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Molecular understanding of new-particle formation from $\alpha$-pinene between −50 and +25 °C - CERN Document Server

<!DOCTYPE html PUBLIC "-//W3C//DTD XHTML 1.0 Transitional//EN" "http://www.w3.org/TR/xhtml1/DTD/xhtml1-transitional.dtd"> <!--[if IEMobile 7]><html class="iem7" xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en" xmlns:og="http://ogp.me/ns#" xmlns:fb="http://ogp.me/ns/fb#"><![endif]--> <!--[if lte IE 6]><html class="ie6 ie6-7 ie6-8" xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en" xmlns:og="http://ogp.me/ns#" xmlns:fb="http://ogp.me/ns/fb#"><![endif]--> <!--[if (IE 7)&(!IEMobile)]><html class="ie7 ie6-7 ie6-8" xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en" xmlns:og="http://ogp.me/ns#" xmlns:fb="http://ogp.me/ns/fb#"><![endif]--> <!--[if IE 8]><html class="ie8 ie6-8" xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en" xmlns:og="http://ogp.me/ns#" xmlns:fb="http://ogp.me/ns/fb#"><![endif]--> <!--[if (gte IE 9)|(gt IEMobile 7)]><!--><html xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en" xmlns:og="http://ogp.me/ns#" xmlns:fb="http://ogp.me/ns/fb#"><!--<![endif]--> <head> <title>Molecular understanding of new-particle formation from $\alpha$-pinene between −50 and +25 °C - CERN Document Server</title> <link href='https://framework.web.cern.ch/framework/2.0/fonts/PTSansWeb/PTSansWeb.css' rel='stylesheet' type='text/css' /> <link rel="stylesheet" href="https://cds.cern.ch/img/invenio.css?v=20141127" type="text/css" /> <link rel="stylesheet" href="https://cds.cern.ch/img/cern_theme/css/cern_theme.css?v=20141127" type="text/css" /> <link rel="stylesheet"href="/css/font-awesome.min.css"> <meta http-equiv="X-UA-Compatible" content="IE=Edge"/> <link rel="stylesheet" href="https://cds.cern.ch/img/cern_toolbar/css/toolbar.css" type="text/css" /> <!--[if lt IE 8]> <link href="https://cds.cern.ch/img/cern_toolbar/css/toolbar-ie.css" rel="stylesheet" type="text/css"> <![endif]--> <!--[if lt IE 8]> <link rel="stylesheet" type="text/css" href="https://cds.cern.ch/img/invenio-ie7.css" /> <![endif]--> <!--[if gt IE 8]> <style type="text/css">div.restrictedflag {filter:none;}</style> <![endif]--> <link rel="canonical" href="https://cds.cern.ch/record/2801559" /> <link rel="alternate" hreflang="el" href="https://cds.cern.ch/record/2801559?ln=el" /> <link rel="alternate" hreflang="fr" href="https://cds.cern.ch/record/2801559?ln=fr" /> <link rel="alternate" hreflang="bg" href="https://cds.cern.ch/record/2801559?ln=bg" /> <link rel="alternate" hreflang="zh-TW" href="https://cds.cern.ch/record/2801559?ln=zh_TW" /> <link rel="alternate" hreflang="pt" href="https://cds.cern.ch/record/2801559?ln=pt" /> <link rel="alternate" hreflang="no" href="https://cds.cern.ch/record/2801559?ln=no" /> <link rel="alternate" hreflang="hr" href="https://cds.cern.ch/record/2801559?ln=hr" /> <link rel="alternate" hreflang="ca" href="https://cds.cern.ch/record/2801559?ln=ca" /> <link rel="alternate" hreflang="de" href="https://cds.cern.ch/record/2801559?ln=de" /> <link rel="alternate" hreflang="it" href="https://cds.cern.ch/record/2801559?ln=it" /> <link rel="alternate" hreflang="zh-CN" href="https://cds.cern.ch/record/2801559?ln=zh_CN" /> <link rel="alternate" hreflang="sv" href="https://cds.cern.ch/record/2801559?ln=sv" /> <link rel="alternate" hreflang="sk" href="https://cds.cern.ch/record/2801559?ln=sk" /> <link rel="alternate" hreflang="en" href="https://cds.cern.ch/record/2801559?ln=en" /> <link rel="alternate" hreflang="pl" href="https://cds.cern.ch/record/2801559?ln=pl" /> <link rel="alternate" hreflang="ru" href="https://cds.cern.ch/record/2801559?ln=ru" /> <link rel="alternate" hreflang="ka" href="https://cds.cern.ch/record/2801559?ln=ka" /> <link rel="alternate" hreflang="ja" href="https://cds.cern.ch/record/2801559?ln=ja" /> <link rel="alternate" hreflang="es" href="https://cds.cern.ch/record/2801559?ln=es" /> <link