Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Matrix Assisted Processes in CH4-Doped Ar Ices Irradiated with an Electron Beam

Version 1 : Received: 6 August 2023 / Approved: 7 August 2023 / Online: 8 August 2023 (10:21:14 CEST)

A peer-reviewed article of this Preprint also exists.

Bludov, M.; Khyzhniy, I.; Uyutnov, S.; Savchenko, E. Matrix-Assisted Processes in CH4-Doped Ar Ices Irradiated with an Electron Beam. Methane 2023, 2, 372-388. Bludov, M.; Khyzhniy, I.; Uyutnov, S.; Savchenko, E. Matrix-Assisted Processes in CH4-Doped Ar Ices Irradiated with an Electron Beam. Methane 2023, 2, 372-388.

Abstract

The relaxation processes induced by an exposure of the Ar matrices doped with CH4 (0.1 – 10%) to an electron beam were studied with a focus on the dynamics of radiolysis products – H atoms, H2 molecules, CH radicals, and energy transfer processes. Three channels of energy transfer to dopant and radiolysis products were discussed: by free charge carriers, free excitons and photons from the “intrinsic source” provided by emission of the self-trapped excitons. Radiolysis products along with the total yield of desorbing particles were monitored in a correlated manner. Analysis of methane transformation reactions induced by free excitons showed that the CH radical can be considered as a marker of the CH3 species. The competition between exciton self-trapping and energy transfer to the dopant and radiolysis products has been demonstrated. A nonlinear concentration behavior of the H atoms in doped Ar matrices has been established. Real-time correlated monitoring of optical emissions (H atom and CH3 radicals), particle ejection, and temperature revealed a nonmonotonic behavior of optical yields with a strong luminescence flash after almost an hour of exposure, which correlated with explosive pulse of particle ejection and temperature. The connection of this phenomenon with the processes of energy transfer and radical-radical recombination is discussed.

Keywords

solid methane; astrophysical ices; matrix isolation; electron irradiation; radiolysis; energy transfer; particle ejection; relaxation processes; luminescence

Subject

Chemistry and Materials Science, Physical Chemistry

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