Size-Dependent Nascent Sea Spray Aerosol Bounce Fractions and Estimated Viscosity: The Role of Divalent Cation Enrichment, Surface Tension, and the Kelvin Effect
Viscosity, or the “thickness,” of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. This research explored the relationship between particle size and vis...
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creator | Tumminello, Paul R. Niles, Renee Valdez, Vanessa Madawala, Chamika K. Gamage, Dilini K. Kimble, Ke’La A. Leibensperger, Raymond J. Huang, Chunxu Kaluarachchi, Chathuri Dinasquet, Julie Malfatti, Francesca Lee, Christopher Deane, Grant B. Stokes, M. Dale Stone, Elizabeth Tivanski, Alexei Prather, Kimberly A. Boor, Brandon E. Slade, Jonathan H. |
description | Viscosity, or the “thickness,” of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. This research explored the relationship between particle size and viscosity of authentic SSA particles through particle bounce, atomic force microscopy analysis, and predictive viscosity modeling from molecular composition. The study found that 40 nm SSA particles had estimated viscosities around 104 Pa·s and bounce fractions three times higher than 100 and 200 nm particles with less than 102 Pa·s at a relative humidity (RH) of 60%. Additional studies revealed the Kelvin effect and particle density, influenced by particle size, have a greater impact on size-dependent bounce fractions than changes in RH across impactor stages. While changes in the level of surfactants can impact particle bounce, the increased viscosity in smaller SSA is attributed to the formation of gel-like phase states caused by cation–organic cross-links between divalent calcium ions and organic anions enriched in the smaller particles. This work shows the smallest gel-like SSA particles observed in the field are highly viscous, which has implications for cloud formation, secondary aerosol growth, and pollutant transport in coastal environments. |
doi_str_mv | 10.1021/acs.est.4c04312 |
format | Article |
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Dale ; Stone, Elizabeth ; Tivanski, Alexei ; Prather, Kimberly A. ; Boor, Brandon E. ; Slade, Jonathan H.</creator><creatorcontrib>Tumminello, Paul R. ; Niles, Renee ; Valdez, Vanessa ; Madawala, Chamika K. ; Gamage, Dilini K. ; Kimble, Ke’La A. ; Leibensperger, Raymond J. ; Huang, Chunxu ; Kaluarachchi, Chathuri ; Dinasquet, Julie ; Malfatti, Francesca ; Lee, Christopher ; Deane, Grant B. ; Stokes, M. Dale ; Stone, Elizabeth ; Tivanski, Alexei ; Prather, Kimberly A. ; Boor, Brandon E. ; Slade, Jonathan H.</creatorcontrib><description>Viscosity, or the “thickness,” of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. This research explored the relationship between particle size and viscosity of authentic SSA particles through particle bounce, atomic force microscopy analysis, and predictive viscosity modeling from molecular composition. The study found that 40 nm SSA particles had estimated viscosities around 104 Pa·s and bounce fractions three times higher than 100 and 200 nm particles with less than 102 Pa·s at a relative humidity (RH) of 60%. Additional studies revealed the Kelvin effect and particle density, influenced by particle size, have a greater impact on size-dependent bounce fractions than changes in RH across impactor stages. While changes in the level of surfactants can impact particle bounce, the increased viscosity in smaller SSA is attributed to the formation of gel-like phase states caused by cation–organic cross-links between divalent calcium ions and organic anions enriched in the smaller particles. This work shows the smallest gel-like SSA particles observed in the field are highly viscous, which has implications for cloud formation, secondary aerosol growth, and pollutant transport in coastal environments.</description><identifier>ISSN: 0013-936X</identifier><identifier>ISSN: 1520-5851</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.4c04312</identifier><identifier>PMID: 39440882</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Aerosols ; Anions ; Atomic force microscopy ; Biogeochemical Cycling ; calcium ; Calcium ions ; cations ; Cations, Divalent ; Chemical composition ; Coastal environments ; crosslinking ; Divalent cations ; ice ; Ice cover ; Ice formation ; Particle density (concentration) ; Particle Size ; Pollutants ; Pollution dispersion ; Pollution transport ; Relative humidity ; Surface Tension ; technology ; Viscosity ; Water absorption ; water uptake</subject><ispartof>Environmental science & technology, 2024-11, Vol.58 (44), p.19666-19678</ispartof><rights>2024 The Authors. Published by American Chemical Society</rights><rights>Copyright American Chemical Society Nov 5, 2024</rights><rights>2024 The Authors. Published by American Chemical Society 2024 The Authors</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-a375t-d852e7a96c04a9943482428ab1f268271c0d9dbd94661fc068ef35017f81695a3</cites><orcidid>0000-0003-2538-3952 ; 0000-0002-1528-2421 ; 0000-0003-1011-4100 ; 0000-0003-0078-141X ; 0000-0002-5026-4229</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.4c04312$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.4c04312$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/39440882$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Tumminello, Paul R.