rel="alternate" type="application/rss+xml" title="CERN Document Server RSS" href="/rss?ln=en" /> <link rel="search" type="application/opensearchdescription+xml" href="https://cds.cern.ch/opensearchdescription" title="CERN Document Server" /> <link rel="unapi-server" type="application/xml" title="unAPI" href="https://cds.cern.ch/unapi" /> <link rel="apple-touch-icon" href="/apple-touch-icon.png"/> <link rel="apple-touch-icon-precomposed" href="/apple-touch-icon-precomposed.png"/> <meta http-equiv="Content-Type" content="text/html; charset=utf-8" /> <meta http-equiv="Content-Language" content="en" /> <meta name="description" content="Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth’s climate. HOMs are formed by rapid, gasphase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ◦C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ◦C to 0.7 % at −50 ◦C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ◦C compared with 25 ◦C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations. Simon, Mario; Dada, Lubna; Heinritzi, Martin; Scholz, Wiebke; Stolzenburg, Dominik; Fischer, Lukas; Wagner, Andrea C; Kürten, Andreas; Rörup, Birte; He, Xu-Cheng; Almeida, João; Baalbaki, Rima; Baccarini, Andrea; Bauer, Paulus S; Beck, Lisa; Bergen, Anton; Bianchi, Federico; Bräkling, Steffen; Brilke, Sophia; Caudillo, Lucia; Chen, Dexian; Chu, Biwu; Dias, António; Draper, Danielle C; Duplissy, Jonathan; El-Haddad, Imad; Finkenzeller, Henning; Frege, Carla; Gonzalez-Carracedo, Loic; Gordon, Hamish; Granzin, Manuel; Hakala, Jani; Hofbauer, Victoria; Hoyle, Christopher R; Kim, Changhyuk; Kong, Weimeng; Lamkaddam, Houssni; Lee, Chuan P; Lehtipalo, Katrianne; Leiminger, Markus; Mai, Huajun; Manninen, Hanna E; Marie, Guillaume; Marten, Ruby; Mentler, Bernhard; Molteni, Ugo; Nichman, Leonid; Nie, Wei; Ojdanic, Andrea; Onnela, Antti; Partoll, Eva; Petäjä, Tuukka; Pfeifer, Joschka; Philippov, Maxim; Quéléver, Lauriane L J; Ranjithkumar, Ananth; Rissanen, Matti P; Schallhart, Simon; Schobesberger, Siegfried; Schuchmann, Simone; Shen, Jiali; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Tauber, Christian; Tham, Yee J; Tomé, António R; Vazquez-Pufleau, Miguel; Vogel, Alexander L; Wagner, Robert; Wang, Mingyi; Wang, Dongyu S; Wang, Yonghong; Weber, Stefan K; Wu, Yusheng; Xiao, Mao; Yan, Chao; Ye, Penglin; Ye, Qing; Zauner-Wieczorek, Marcel; Zhou, Xueqin; Baltensperger, Urs; Dommen, Josef; Flagan, Richard C; Hansel, Armin; Kulmala, Markku; Volkamer, Rainer; Winkler, Paul M; Worsnop, Douglas R; Donahue, Neil M; Kirkby, Jasper; Curtius, Joachim" /> <meta name="keywords" content="CERN Document Server, WebSearch, CERN Document Server" /> <script type="text/javascript" src="https://cds.cern.ch/js/jquery.min.js"></script> <!-- WebNews CSS library --> <link rel="stylesheet" href="https://cds.cern.ch/img/webnews.css" type="text/css" /> <!-- WebNews JS library --> <script type="text/javascript" src="https://cds.cern.ch/js/webnews.js?v=20131009"></script> <meta 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Chem. Phys." name="citation_journal_title" /> <meta content="20" name="citation_volume" /> <meta content="9183-9207" name="citation_firstpage" /> <meta content="2020" name="citation_publication_date" /> <meta name="citation_online_date" content="2022/02/15"> <meta content="10.5194/acp-20-9183-2020" name="citation_doi" /> <!-- OpenGraph --> <meta content="submitter" property="og:title" /> <meta content="Molecular understanding of new-particle formation from $\alpha$-pinene between −50 and +25 °C" property="og:title" /> <meta content="website" property="og:type" /> <meta content="https://cds.cern.ch/record/2801559" property="og:url" /> <meta content="CERN Document Server" property="og:site_name" /> <meta content="submitter" property="og:description" /> <meta content="Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth’s climate. HOMs are formed by rapid, gasphase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ◦C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ◦C to 0.7 % at −50 ◦C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ◦C compared with 25 ◦C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations." property="og:description" /> <!