Clark, VHJ;
Yurchenko, SN;
(2021)
Modelling the non-local thermodynamic equilibrium spectra of silylene (SiH2).
Physical Chemistry Chemical Physics
10.1039/d1cp00839k.
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Abstract
This paper sets out a robust methodology for modelling spectra of polyatomic molecules produced in reactive or dissociative environments, with vibrational populations outside local thermal equilibrium (LTE). The methodology is based on accurate, extensive ro-vibrational line lists containing transitions with high vibrational excitations and relies on the detailed ro-vibrational assignments. The developed methodology is applied to model non-LTE IR and visible spectra of silylene (SiH2) produced in a decomposition of disilane (Si2H6), a reaction of technological importance. Two approaches for non-LTE vibrational populations of the product SiH2 are introduced: a simplistic 1D approach based on the Harmonic approximation and a full 3D model incorporating accurate vibrational wavefunctions of SiH2 computed variationally with the TROVE (Theoretical ROVibrational Energy) program. We show how their non-LTE spectral signatures can be used to trace different reaction channels of molecular dissociations.
| Type: | Article |
|---|---|
| Title: | Modelling the non-local thermodynamic equilibrium spectra of silylene (SiH2) |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1039/d1cp00839k |
| Publisher version: | http://dx.doi.org/10.1039/d1cp00839k |
| Language: | English |
| Additional information: | This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. |
| Keywords: | LASER-INDUCED-FLUORESCENCE, AB-INITIO CALCULATIONS, HYDROGENATED SILICON CLUSTERS, RADIATIVE-TRANSFER MODEL, ABSOLUTE RATE CONSTANTS, AUXILIARY BASIS-SETS, EXOMOL LINE LISTS, THERMAL-DECOMPOSITION, MIDDLE ATMOSPHERE, ABSORPTION-SPECTROSCOPY |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10129030 |
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