</creatorcontrib><creatorcontrib>Niles, Renee</creatorcontrib><creatorcontrib>Valdez, Vanessa</creatorcontrib><creatorcontrib>Madawala, Chamika K.</creatorcontrib><creatorcontrib>Gamage, Dilini K.</creatorcontrib><creatorcontrib>Kimble, Ke’La A.</creatorcontrib><creatorcontrib>Leibensperger, Raymond J.</creatorcontrib><creatorcontrib>Huang, Chunxu</creatorcontrib><creatorcontrib>Kaluarachchi, Chathuri</creatorcontrib><creatorcontrib>Dinasquet, Julie</creatorcontrib><creatorcontrib>Malfatti, Francesca</creatorcontrib><creatorcontrib>Lee, Christopher</creatorcontrib><creatorcontrib>Deane, Grant B.</creatorcontrib><creatorcontrib>Stokes, M. Dale</creatorcontrib><creatorcontrib>Stone, Elizabeth</creatorcontrib><creatorcontrib>Tivanski, Alexei</creatorcontrib><creatorcontrib>Prather, Kimberly A.</creatorcontrib><creatorcontrib>Boor, Brandon E.</creatorcontrib><creatorcontrib>Slade, Jonathan H.</creatorcontrib><title>Size-Dependent Nascent Sea Spray Aerosol Bounce Fractions and Estimated Viscosity: The Role of Divalent Cation Enrichment, Surface Tension, and the Kelvin Effect</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>Viscosity, or the “thickness,” of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. 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This work shows the smallest gel-like SSA particles observed in the field are highly viscous, which has implications for cloud formation, secondary aerosol growth, and pollutant transport in coastal environments.</description><subject>Aerosols</subject><subject>Anions</subject><subject>Atomic force microscopy</subject><subject>Biogeochemical Cycling</subject><subject>calcium</subject><subject>Calcium ions</subject><subject>cations</subject><subject>Cations, Divalent</subject><subject>Chemical composition</subject><subject>Coastal environments</subject><subject>crosslinking</subject><subject>Divalent cations</subject><subject>ice</subject><subject>Ice cover</subject><subject>Ice formation</subject><subject>Particle density (concentration)</subject><subject>Particle Size</subject><subject>Pollutants</subject><subject>Pollution dispersion</subject><subject>Pollution transport</subject><subject>Relative humidity</subject><subject>Surface Tension</subject><subject>technology</subject><subject>Viscosity</subject><subject>Water absorption</subject><subject>water uptake</subject><issn>0013-936X</issn><issn>1520-5851</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqNkk1vEzEQhlcIREPhzA1Z4lKJbuqP_bB7qUqatogKJBIQt5XjHZOtNnawdyOFf8M_ZZaECJCQOI3ked53PB9J8pzRMaOcnWkTxxC7cWZoJhh_kIxYzmmay5w9TEaUMpEqUXw-Sp7EeE8p5YLKx8mRUFlGpeSj5Pus-QbpFazB1eA68k5HM8QZaDJbB70llxB89C157XtngFwHbbrGu0i0q8k0ds1Kd1CTT000Pjbd9pzMl0A--BaIt-Sq2eh2MJzoQUWmLjRmucKXUzLrg9VoOQcXMXf607FD8VtoNw2y1oLpniaPrG4jPNvH4-Tj9XQ-uU3v3t-8mVzepVqUeZfWMudQalXgJLRSmcgkz7jUC2Z5IXnJDK1VvahVVhTMGlpIsCKnrLSSFSrX4ji52Pmu-8UK6mEKQbfVOmCDYVt53VR_ZlyzrL74TcVYjoWkRIeTvUPwX3tcS7XCoUDbage-j5VAkEksz_4DZarkmaAloi__Qu99HxyOAikulRRUKKTOdpTBbcUA9vBxRqvhVCo8lWpQ708FFS9-7_fA_7oNBF7tgEF5qPkvux-Fo8pA</recordid><startdate>20241105</startdate><enddate>20241105</enddate><creator>Tumminello, Paul R.</creator><creator>Niles, Renee</creator><creator>Valdez, Vanessa</creator><creator>Madawala, Chamika K.</creator><creator>Gamage, Dilini K.</creator><creator>Kimble, Ke’La A.</creator><creator>Leibensperger, Raymond J.</creator><creator>Huang, Chunxu</creator><creator>Kaluarachchi, Chathuri</creator><creator>Dinasquet, Julie</creator><creator>Malfatti, Francesca</creator><creator>Lee, Christopher</creator><creator>Deane, Grant B.</creator><creator>Stokes, M. 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This research explored the relationship between particle size and viscosity of authentic SSA particles through particle bounce, atomic force microscopy analysis, and predictive viscosity modeling from molecular composition. The study found that 40 nm SSA particles had estimated viscosities around 104 Pa·s and bounce fractions three times higher than 100 and 200 nm particles with less than 102 Pa·s at a relative humidity (RH) of 60%. Additional studies revealed the Kelvin effect and particle density, influenced by particle size, have a greater impact on size-dependent bounce fractions than changes in RH across impactor stages. While changes in the level of surfactants can impact particle bounce, the increased viscosity in smaller SSA is attributed to the formation of gel-like phase states caused by cation–organic cross-links between divalent calcium ions and organic anions enriched in the smaller particles. 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subjects | Aerosols Anions Atomic force microscopy Biogeochemical Cycling calcium Calcium ions cations Cations, Divalent Chemical composition Coastal environments crosslinking Divalent cations ice Ice cover Ice formation Particle density (concentration) Particle Size Pollutants Pollution dispersion Pollution transport Relative humidity Surface Tension technology Viscosity Water absorption water uptake |
title | Size-Dependent Nascent Sea Spray Aerosol Bounce Fractions and Estimated Viscosity: The Role of Divalent Cation Enrichment, Surface Tension, and the Kelvin Effect |
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