-- Twitter Card --> <meta content="summary" name="twitter:card" /> <style></style> </head> <body class="CERN32Document32Server search" lang="en"> <!-- toolbar starts --> <div id="cern-toolbar"> <h1><a href="http://cern.ch" title="CERN">CERN <span>Accelerating science</span></a></h1> <ul> <li class="cern-accountlinks"><a class="cern-account" href="https://cds.cern.ch/youraccount/login?ln=en&amp;referer=https%3A//cds.cern.ch/record/2801559" title="Sign in to your CERN account">Sign in</a></li> <li><a class="cern-directory" href="http://cern.ch/directory" title="Search CERN resources and browse the directory">Directory</a></li> </ul> </div> <!-- toolbar ends --> <!-- Nav header starts--> <div role="banner" class="clearfix" id="header"> <div class="header-inner inner"> <hgroup class="clearfix"> <h2 id="site-name"> <a rel="home" title="Home" href="/"><span>CERN Document Server</span></a> </h2> <h3 id="site-slogan">Access articles, reports and multimedia content in HEP</h3> </hgroup><!-- /#name-and-slogan --> <div role="navigation" id="main-navigation" class="cdsmenu"> <h2 class="element-invisible">Main menu</h2><ul class="links inline clearfix"> <li class="menu-386 first active-trail"><a class="active-trail" href="https://cds.cern.ch/?ln=en">Search</a></li> <li class="menu-444 "><a class="" title="" href="https://cds.cern.ch/submit?ln=en">Submit</a></li> <li class="menu-426 "><a class="" href="https://cds.cern.ch/help/?ln=en">Help</a></li> <li class="leaf hassubcdsmenu"> <a hreflang="en" class="header" href="https://cds.cern.ch/youraccount/display?ln=en">Personalize</a> <ul class="subsubcdsmenu"><li><a href="https://cds.cern.ch/youralerts/list?ln=en">Your alerts</a></li><li><a href="https://cds.cern.ch/yourbaskets/display?ln=en">Your baskets</a></li><li><a href="https://cds.cern.ch/yourcomments?ln=en">Your comments</a></li><li><a href="https://cds.cern.ch/youralerts/display?ln=en">Your searches</a></li></ul></li> </ul> </div> </div> </div> <!-- Nav header ends--> <table class="navtrailbox"> <tr> <td class="navtrailboxbody"> <a href="/?ln=en" class="navtrail">Home</a> &gt; Molecular understanding of new-particle formation from $\alpha$-pinene between −50 and +25 °C </td> </tr> </table> </div> <div class="pagebody"><div class="pagebodystripemiddle"> <div class="detailedrecordbox"> <div class="detailedrecordtabs"> <div> <ul class="detailedrecordtabs"><li class="on first"><a href="/record/2801559/?ln=en">Information </a></li><li class="disabled"><a>Files </a></li></ul> <div id="tabsSpacer" style="clear:both;height:0px">&nbsp;</div></div> </div> <div class="detailedrecordboxcontent"> <div class="top-left-folded"></div> <div class="top-right-folded"></div> <div class="inside"> <!--<div style="height:0.1em;">&nbsp;</div> <p class="notopgap">&nbsp;</p>--> <abbr class="unapi-id" title="2801559"></abbr> <style type="text/css"> <!-- ul.detailedrecordtabs li.on a{background-color:#4D94CC;color:#fff !important;border-bottom:1px solid #4D94CC!important;} div.detailedrecordboxcontent {padding-top:0px !important;} --> </style> <table class="formatRecordTableFullWidth" > <tr> <td class="formatRecordHeader" style="background-image: url('https://cds.cern.ch/img/journals.jpg');" colspan="2"> <!