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利用共振红外辐射研究星际冰类似物中的纯CH以及CH与HO的相互作用。

Studying Pure CH and the Interaction of CH and HO in Interstellar Ice Analogues with On-Resonance Infrared Irradiation.

作者信息

Schrauwen Johanna G M, Cuppen Herma M, Ioppolo Sergio, Redlich Britta

机构信息

HFML-FELIX Laboratory, IMM, Radboud University, 6525 ED Nijmegen, The Netherlands.

Institute of Molecules and Materials (IMM), Radboud University, 6525 AJ Nijmegen, The Netherlands.

出版信息

J Phys Chem A. 2025 Jul 31;129(30):6883-6895. doi: 10.1021/acs.jpca.5c03186. Epub 2025 Jul 18.

Abstract

Methane in the solid state is often studied in interaction with water, either as clathrate hydrates or as interstellar ice in a water-rich ice environment. Using free-electron laser infrared irradiation, we studied the interaction between CH and HO through energy dissipation after on-resonance vibrational excitation. The observed changes in the ice structure are largely independent of the vibrational mode excited and suggest an energy-dissipation-induced local heating of the ice. Local heating results in desorption for the two pure crystalline phases of CH, a phase transition to phase II for metastable CH and a 1:10 HO:CH mixture, and segregation for the 1:1 and 1:5 HO:CH ice mixtures. Local heating only occurs when the infrared irradiation is on resonance with a vibrational mode of the system in the case of the pure CH ices, suggesting that a sufficient absorption cross section is required to convert the on-resonance vibrational energy into general heating.

摘要

固态甲烷通常在与水相互作用的情况下被研究,其形式可以是笼形水合物,也可以是富含水的冰环境中的星际冰。我们使用自由电子激光红外辐射,通过共振振动激发后的能量耗散研究了CH与HO之间的相互作用。观察到的冰结构变化在很大程度上与激发的振动模式无关,这表明能量耗散导致了冰的局部加热。局部加热导致CH的两种纯晶相发生解吸,亚稳态CH和1:10 HO:CH混合物转变为II相,以及1:1和1:5 HO:CH冰混合物发生分离。在纯CH冰的情况下,只有当红外辐射与系统的振动模式共振时才会发生局部加热,这表明需要足够的吸收截面才能将共振振动能量转化为一般加热。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f1e5/12319911/35c2a89425ca/jp5c03186_0001.jpg

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