Qiaorong Xie, Sepehr Nikkho, Zoë M. Golay, Isaac S. Morton, Emily R. Halpern, Robert VanGundy, Alla Zelenyuk, Manish Shrivastava, Rahul A. Zaveri, Allan K. Bertram and Alexander Laskin*,
{"title":"α-蒎烯与辛烯衍生的二级有机气溶胶的气粒分配和粘度特性","authors":"Qiaorong Xie, Sepehr Nikkho, Zoë M. Golay, Isaac S. Morton, Emily R. Halpern, Robert VanGundy, Alla Zelenyuk, Manish Shrivastava, Rahul A. Zaveri, Allan K. Bertram and Alexander Laskin*, ","doi":"10.1021/acsestair.5c00108","DOIUrl":null,"url":null,"abstract":"<p >Secondary organic aerosols (SOA) have complex, multicomponent composition that controls particle viscosity and gas-particle partitioning, key factors to their atmospheric evolution. This study investigates the chemical composition, volatility and viscosity of SOA formed by ozonolysis of cyclic α-pinene (PSOA) and acyclic ocimene (OSOA) monoterpenes. Using Temperature-Programmed Desorption combined with Direct Analysis in Real-Time ionization and High-Resolution Mass Spectrometry, we determined the molecular composition and saturation mass concentration of individual SOA constituents. These data enabled gas-particle partitioning and viscosity estimates under varied atmospheric conditions. PSOA, composed of higher molecular weight and less oxidized species, shows higher condensability and viscosity under high total organic mass (<i>tOM</i>) loadings. In contrast, OSOA, consisting of more oxidized, lower molecular weight species, exhibits greater sensitivity to <i>tOM</i>, with viscosity increasing significantly upon dilution. Poke-flow experiments support this trend, indicating that OSOA undergoes more dynamic compositional and phase changes during atmospheric aging. These observations reveal distinct dynamic trends in the atmospheric transformations and reactivity of SOA from cyclic and acyclic monoterpenes, with the latter showing greater compositional changes during aging that alter viscosity and diffusion. This highlights the importance of incorporating such dynamic transformations into atmospheric models to improve predictions of SOA atmospheric loadings, lifetimes, and impacts.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 9","pages":"1916–1926"},"PeriodicalIF":0.0000,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Distinct Gas-Particle Partitioning and Viscosity Characteristics of Secondary Organic Aerosols Derived from α-Pinene versus Ocimene\",\"authors\":\"Qiaorong Xie, Sepehr Nikkho, Zoë M. Golay, Isaac S. Morton, Emily R. Halpern, Robert VanGundy, Alla Zelenyuk, Manish Shrivastava, Rahul A. Zaveri, Allan K. Bertram and Alexander Laskin*, \",\"doi\":\"10.1021/acsestair.5c00108\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Secondary organic aerosols (SOA) have complex, multicomponent composition that controls particle viscosity and gas-particle partitioning, key factors to their atmospheric evolution. This study investigates the chemical composition, volatility and viscosity of SOA formed by ozonolysis of cyclic α-pinene (PSOA) and acyclic ocimene (OSOA) monoterpenes. Using Temperature-Programmed Desorption combined with Direct Analysis in Real-Time ionization and High-Resolution Mass Spectrometry, we determined the molecular composition and saturation mass concentration of individual SOA constituents. These data enabled gas-particle partitioning and viscosity estimates under varied atmospheric conditions. PSOA, composed of higher molecular weight and less oxidized species, shows higher condensability and viscosity under high total organic mass (<i>tOM</i>) loadings. In contrast, OSOA, consisting of more oxidized, lower molecular weight species, exhibits greater sensitivity to <i>tOM</i>, with viscosity increasing significantly upon dilution. Poke-flow experiments support this trend, indicating that OSOA undergoes more dynamic compositional and phase changes during atmospheric aging. These observations reveal distinct dynamic trends in the atmospheric transformations and reactivity of SOA from cyclic and acyclic monoterpenes, with the latter showing greater compositional changes during aging that alter viscosity and diffusion. This highlights the importance of incorporating such dynamic transformations into atmospheric models to improve predictions of SOA atmospheric loadings, lifetimes, and impacts.</p>\",\"PeriodicalId\":100014,\"journal\":{\"name\":\"ACS ES&T Air\",\"volume\":\"2 9\",\"pages\":\"1916–1926\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-08-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS ES&T Air\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsestair.5c00108\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS ES&T Air","FirstCategoryId":"1085","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsestair.5c00108","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Distinct Gas-Particle Partitioning and Viscosity Characteristics of Secondary Organic Aerosols Derived from α-Pinene versus Ocimene
Secondary organic aerosols (SOA) have complex, multicomponent composition that controls particle viscosity and gas-particle partitioning, key factors to their atmospheric evolution. This study investigates the chemical composition, volatility and viscosity of SOA formed by ozonolysis of cyclic α-pinene (PSOA) and acyclic ocimene (OSOA) monoterpenes. Using Temperature-Programmed Desorption combined with Direct Analysis in Real-Time ionization and High-Resolution Mass Spectrometry, we determined the molecular composition and saturation mass concentration of individual SOA constituents. These data enabled gas-particle partitioning and viscosity estimates under varied atmospheric conditions. PSOA, composed of higher molecular weight and less oxidized species, shows higher condensability and viscosity under high total organic mass (tOM) loadings. In contrast, OSOA, consisting of more oxidized, lower molecular weight species, exhibits greater sensitivity to tOM, with viscosity increasing significantly upon dilution. Poke-flow experiments support this trend, indicating that OSOA undergoes more dynamic compositional and phase changes during atmospheric aging. These observations reveal distinct dynamic trends in the atmospheric transformations and reactivity of SOA from cyclic and acyclic monoterpenes, with the latter showing greater compositional changes during aging that alter viscosity and diffusion. This highlights the importance of incorporating such dynamic transformations into atmospheric models to improve predictions of SOA atmospheric loadings, lifetimes, and impacts.