--YTD: record may have more than one 690C.a tag--> Article </td> </tr> <script type="text/javascript"> $( document ).ready(function() { $('.showAuthor').on('click', function() { var author = '<p>' + $(this).data('name') + '</p>'; var affiliation = $(this).data('affiliation') + '</br>'; var contribution = $(this).data('contribution') + '</br>'; $.magnificPopup.open({ items: { src: '<div id="ovelary-mathjax" class="overlay-white oc-content overlay-white-500">' + author + affiliation + contribution + '</div>', type: 'inline' }, callbacks: { open: function() { var div = document.getElementById("overlay-mathjax") MathJax.Hub.Queue(["Typeset", MathJax.Hub, div]); }, } }) }) }); </script> <tr><td class="formatRecordLabel"> Title </td><td style="padding-left:5px;"><b>Molecular understanding of new-particle formation from $\alpha$-pinene between −50 and +25 °C</b></td></tr> <tr><td class="formatRecordLabel"><span style="white-space:nowrap;"> Author(s) </span> </td><td style="padding-left:5px;"> <script type="text/javascript"> function toggle_authors_visibility(){ var more = document.getElementById('more'); var link = document.getElementById('link'); var extension = document.getElementById('extension'); if (more.style.display=='none'){ more.style.display = ''; extension.style.display = 'none'; link.innerHTML = "Hide" } else { more.style.display = 'none'; extension.style.display = ''; link.innerHTML = "Show all 92 authors" } link.style.color = "rgb(204,0,0);" } function set_up(){ var extension = document.getElementById('extension'); extension.innerHTML = ""; toggle_authors_visibility(); } </script> <a name="show_hide" /><a href="https://cds.cern.ch/search?f=author&amp;p=Simon%2C%20Mario&amp;ln=en">Simon, Mario</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Dada%2C%20Lubna&amp;ln=en">Dada, Lubna</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Heinritzi%2C%20Martin&amp;ln=en">Heinritzi, Martin</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Scholz%2C%20Wiebke&amp;ln=en">Scholz, Wiebke</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Stolzenburg%2C%20Dominik&amp;ln=en">Stolzenburg, Dominik</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Fischer%2C%20Lukas&amp;ln=en">Fischer, Lukas</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wagner%2C%20Andrea%20C&amp;ln=en">Wagner, Andrea C</a> (Frankfurt U. ; U. Colorado, Boulder) ; <a href="https://cds.cern.ch/search?f=author&amp;p=K%C3%BCrten%2C%20Andreas&amp;ln=en">Kürten, Andreas</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=R%C3%B6rup%2C%20Birte&amp;ln=en">Rörup, Birte</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=He%2C%20Xu-Cheng&amp;ln=en">He, Xu-Cheng</a> (Helsinki U.)<span id="more" style=""> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Almeida%2C%20Jo%C3%A3o&amp;ln=en">Almeida, João</a> (CERN ; Lisbon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Baalbaki%2C%20Rima&amp;ln=en">Baalbaki, Rima</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Baccarini%2C%20Andrea&amp;ln=en">Baccarini, Andrea</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Bauer%2C%20Paulus%20S&amp;ln=en">Bauer, Paulus S</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Beck%2C%20Lisa&amp;ln=en">Beck, Lisa</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Bergen%2C%20Anton&amp;ln=en">Bergen, Anton</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Bianchi%2C%20Federico&amp;ln=en">Bianchi, Federico</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Br%C3%A4kling%2C%20Steffen&amp;ln=en">Bräkling, Steffen</a> (Unlisted, CH) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Brilke%2C%20Sophia&amp;ln=en">Brilke, Sophia</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Caudillo%2C%20Lucia&amp;ln=en">Caudillo, Lucia</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Chen%2C%20Dexian&amp;ln=en">Chen, Dexian</a> (Carnegie Mellon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Chu%2C%20Biwu&amp;ln=en">Chu, Biwu</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Dias%2C%20Ant%C3%B3nio&amp;ln=en">Dias, António</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Draper%2C%20Danielle%20C&amp;ln=en">Draper, Danielle