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Article ; Online: Heterogeneous Nucleation of Supersaturated Water Vapor onto Sub-10 nm Nanoplastic Particles.

Wlasits, Peter J / Konrat, Ruth / Winkler, Paul M

Environmental science & technology

2023 Volume 57, Issue 4, Page(s) 1584–1591

Abstract: Nanoplastic pollution by atmospheric transport processes is a recently discovered environmental problem on a global scale that is attributed to the dispersion of aerosolized nanoplastics. However, knowledge about the basic physicochemical properties of ... ...

Abstract	Nanoplastic pollution by atmospheric transport processes is a recently discovered environmental problem on a global scale that is attributed to the dispersion of aerosolized nanoplastics. However, knowledge about the basic physicochemical properties of aerosol nanoplastic particles is scarce. Here, we present experiments on the heterogeneous nucleation of supersaturated water vapor onto sub-10 nm polyethylene terephthalate (PET) seeds. We determined onset saturation ratios for the activation of PET seeds in comparison to the well-documented reference system of silver particles, resulting in lower onset saturation ratios of the PET seeds compared to silver seeds. By using different PET bulk materials for the generation of nanoparticles, we report a strong material dependence of the onset saturation ratios, pointing to a strong effect of additives from commodity plastics in heterogeneous nucleation. Moreover, our results show a strong dependence on nucleation temperature that might be of immediate atmospheric relevance. Our work can be considered as an initial step in airborne nanoplastic detection by condensation techniques, and we anticipate our study to serve as a basis for further research that will eventually allow assessing the impact of nanoplastic dispersion on atmospheric processes.
MeSH term(s)	Microplastics ; Steam ; Silver ; Plastics
Chemical Substances	Microplastics ; Steam ; Silver (3M4G523W1G) ; Plastics
Language	English
Publishing date	2023-01-19
Publishing country	United States
Document type	Journal Article
ISSN	1520-5851
ISSN (online)	1520-5851
DOI	10.1021/acs.est.2c07643
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: A unifying identity for the work of cluster formation in heterogeneous and homogeneous nucleation theory.

McGraw, Robert L / Winkler, Paul M / Wagner, Paul E

The Journal of chemical physics

2018 Volume 149, Issue 8, Page(s) 84702

Abstract: A unifying identity is derived relating the reversible work of cluster formation (W) and its molecular number content (n) and surface work (Φ) components, each ratioed to the corresponding values for a spherical capillary drop of critical size in ... ...

Abstract	A unifying identity is derived relating the reversible work of cluster formation (W) and its molecular number content (n) and surface work (Φ) components, each ratioed to the corresponding values for a spherical capillary drop of critical size in classical nucleation theory. The result is a relationship that connects these ratios:
Language	English
Publishing date	2018-09-11
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/1.5040459
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Article ; Online: Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale.

McGraw, Robert L / Winkler, Paul M / Wagner, Paul E

Scientific reports

2017 Volume 7, Issue 1, Page(s) 16896

Abstract: A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. ...

Abstract	A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. Temperature dependence is correlated with cluster stabilization by the nanoparticle seed and previously found cases of unusual increasing nucleation onset saturation ratio with increasing temperature are explained. A necessary condition for the unusual positive temperature dependence is identified, namely that the critical cluster be more stable, on a per molecule basis, than the bulk liquid to exhibit the effect. Temperature dependence is next examined in the classical Fletcher model, modified here to make the energy of cluster formation explicit in the model. The contact angle used in the Fletcher model is identified as the microscopic contact angle, which can be directly obtained from heterogeneous nucleation experimental data by a recently developed analysis method. Here an equivalent condition, increasing contact angle with temperature, is found necessary for occurrence of unusual temperature dependence. Our findings have immediate applications to atmospheric particle formation and nanoparticle detection in condensation particle counters (CPCs).
Language	English
Publishing date	2017-12-04
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	2615211-3
ISSN	2045-2322 ; 2045-2322
ISSN (online)	2045-2322
ISSN	2045-2322
DOI	10.1038/s41598-017-16692-9
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Article ; Online: Robust metric for quantifying the importance of stochastic effects on nanoparticle growth.

Olenius, Tinja / Pichelstorfer, Lukas / Stolzenburg, Dominik / Winkler, Paul M / Lehtinen, Kari E J / Riipinen, Ilona

Scientific reports

2018 Volume 8, Issue 1, Page(s) 14160

Abstract: Comprehensive representation of nanoparticle dynamics is necessary for understanding nucleation and growth phenomena. This is critical in atmospheric physics, as airborne particles formed from vapors have significant but highly uncertain effects on ... ...

