期刊
FARADAY DISCUSSIONS
卷 157, 期 -, 页码 27-39出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2fd20010d
关键词
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资金
- Department of Energy [DE-FG02-97ER14782]
We report Trajectory Surface Hopping (TSH) calculations of CH3CHO photodissociation involving three electronic states, S-1, T-1, and S-0, with a focus on the radical products CH3 + HCO, which can be formed from both T-1 and S-0. We use previously reported potential energy surfaces and spin-orbit couplings for T-1 and S-0 and report a new potential and spin-orbit coupling for S-1 here. Roughly 32 000 trajectories are performed at energies corresponding to seven photolysis wavelengths between 372 and 230 nm. Motivated by recent experiments, we examine the branching ratio of the T-1 to S-0 pathways as a function of photolysis energy. We also present the relative translational energy and CH3 vibrational energy distributions from these pathways at a photolysis energy of 100 kcal mol(-1), formed from both the T-1 and S-0 potentials. As with standard quasiclassical trajectory calculations, violation of zero-point energy for products also occurs in TSH calculations. This is shown to be a serious issue for this branching ratio and one of several methods considered to deal with this issue is shown to give satisfactory results.
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