C</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Duplissy%2C%20Jonathan&amp;ln=en">Duplissy, Jonathan</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=El-Haddad%2C%20Imad&amp;ln=en">El-Haddad, Imad</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Finkenzeller%2C%20Henning&amp;ln=en">Finkenzeller, Henning</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Frege%2C%20Carla&amp;ln=en">Frege, Carla</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Gonzalez-Carracedo%2C%20Loic&amp;ln=en">Gonzalez-Carracedo, Loic</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Gordon%2C%20Hamish&amp;ln=en">Gordon, Hamish</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Granzin%2C%20Manuel&amp;ln=en">Granzin, Manuel</a> ; <a href="https://cds.cern.ch/search?f=author&amp;p=Hakala%2C%20Jani&amp;ln=en">Hakala, Jani</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Hofbauer%2C%20Victoria&amp;ln=en">Hofbauer, Victoria</a> (Carnegie Mellon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Hoyle%2C%20Christopher%20R&amp;ln=en">Hoyle, Christopher R</a> (PSI, Villigen ; Zurich, ETH) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Kim%2C%20Changhyuk&amp;ln=en">Kim, Changhyuk</a> (Pusan Natl. U. ; Caltech) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Kong%2C%20Weimeng&amp;ln=en">Kong, Weimeng</a> (Caltech) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Lamkaddam%2C%20Houssni&amp;ln=en">Lamkaddam, Houssni</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Lee%2C%20Chuan%20P&amp;ln=en">Lee, Chuan P</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Lehtipalo%2C%20Katrianne&amp;ln=en">Lehtipalo, Katrianne</a> (Helsinki U. ; Finnish Meteorological Inst.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Leiminger%2C%20Markus&amp;ln=en">Leiminger, Markus</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Mai%2C%20Huajun&amp;ln=en">Mai, Huajun</a> (Caltech) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Manninen%2C%20Hanna%20E&amp;ln=en">Manninen, Hanna E</a> (CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Marie%2C%20Guillaume&amp;ln=en">Marie, Guillaume</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Marten%2C%20Ruby&amp;ln=en">Marten, Ruby</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Mentler%2C%20Bernhard&amp;ln=en">Mentler, Bernhard</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Molteni%2C%20Ugo&amp;ln=en">Molteni, Ugo</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Nichman%2C%20Leonid&amp;ln=en">Nichman, Leonid</a> (Manchester U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Nie%2C%20Wei&amp;ln=en">Nie, Wei</a> (Nanjing U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Ojdanic%2C%20Andrea&amp;ln=en">Ojdanic, Andrea</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Onnela%2C%20Antti&amp;ln=en">Onnela, Antti</a> (CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Partoll%2C%20Eva&amp;ln=en">Partoll, Eva</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Pet%C3%A4j%C3%A4%2C%20Tuukka&amp;ln=en">Petäjä, Tuukka</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Pfeifer%2C%20Joschka&amp;ln=en">Pfeifer, Joschka</a> (Frankfurt U. ; CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Philippov%2C%20Maxim&amp;ln=en">Philippov, Maxim</a> (Lebedev Inst.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Qu%C3%A9l%C3%A9ver%2C%20Lauriane%20L%20J&amp;ln=en">Quéléver, Lauriane L J</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Ranjithkumar%2C%20Ananth&amp;ln=en">Ranjithkumar, Ananth</a> (Leeds U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Rissanen%2C%20Matti%20P&amp;ln=en">Rissanen, Matti P</a> (Helsinki U. ; Tampere U. of Tech.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Schallhart%2C%20Simon&amp;ln=en">Schallhart, Simon</a> (Helsinki U. ; Finnish Meteorological Inst.