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New Particle Formation from the Vapor Phase: From Barrier-Controlled Nucleation to the Collisional Limit.


ABSTRACT: Studies of vapor phase nucleation have largely been restricted to one of two limiting cases-nucleation controlled by a substantial free energy barrier or the collisional limit where the barrier is negligible. For weakly bound systems, exploring the transition between these regimes has been an experimental challenge, and how nucleation evolves in this transition remains an open question. We overcome these limitations by combining complementary Laval expansion experiments, providing new particle formation data for carbon dioxide over a uniquely broad range of conditions. Our experimental data together with a kinetic model using rate constants from high-level quantum chemical calculations provide a comprehensive picture of new particle formation as nucleation transitions from a barrier-dominated process to the collisional limit.

SUBMITTER: Dingilian KK 

PROVIDER: S-EPMC8154860 | biostudies-literature | 2021 May

REPOSITORIES: biostudies-literature

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New Particle Formation from the Vapor Phase: From Barrier-Controlled Nucleation to the Collisional Limit.

Dingilian Kayane K KK   Lippe Martina M   Kubečka Jakub J   Krohn Jan J   Li Chenxi C   Halonen Roope R   Keshavarz Fatemeh F   Reischl Bernhard B   Kurtén Theo T   Vehkamäki Hanna H   Signorell Ruth R   Wyslouzil Barbara E BE  

The journal of physical chemistry letters 20210510 19


Studies of vapor phase nucleation have largely been restricted to one of two limiting cases-nucleation controlled by a substantial free energy barrier or the collisional limit where the barrier is negligible. For weakly bound systems, exploring the transition between these regimes has been an experimental challenge, and how nucleation evolves in this transition remains an open question. We overcome these limitations by combining complementary Laval expansion experiments, providing new particle f  ...[more]

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