scholars Foundation for financial support. the MESSy Consortium , Wang , M , Xiao , M , Rörup , B , He , X-C , Shen , J , Dada , L , Baalbaki , R , Manninen , H E , Brasseur , Z , Duplissy , J , Korhonen , K , Lehtipalo , K , Onnela , A , Petäjä , T , Piedehierro , A A , Schobesberger , S , Welti , A , Wu , Y , Sipilä , M , Kulmala , M , Riipinen , I & Worsnop , D R 2022 , ' Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation ' , Nature , vol. 605 , no. 7910 , pp. 483-+ . https://doi.org/10.1038/s41586-022-04605-4 ORCID: /0000-0002-1881-9044/work/117943270 ORCID: /0000-0002-1660-2706/work/117943695 ORCID: /0000-0002-8594-7003/work/117943984 ORCID: /0000-0002-4480-2107/work/117948056 ORCID: /0000-0003-1105-9043/work/117948478 ORCID: /0000-0001-5387-018X/work/117949623 ORCID: /0000-0002-7416-306X/work/156151984 http://hdl.handle.net/10138/347174 01763078-63d3-4b5c-855f-0afddc014937 35585346 85130214705 000797641900024 |
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cc_by info:eu-repo/semantics/openAccess openAccess |
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ftunivhelsihelda:oai:helda.helsinki.fi:10138/347174 2024-04-21T07:54:28+00:00 Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation the MESSy Consortium Wang, Mingyi Xiao, Mao Rörup, Birte He, Xu-Cheng Shen, Jiali Dada, Lubna Baalbaki, Rima Manninen, Hanna E. Brasseur, Zoe Duplissy, Jonathan Korhonen, Kimmo Lehtipalo, Katrianne Onnela, Antti Petäjä, Tuukka Piedehierro, Ana A. Schobesberger, Siegfried Welti, Andre Wu, Yusheng Sipilä, Mikko Kulmala, Markku Riipinen, Ilona Worsnop, Douglas R. Institute for Atmospheric and Earth System Research (INAR) Polar and arctic atmospheric research (PANDA) Air quality research group Helsinki Institute of Physics Department of Physics 2022-08-22T14:03:10Z 23 application/pdf http://hdl.handle.net/10138/347174 eng eng Nature Publishing Group 10.1038/s41586-022-04605-4 We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources. This research has received funding from the US National Science Foundation (nos. AGS-1801574, AGS-1801897, AGS-1602086, AGS-1801329, AGS-2132089 and AGS-1801280), the European Union's Horizon 2020 programme (Marie Sklodowska-Curie ITN no. 764991 'CLOUD-MOTION'), the European Commission, H2020 Research Infrastructures (FORCeS, no. 821205), the European Union's Horizon 2020 research and innovation programme (Marie Sklodowska-Curie no. 895875 'NPF-PANDA'), a European Research Council (ERC) project ATM-GTP contract (no. 742206), an ERC-CoG grant INTEGRATE (no. 867599), the Swiss National Science Foundation (nos. 200021_169090, 200020_172602 and 20FI20_172622), the Academy of Finland ACCC Flagship (no. 337549), the Academy of Finland Academy professorship (no. 302958), the Academy of Finland (nos. 1325656, 316114 and 325647), Russian MegaGrant project 'Megapolis - heat and pollution island: interdisciplinary hydroclimatic, geochemical and ecological analysis' (application reference 2020-220-08-5835), Jane and Aatos Erkko Foundation 'Quantifying carbon sink, CarbonSink+ and their interaction with air quality' INAR project, Samsung PM2.5 SRP, Prince Albert Foundation 'the Arena for the gap analysis of the existing Arctic Science Co-Operations (AASCO)' (no. 2859), the German Federal Ministry of Education and Research (CLOUD-16 project nos. 01LK1601A and 01LK1601C), the Knut and Alice Wallenberg Foundation Wallenberg Academy Fellows project AtmoRemove (no. 2015.0162), the Portuguese Foundation for Science and Technology (no. CERN/FIS-COM/0014/2017) and the Technology Transfer Project N059 of the Karlsruhe Institute of Technology (KIT). The FIGAERO-CIMS was supported by a Major Research Instrumentation (MRI) grant for the US NSF AGS-1531284, as well as the Wallace Research Foundation. The computations by R.Bardakov were performed on resources provided by the Swedish National Infrastructure for Computing (SNIC) at the National Supercomputer Center (NSC). I.R. thanks the Max Planck Society for a sabbatical award. M.W. thanks Siebel Scholars Foundation for financial support. the MESSy Consortium , Wang , M , Xiao , M , Rörup , B , He , X-C , Shen , J , Dada , L , Baalbaki , R , Manninen , H E , Brasseur , Z , Duplissy , J , Korhonen , K , Lehtipalo , K , Onnela , A , Petäjä , T , Piedehierro , A A , Schobesberger , S , Welti , A , Wu , Y , Sipilä , M , Kulmala , M , Riipinen , I & Worsnop , D R 2022 , ' Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation ' , Nature , vol. 605 , no. 7910 , pp. 483-+ . https://doi.org/10.1038/s41586-022-04605-4 ORCID: /0000-0002-1881-9044/work/117943270 ORCID: /0000-0002-1660-2706/work/117943695 ORCID: /0000-0002-8594-7003/work/117943984 ORCID: /0000-0002-4480-2107/work/117948056 ORCID: /0000-0003-1105-9043/work/117948478 ORCID: /0000-0001-5387-018X/work/117949623 ORCID: /0000-0002-7416-306X/work/156151984 http://hdl.handle.net/10138/347174 01763078-63d3-4b5c-855f-0afddc014937 35585346 85130214705 000797641900024 cc_by info:eu-repo/semantics/openAccess openAccess 114 Physical sciences Article publishedVersion 2022 ftunivhelsihelda 2024-03-27T17:51:23Z New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)(1-4). However, the precursorvapoursthat drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we showthat nitric acid, sulfuric acid and ammonia form particles synergistically, at ratesthat are orders of magnitude faster than those from any two ofthe three components. The importance ofthis mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the uppertroposphere overthe Asian monsoon region(5,6). Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements showthat these CCN are also highly efficient ice nucleating particles-comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3-H2SO4-NH3 nucleation in the uppertroposphere and producing ice nucleating particles that spread acrossthe mid-latitude Northern Hemisphere. Peer reviewed Article in Journal/Newspaper Arctic HELDA – University of Helsinki Open Repository |