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Schobesberger%2C%20Siegfried&amp;ln=en">Schobesberger, Siegfried</a> (UEF, Kuopio) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Schuchmann%2C%20Simone&amp;ln=en">Schuchmann, Simone</a> (CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Shen%2C%20Jiali&amp;ln=en">Shen, Jiali</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Sipil%C3%A4%2C%20Mikko&amp;ln=en">Sipilä, Mikko</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Steiner%2C%20Gerhard&amp;ln=en">Steiner, Gerhard</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Stozhkov%2C%20Yuri&amp;ln=en">Stozhkov, Yuri</a> (Lebedev Inst.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Tauber%2C%20Christian&amp;ln=en">Tauber, Christian</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Tham%2C%20Yee%20J&amp;ln=en">Tham, Yee J</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Tom%C3%A9%2C%20Ant%C3%B3nio%20R&amp;ln=en">Tomé, António R</a> (Beira Interior U., Covilha) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Vazquez-Pufleau%2C%20Miguel&amp;ln=en">Vazquez-Pufleau, Miguel</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Vogel%2C%20Alexander%20L&amp;ln=en">Vogel, Alexander L</a> (Frankfurt U. ; CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wagner%2C%20Robert&amp;ln=en">Wagner, Robert</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wang%2C%20Mingyi&amp;ln=en">Wang, Mingyi</a> (Carnegie Mellon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wang%2C%20Dongyu%20S&amp;ln=en">Wang, Dongyu S</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wang%2C%20Yonghong&amp;ln=en">Wang, Yonghong</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Weber%2C%20Stefan%20K&amp;ln=en">Weber, Stefan K</a> (CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Wu%2C%20Yusheng&amp;ln=en">Wu, Yusheng</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Xiao%2C%20Mao&amp;ln=en">Xiao, Mao</a> (CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Yan%2C%20Chao&amp;ln=en">Yan, Chao</a> (Helsinki U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Ye%2C%20Penglin&amp;ln=en">Ye, Penglin</a> (Carnegie Mellon U. ; Aerodyne Research, Billerica) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Ye%2C%20Qing&amp;ln=en">Ye, Qing</a> (Carnegie Mellon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Zauner-Wieczorek%2C%20Marcel&amp;ln=en">Zauner-Wieczorek, Marcel</a> (Frankfurt U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Zhou%2C%20Xueqin&amp;ln=en">Zhou, Xueqin</a> (Frankfurt U. ; PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Baltensperger%2C%20Urs&amp;ln=en">Baltensperger, Urs</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Dommen%2C%20Josef&amp;ln=en">Dommen, Josef</a> (PSI, Villigen) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Flagan%2C%20Richard%20C&amp;ln=en">Flagan, Richard C</a> (Caltech) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Hansel%2C%20Armin&amp;ln=en">Hansel, Armin</a> (Innsbruck U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Kulmala%2C%20Markku&amp;ln=en">Kulmala, Markku</a> (Helsinki U. ; Helsinki Inst. of Phys. ; Nanjing U. ; Beijing U. of Chem. Tech.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Volkamer%2C%20Rainer&amp;ln=en">Volkamer, Rainer</a> (U. Colorado, Boulder) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Winkler%2C%20Paul%20M&amp;ln=en">Winkler, Paul M</a> (Vienna U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Worsnop%2C%20Douglas%20R&amp;ln=en">Worsnop, Douglas R</a> (Helsinki U. ; Aerodyne Research, Billerica) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Donahue%2C%20Neil%20M&amp;ln=en">Donahue, Neil M</a> (Carnegie Mellon U.) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Kirkby%2C%20Jasper&amp;ln=en">Kirkby, Jasper</a> (Frankfurt U. ; CERN) ; <a href="https://cds.cern.ch/search?f=author&amp;p=Curtius%2C%20Joachim&amp;ln=en">Curtius, Joachim</a> (Frankfurt U.)