Timescales of N-H bond dissociation in pyrrole: a nonadiabatic dynamics study.
作者： Marin Sapunar , Aurora Ponzi , Sermsiri Chaiwongwattana , Momir Mališ , Antonio Prlj
DOI: 10.1039/C5CP02100F
关键词:
摘要: The excitation wavelength dependent photodynamics of pyrrole are investigated by nonadiabatic trajectory-surface-hopping dynamics simulations based on time density functional theory (TDDFT) and the algebraic diagrammatic construction method to second order (ADC(2)). ADC(2) results confirm that N–H bond dissociation occurring upon at origin first excited state, S1(πσ*), is driven tunnelling [Roberts et al., Faraday Discuss., 2013, 163, 95] as a barrier ΔE = 1780 cm−1 traps population in quasi-bound minimum. Upon S1(πσ*) range 236–240 nm, direct takes place with constant 28 fs. computed very good agreement recently reported measurements. Excitation lowest B2 state 198–202 nm returns for fission 48 fs B3LYP/def2-TZVPD level, perfect experiment al. 95]. For same ADC(2)/aug-cc-pVDZ decay more than three times longer experimentally one. accuracy checked against reference complete-active-space second-order perturbation (CASPT2) calculations explained terms correct topography ππ* surface lack mixing between 3px Rydberg states which occurs method.
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