Abstract	Comprehensive representation of nanoparticle dynamics is necessary for understanding nucleation and growth phenomena. This is critical in atmospheric physics, as airborne particles formed from vapors have significant but highly uncertain effects on climate. While the vapor-particle mass exchange driving particle growth can be described by a macroscopic, continuous substance for large enough particles, the growth dynamics of the smallest nanoparticles involve stochastic fluctuations in particle size due to discrete molecular collision and decay processes. To date, there have been no generalizable methods for quantifying the particle size regime where the discrete effects become negligible and condensation models can be applied. By discrete simulations of sub-10 nm particle populations, we demonstrate the importance of stochastic effects in the nanometer size range. We derive a novel, theory-based, simple and robust metric for identifying the exact sizes where these effects cannot be omitted for arbitrary molecular systems. The presented metric, based on examining the second- and first-order derivatives of the particle size distribution function, is directly applicable to experimental size distribution data. This tool enables quantifying the onset of condensational growth without prior information on the properties of the vapors and particles, thus allowing robust experimental resolving of nanoparticle formation physics.
Language	English
Publishing date	2018-09-21
Publishing country	England
Document type	Journal Article
ZDB-ID	2615211-3
ISSN	2045-2322 ; 2045-2322
ISSN (online)	2045-2322
ISSN	2045-2322
DOI	10.1038/s41598-018-32610-z
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Article ; Online: Heterogeneous Nucleation onto Monoatomic Ions: Support for the Kelvin-Thomson Theory.

Tauber, Christian / Chen, Xiaoshuang / Wagner, Paul E / Winkler, Paul M / Hogan, Christopher J / Maißer, Anne

Chemphyschem : a European journal of chemical physics and physical chemistry

2018 Volume 19, Issue 22, Page(s) 3144–3149

Abstract: In this study, the process of heterogeneous nucleation is investigated by coupling a high-resolution differential mobility analyser (DMA) to an expansion-type condensation particle counter, the size-analyzing nuclei counter (SANC). More specifically, we ... ...

Abstract	In this study, the process of heterogeneous nucleation is investigated by coupling a high-resolution differential mobility analyser (DMA) to an expansion-type condensation particle counter, the size-analyzing nuclei counter (SANC). More specifically, we measured the activation probabilities of monoatomic ions of both polarities by using n-butanol as condensing liquid. All seed ions were activated to grow into macroscopic sizes at saturation ratios well below the onset of homogeneous nucleation, showing for the first time that the SANC is capable of detecting sub-nanometer sized, atomic seed ions. The measured onset saturation ratios for each ion were compared to the Kelvin-Thomson (KT) theory. Despite the fact that certain dependencies of activation behaviour on seed ion properties cannot be predicted by the KT theory, it was found that with a simple adjustment of the n-butanol molecular volume (9-15 % lower compared to bulk properties) good agreement with experimental results is achievable. The corresponding density increase may result from the dipole-charge interaction. This study thus offers support for the application of the KT model for heterogeneous, ion-induced nucleation studies at the sub-nanometer level.
Language	English
Publishing date	2018-10-12
Publishing country	Germany
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1439-7641
ISSN (online)	1439-7641
DOI	10.1002/cphc.201800698
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Article: Near-Unity Mass Accommodation Coefficient of Organic Molecules of Varying Structure

Julin, Jan / Winkler, Paul M / Donahue, Neil M / Wagner, Paul E / Riipinen, Ilona

Environmental Science & Technology. 2014 Oct. 21, v. 48, no. 20

2014

Abstract: Atmospheric aerosol particles have a significant effect on global climate, air quality, and consequently human health. Condensation of organic vapors is a key process in the growth of nanometer-sized particles to climate relevant sizes. This growth is ... ...

Abstract	Atmospheric aerosol particles have a significant effect on global climate, air quality, and consequently human health. Condensation of organic vapors is a key process in the growth of nanometer-sized particles to climate relevant sizes. This growth is very sensitive to the mass accommodation coefficient α, a quantity describing the vapor uptake ability of the particles, but knowledge on α of atmospheric organics is lacking. In this work, we have determined α for four organic molecules with diverse structural properties: adipic acid, succinic acid, naphthalene, and nonane. The coefficients are studied using molecular dynamics simulations, complemented with expansion chamber measurements. Our results are consistent with α = 1 (indicating nearly perfect accommodation), regardless of the molecular structural properties, the phase state of the bulk condensed phase, or surface curvature. The results highlight the need for experimental techniques capable of resolving the internal structure of nanoparticles to better constrain the accommodation of atmospheric organics.
Keywords	adipic acid ; aerosols ; air quality ; climate ; human health ; molecular dynamics ; nanoparticles ; naphthalene ; succinic acid ; vapors
Language	English
Dates of publication	2014-1021
Size	p. 12083-12089.
Publishing place	American Chemical Society
Document type	Article
ISSN	1520-5851
DOI	10.1021%2Fes501816h
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Near-unity mass accommodation coefficient of organic molecules of varying structure.