</span> <span id="extension"></span> <small><i><a id="link" href="#" onclick="toggle_authors_visibility()" style="color:rgb(204,0,0);"></a></i></small><script type="text/javascript">set_up()</script></td></tr> <tr><td class="formatRecordLabel"> Publication </td><td style="padding-left:5px;">2020</td></tr> <tr><td class="formatRecordLabel"> Number of pages </td><td style="padding-left:5px;">25</td></tr> <tr><td class="formatRecordLabel"> In: </td><td style="padding-left:5px;"><a href="http://dx.doi.org/10.5194/acp-20-9183-2020"><i>Atmos. Chem. Phys.</i> 20 (2020) 9183-9207</a> </a></td></tr> <tr><td class="formatRecordLabel"> DOI </td><td style="padding-left:5px;"><a href="http://dx.doi.org/10.5194/acp-20-9183-2020" title="DOI" target="_blank">10.5194/acp-20-9183-2020</a> <tr><td class="formatRecordLabel"> Subject category </td><td style="padding-left:5px;">Astrophysics and Astronomy ; Chemical Physics and Chemistry</td></tr> <tr><td class="formatRecordLabel"> Accelerator/Facility, Experiment </td><td style="padding-left:5px;"><a href="https://cds.cern.ch/search?p=CLOUD&amp;f=693__a">CLOUD</a></td></tr> <tr><td class="formatRecordLabel"> Abstract </td><td style="padding-left:5px;">Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth’s climate. HOMs are formed by rapid, gasphase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ◦C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ◦C to 0.7 % at −50 ◦C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ◦C compared with 25 ◦C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.</td></tr> <tr><td class="formatRecordLabel"> Copyright/License </td><td style="padding-left:5px;">publication: &copy; 2020-2025 Author(s) (License: <a href="https://creativecommons.org/licenses/by/4.0/">CC-BY-4.0</a>)</td></tr> </table> <br/>Corresponding record in: <a href="http://inspirehep.net/record/2018461">Inspire</a> <small> </small> <br/> <br/><br/><div align="right"><div style="padding-bottom:2px;padding-top:30px;"><span class="moreinfo" style="margin-right:10px;"> <a href="" class="moreinfo">Back to search</a> </span></div></div> <div class="bottom-left-folded"><div class="recordlastmodifiedbox" style="position:relative;margin-left:1px">&nbsp;Record created 2022-02-15, last modified 2022-10-31</div></div> <div class="bottom-right-folded" style="text-align:right;padding-bottom:2px;"> <span class="moreinfo" style="margin-right:10px;"><a href="/search?ln=en&amp;p=recid%3A2801559&amp;rm=wrd" class="moreinfo">Similar records</a></span></div> </div> </div> </div> <br/> <br /> <div class="detailedrecordminipanel"> <div class="top-left"></div><div class="top-right"></div> <div class="inside"> <div id="detailedrecordminipanelfile" style="width:33%;float:left;text-align:center;margin-top:0"> <br/> </div> <div id="detailedrecordminipanelreview" style="width:30%;float:left;text-align:center"> </div> <div id="detailedrecordminipanelactions" style="width:36%;float:right;text-align:right;"> <ul class="detailedrecordactions"> <li><a href="/yourbaskets/add?ln=en&amp;recid=2801559">Add to personal basket</a></li> <li>Export as <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/hx?ln=en">BibTeX</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/hm?ln=en">MARC</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xm?ln=en">MARCXML</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xd?ln=en">DC</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xe?ln=en">EndNote</a>, <!-- <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xe8x?ln=en">EndNote (8-X)</a>,--> <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xn?ln=en">NLM</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2801559/export/xw?ln=en">RefWorks</a> </li> </ul> <div style='padding-left: 13px;'> <!