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Title: Pore condensation and freezing is responsible for ice formation below water saturation for porous particles
Authors : David, Robert O.
Marcolli, Claudia
Fahrni, Jonas
Qiu, Yuqing
Perez Sirkin, Yamila A.
Molinero, Valeria
Mahrt, Fabian
Brühwiler, Dominik
Lohmann, Ulrike
Kanji, Zamin A.
Published in : Proceedings of the National Academy of Sciences of the United States of America
Volume(Issue) : 116
Issue : 17
Pages : 8184
Pages to: 8189
Publisher / Ed. Institution : National Academy of Sciences
Issue Date: 2019
License (according to publishing contract) : CC BY-NC-ND 4.0: Attribution - Non commercial - No derivatives 4.0 International
Type of review: Peer review (publication)
Language : English
Subjects : Cirrus; Cloud; Deposition nucleation; Ice nucleation; Pore condensation and freezing
Subject (DDC) : 500: Natural sciences and mathematics
Abstract: Ice nucleation in the atmosphere influences cloud properties, altering precipitation and the radiative balance, ultimately regulating Earth's climate. An accepted ice nucleation pathway, known as deposition nucleation, assumes a direct transition of water from the vapor to the ice phase, without an intermediate liquid phase. However, studies have shown that nucleation occurs through a liquid phase in porous particles with narrow cracks or surface imperfections where the condensation of liquid below water saturation can occur, questioning the validity of deposition nucleation. We show that deposition nucleation cannot explain the strongly enhanced ice nucleation efficiency of porous compared with nonporous particles at temperatures below -40 °C and the absence of ice nucleation below water saturation at -35 °C. Using classical nucleation theory (CNT) and molecular dynamics simulations (MDS), we show that a network of closely spaced pores is necessary to overcome the barrier for macroscopic ice-crystal growth from narrow cylindrical pores. In the absence of pores, CNT predicts that the nucleation barrier is insurmountable, consistent with the absence of ice formation in MDS. Our results confirm that pore condensation and freezing (PCF), i.e., a mechanism of ice formation that proceeds via liquid water condensation in pores, is a dominant pathway for atmospheric ice nucleation below water saturation. We conclude that the ice nucleation activity of particles in the cirrus regime is determined by the porosity and wettability of pores. PCF represents a mechanism by which porous particles like dust could impact cloud radiative forcing and, thus, the climate via ice cloud formation.
Departement: Life Sciences and Facility Management
Organisational Unit: Institute of Chemistry and Biotechnology (ICBT)
Publication type: Article in scientific journal
DOI : 10.21256/zhaw-3312
ISSN: 0027-8424
Appears in Collections:Publikationen Life Sciences und Facility Management

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