Julin, Jan / Winkler, Paul M / Donahue, Neil M / Wagner, Paul E / Riipinen, Ilona

Environmental science & technology

2014 Volume 48, Issue 20, Page(s) 12083–12089

Abstract	Atmospheric aerosol particles have a significant effect on global climate, air quality, and consequently human health. Condensation of organic vapors is a key process in the growth of nanometer-sized particles to climate relevant sizes. This growth is very sensitive to the mass accommodation coefficient α, a quantity describing the vapor uptake ability of the particles, but knowledge on α of atmospheric organics is lacking. In this work, we have determined α for four organic molecules with diverse structural properties: adipic acid, succinic acid, naphthalene, and nonane. The coefficients are studied using molecular dynamics simulations, complemented with expansion chamber measurements. Our results are consistent with α = 1 (indicating nearly perfect accommodation), regardless of the molecular structural properties, the phase state of the bulk condensed phase, or surface curvature. The results highlight the need for experimental techniques capable of resolving the internal structure of nanoparticles to better constrain the accommodation of atmospheric organics.
MeSH term(s)	Adipates/chemistry ; Aerosols/chemistry ; Alkanes/chemistry ; Climate ; Gases/chemistry ; Humans ; Molecular Dynamics Simulation ; Molecular Weight ; Nanoparticles/chemistry ; Naphthalenes/chemistry ; Particle Size ; Particulate Matter/chemistry ; Succinic Acid/chemistry
Chemical Substances	Adipates ; Aerosols ; Alkanes ; Gases ; Naphthalenes ; Particulate Matter ; naphthalene (2166IN72UN) ; adipic acid (76A0JE0FKJ) ; Succinic Acid (AB6MNQ6J6L) ; nonane (T9W3VH6G10)
Language	English
Publishing date	2014-10-09
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
ISSN	1520-5851
ISSN (online)	1520-5851
DOI	10.1021/es501816h
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Article ; Online: Role of sesquiterpenes in biogenic new particle formation.

Dada, Lubna / Stolzenburg, Dominik / Simon, Mario / Fischer, Lukas / Heinritzi, Martin / Wang, Mingyi / Xiao, Mao / Vogel, Alexander L / Ahonen, Lauri / Amorim, Antonio / Baalbaki, Rima / Baccarini, Andrea / Baltensperger, Urs / Bianchi, Federico / Daellenbach, Kaspar R / DeVivo, Jenna / Dias, Antonio / Dommen, Josef / Duplissy, Jonathan /

Finkenzeller, Henning / Hansel, Armin / He, Xu-Cheng / Hofbauer, Victoria / Hoyle, Christopher R / Kangasluoma, Juha / Kim, Changhyuk / Kürten, Andreas / Kvashnin, Aleksander / Mauldin, Roy / Makhmutov, Vladimir / Marten, Ruby / Mentler, Bernhard / Nie, Wei / Petäjä, Tuukka / Quéléver, Lauriane L J / Saathoff, Harald / Tauber, Christian / Tome, Antonio / Molteni, Ugo / Volkamer, Rainer / Wagner, Robert / Wagner, Andrea C / Wimmer, Daniela / Winkler, Paul M / Yan, Chao / Zha, Qiaozhi / Rissanen, Matti / Gordon, Hamish / Curtius, Joachim / Worsnop, Douglas R / Lehtipalo, Katrianne / Donahue, Neil M / Kirkby, Jasper / El Haddad, Imad / Kulmala, Markku

Science advances

2023 Volume 9, Issue 36, Page(s) eadi5297

Abstract: Biogenic vapors form new particles in the atmosphere, affecting global climate. The contributions of monoterpenes and isoprene to new particle formation (NPF) have been extensively studied. However, sesquiterpenes have received little attention despite a ...

Abstract	Biogenic vapors form new particles in the atmosphere, affecting global climate. The contributions of monoterpenes and isoprene to new particle formation (NPF) have been extensively studied. However, sesquiterpenes have received little attention despite a potentially important role due to their high molecular weight. Via chamber experiments performed under atmospheric conditions, we report biogenic NPF resulting from the oxidation of pure mixtures of β-caryophyllene, α-pinene, and isoprene, which produces oxygenated compounds over a wide range of volatilities. We find that a class of vapors termed ultralow-volatility organic compounds (ULVOCs) are highly efficient nucleators and quantitatively determine NPF efficiency. When compared with a mixture of isoprene and monoterpene alone, adding only 2% sesquiterpene increases the ULVOC yield and doubles the formation rate. Thus, sesquiterpene emissions need to be included in assessments of global aerosol concentrations in pristine climates where biogenic NPF is expected to be a major source of cloud condensation nuclei.
Language	English
Publishing date	2023-09-08
Publishing country	United States
Document type	Journal Article
ZDB-ID	2810933-8
ISSN	2375-2548 ; 2375-2548
ISSN (online)	2375-2548
ISSN	2375-2548
DOI	10.1126/sciadv.adi5297
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Article ; Online: Experiments on the temperature dependence of heterogeneous nucleation on nanometer-sized NaCl and Ag particles.