-- JQuery Bookmark Button BEGIN --> <div id="bookmark"></div> <div id="bookmark_sciencewise"></div> <style type="text/css"> #bookmark_sciencewise, #bookmark {float: left;} #bookmark_sciencewise li {padding: 2px; width: 25px;} #bookmark_sciencewise ul, #bookmark ul {list-style-image: none;} </style> <script type="text/javascript" src="/js/jquery.bookmark.min.js"></script> <style type="text/css">@import "/css/jquery.bookmark.css";</style> <script type="text/javascript">// <![CDATA[ $.bookmark.addSite('sciencewise', 'ScienceWise.info', 'https://cds.cern.ch/img/sciencewise.png', 'en', 'bookmark', 'http://sciencewise.info/bookmarks/cds:2801559/add'); $('#bookmark_sciencewise').bookmark({sites: ['sciencewise']}); $('#bookmark').bookmark({ sites: ['facebook', 'twitter', 'linkedin', 'google_plusone'], icons: '/img/bookmarks.png', url: 'https://cds.cern.ch/record/2801559', addEmail: true, title: "Molecular understanding of new-particle formation from $\\alpha$-pinene between \u221250 and +25\u2009\u00b0C", description: "Highly oxygenated organic molecules (HOMs)\ncontribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human\nhealth and Earth\u2019s climate. HOMs are formed by rapid, gasphase autoxidation of volatile organic compounds (VOCs)\nsuch as \u03b1-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs\ncan play an important role in new-particle formation (NPF)\nand the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds\nsuch as sulfuric acid. Both the autoxidation reaction forming\nHOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both\neffects are limited. Dedicated experiments were performed at\nthe CLOUD (Cosmics Leaving OUtdoor Droplets) chamber\nat CERN to address this question. In this study, we show that\na decrease in temperature (from +25 to \u221250 \u25e6C) results in a\nreduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially.\nMeasurements with two different chemical ionization mass\nspectrometers (using nitrate and protonated water as reagent\nion, respectively) provide the molecular composition of the\ngaseous oxidation products, and a two-dimensional volatility\nbasis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 %\nat 25 \u25e6C to 0.7 % at \u221250 \u25e6C. However, there is a strong reduction of the saturation vapor pressure of each oxidation\nstate as the temperature is reduced. Overall, the reduction in\nvolatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at \u221250 \u25e6C compared with 25 \u25e6C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature,\nsince the neutral molecular clusters have increased stability\nagainst evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF\nat the molecular level. Our measurements, therefore, improve\nour understanding of pure biogenic NPF for a wide range of\ntropospheric temperatures and precursor concentrations." }); // ]]> </script> <!-- JQuery Bookmark Button END --> </div> </div> <div style="clear:both;margin-bottom: 0;"></div> </div> <div class="bottom-left"></div><div class="bottom-right"></div> </div> </div></div> <footer id="footer" class="pagefooter clearfix"> <!-- replaced page footer --> <div class="pagefooterstripeleft"> CERN Document Server&nbsp;::&nbsp;<a class="footer" href="https://cds.cern.ch/?ln=en">Search</a>&nbsp;::&nbsp;<a class="footer" href="https://cds.cern.ch/submit?ln=en">Submit</a>&nbsp;::&nbsp;<a class="footer" href="https://cds.cern.ch/youraccount/display?ln=en">Personalize</a>&nbsp;::&nbsp;<a class="footer" href="https://cds.cern.ch/help/?ln=en">Help</a>&nbsp;::&nbsp;<a class="footer" href="https://cern.service-now.com/service-portal?id=privacy_policy&se=CDS-Service" target="_blank">Privacy Notice</a>&nbsp;::&nbsp;<a class="footer" href="https://repository.cern/content-policy" target="_blank">Content Policy</a>&nbsp;::&nbsp;<a class="footer" href="https://repository.cern/terms" target="_blank">Terms and Conditions</a> <br /> Powered by <a class="footer" href="http://invenio-software.org/">Invenio</a> <br /> Maintained by <a class="footer" href="https://cern.service-now.com/service-portal?id=service_element&name=CDS-Service">CDS Service</a> - Need help? 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