Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas

The surfaces of ice crystals near the melting point are covered with thin liquid water layers, called quasi-liquid layers (QLLs), which play crucial roles in various chemical reactions in nature. So far, there have been many spectroscopic studies of such chemical reactions on ice surfaces, however,...

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Main Authors: Ken Nagashima, Josée Maurais, Ken-ichiro Murata, Yoshinori Furukawa, Patrick Ayotte, Gen Sazaki
Format: Article
Language:English
Published: MDPI AG 2020-01-01
Series:Crystals
Subjects:
Online Access:https://www.mdpi.com/2073-4352/10/2/72
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author Ken Nagashima
Josée Maurais
Ken-ichiro Murata
Yoshinori Furukawa
Patrick Ayotte
Gen Sazaki
author_facet Ken Nagashima
Josée Maurais
Ken-ichiro Murata
Yoshinori Furukawa
Patrick Ayotte
Gen Sazaki
author_sort Ken Nagashima
collection DOAJ
description The surfaces of ice crystals near the melting point are covered with thin liquid water layers, called quasi-liquid layers (QLLs), which play crucial roles in various chemical reactions in nature. So far, there have been many spectroscopic studies of such chemical reactions on ice surfaces, however, revealing the effects of atmospheric gases on ice surfaces remains an experimental challenge. In this study, we chose HNO<sub>3</sub> as a model atmospheric gas, and directly observed the ice basal faces by advanced optical microscopy under partial pressure of HNO<sub>3</sub> (~10<sup>&#8722;4</sup> Pa), relevant to those found in the atmosphere. We found that droplets (HNO<sub>3</sub>-QLLs) appeared on ice surfaces at temperatures ranging from &#8722;0.9 to &#8722;0.2 &#176;C with an increase in temperature, and that they disappeared at temperatures ranging from &#8722;0.6 to &#8722;1.3 &#176;C with decreasing temperature. We also found that the size of the HNO<sub>3</sub>-QLLs decreased immediately after we started reducing the temperature. From the changes in size and the liquid&#8722;solid phase diagram of the HNO<sub>3</sub>-H<sub>2</sub>O binary system, we concluded that the HNO<sub>3</sub>-QLLs did not consist of pure water, but rather aqueous HNO<sub>3</sub> solutions, and that the temperature and HNO<sub>3</sub> concentration of the HNO<sub>3</sub>-QLLs also coincided with those along a liquidus line.
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spelling doaj.art-05e3cd760a354d928b7d8306cd168f042022-12-22T02:55:31ZengMDPI AGCrystals2073-43522020-01-011027210.3390/cryst10020072cryst10020072Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid GasKen Nagashima0Josée Maurais1Ken-ichiro Murata2Yoshinori Furukawa3Patrick Ayotte4Gen Sazaki5Institute of Low Temperature Science, Hokkaido University, N19-W8, Kita-ku, Sapporo 060-0819, JapanDépartement de Chimie, Université de Sherbrooke, 2500 Boulevard Université, Sherbrooke, QC J1K 2R1, CanadaInstitute of Low Temperature Science, Hokkaido University, N19-W8, Kita-ku, Sapporo 060-0819, JapanInstitute of Low Temperature Science, Hokkaido University, N19-W8, Kita-ku, Sapporo 060-0819, JapanDépartement de Chimie, Université de Sherbrooke, 2500 Boulevard Université, Sherbrooke, QC J1K 2R1, CanadaInstitute of Low Temperature Science, Hokkaido University, N19-W8, Kita-ku, Sapporo 060-0819, JapanThe surfaces of ice crystals near the melting point are covered with thin liquid water layers, called quasi-liquid layers (QLLs), which play crucial roles in various chemical reactions in nature. So far, there have been many spectroscopic studies of such chemical reactions on ice surfaces, however, revealing the effects of atmospheric gases on ice surfaces remains an experimental challenge. In this study, we chose HNO<sub>3</sub> as a model atmospheric gas, and directly observed the ice basal faces by advanced optical microscopy under partial pressure of HNO<sub>3</sub> (~10<sup>&#8722;4</sup> Pa), relevant to those found in the atmosphere. We found that droplets (HNO<sub>3</sub>-QLLs) appeared on ice surfaces at temperatures ranging from &#8722;0.9 to &#8722;0.2 &#176;C with an increase in temperature, and that they disappeared at temperatures ranging from &#8722;0.6 to &#8722;1.3 &#176;C with decreasing temperature. We also found that the size of the HNO<sub>3</sub>-QLLs decreased immediately after we started reducing the temperature. From the changes in size and the liquid&#8722;solid phase diagram of the HNO<sub>3</sub>-H<sub>2</sub>O binary system, we concluded that the HNO<sub>3</sub>-QLLs did not consist of pure water, but rather aqueous HNO<sub>3</sub> solutions, and that the temperature and HNO<sub>3</sub> concentration of the HNO<sub>3</sub>-QLLs also coincided with those along a liquidus line.https://www.mdpi.com/2073-4352/10/2/72ice crystalsquasi-liquid layernitric acid gasoptical microscopy
spellingShingle Ken Nagashima
Josée Maurais
Ken-ichiro Murata
Yoshinori Furukawa
Patrick Ayotte
Gen Sazaki
Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
Crystals
ice crystals
quasi-liquid layer
nitric acid gas
optical microscopy
title Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
title_full Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
title_fullStr Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
title_full_unstemmed Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
title_short Appearance and Disappearance of Quasi-Liquid Layers on Ice Crystals in the Presence of Nitric Acid Gas
title_sort appearance and disappearance of quasi liquid layers on ice crystals in the presence of nitric acid gas
topic ice crystals
quasi-liquid layer
nitric acid gas
optical microscopy
url https://www.mdpi.com/2073-4352/10/2/72
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