Schobesberger, Siegfried / Winkler, Paul M / Pinterich, Tamara / Vrtala, Aron / Kulmala, Markku / Wagner, Paul E

Chemphyschem : a European journal of chemical physics and physical chemistry

2010 Volume 11, Issue 18, Page(s) 3874–3882

Abstract: Experimental investigations on the activation of NaCl and Ag aerosol particles by heterogeneous nucleation of n-propanol vapor at well-defined vapor saturation ratios are presented. Particular emphasis is placed on the temperature dependence of this ... ...

Abstract	Experimental investigations on the activation of NaCl and Ag aerosol particles by heterogeneous nucleation of n-propanol vapor at well-defined vapor saturation ratios are presented. Particular emphasis is placed on the temperature dependence of this process from -11 to +14 °C. Aerosols are generated in a tube furnace and electrostatically classified at mean geometric mobility equivalent diameters between 3.6 and 11 nm. Activation probabilities are measured by means of expansion chamber experiments, and onset n-propanol saturation ratios are subsequently determined. The experiments with Ag particles do not produce any unexpected results. The results for NaCl particles, however, show a temperature trend of the onset saturation ratios that is opposite to that predicted by classical nucleation theory. This stresses the important role that surface properties play in heterogeneous nucleation processes. By tentatively assuming a temperature-dependent contact angle, we are able to theoretically reproduce this reversed temperature trend. In addition, the shrinkage of NaCl condensation particles is investigated for varying amounts of n-propanol vapor, and contact angle measurements are performed at temperatures ranging from -7 to +30 °C.
Language	English
Publishing date	2010-12-17
Publishing country	Germany
Document type	Journal Article
ISSN	1439-7641
ISSN (online)	1439-7641
DOI	10.1002/cphc.201000417
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Article ; Online: Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere.

He, Xu-Cheng / Simon, Mario / Iyer, Siddharth / Xie, Hong-Bin / Rörup, Birte / Shen, Jiali / Finkenzeller, Henning / Stolzenburg, Dominik / Zhang, Rongjie / Baccarini, Andrea / Tham, Yee Jun / Wang, Mingyi / Amanatidis, Stavros / Piedehierro, Ana A / Amorim, Antonio / Baalbaki, Rima / Brasseur, Zoé / Caudillo, Lucía / Chu, Biwu /

Dada, Lubna / Duplissy, Jonathan / El Haddad, Imad / Flagan, Richard C / Granzin, Manuel / Hansel, Armin / Heinritzi, Martin / Hofbauer, Victoria / Jokinen, Tuija / Kemppainen, Deniz / Kong, Weimeng / Krechmer, Jordan / Kürten, Andreas / Lamkaddam, Houssni / Lopez, Brandon / Ma, Fangfang / Mahfouz, Naser G A / Makhmutov, Vladimir / Manninen, Hanna E / Marie, Guillaume / Marten, Ruby / Massabò, Dario / Mauldin, Roy L / Mentler, Bernhard / Onnela, Antti / Petäjä, Tuukka / Pfeifer, Joschka / Philippov, Maxim / Ranjithkumar, Ananth / Rissanen, Matti P / Schobesberger, Siegfried / Scholz, Wiebke / Schulze, Benjamin / Surdu, Mihnea / Thakur, Roseline C / Tomé, António / Wagner, Andrea C / Wang, Dongyu / Wang, Yonghong / Weber, Stefan K / Welti, André / Winkler, Paul M / Zauner-Wieczorek, Marcel / Baltensperger, Urs / Curtius, Joachim / Kurtén, Theo / Worsnop, Douglas R / Volkamer, Rainer / Lehtipalo, Katrianne / Kirkby, Jasper / Donahue, Neil M / Sipilä, Mikko / Kulmala, Markku

Science (New York, N.Y.)

2023 Volume 382, Issue 6676, Page(s) 1308–1314

Abstract: The main nucleating vapor in the atmosphere is thought to be sulfuric acid ( ... ...

Abstract	The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H
Language	English
Publishing date	2023-12-14
Publishing country	United States
Document type	Journal Article
ZDB-ID	128410-1
ISSN	1095-9203 ; 0036-8075
ISSN (online)	1095-9203
ISSN	0036-8075
DOI	10.1126/science.adh2526
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