Observing Vibrational Wavepackets during an Ultrafast Electron Transfer Reaction.
作者： Shahnawaz Rafiq , Jacob C. Dean , Gregory D. Scholes
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摘要: Recent work has proposed that coherent effects impact ultrafast electron transfer reactions. Here we report studies using broadband pump-probe and two-dimensional electronic spectroscopy of intramolecular nuclear motion on the time scale between oxazine 1 (Ox1) dimethylaniline (DMA). We performed time-frequency analysis domain data to assign signal amplitude modulations ground or excited states in reactive system (Ox1 DMA) relative control chloronaphthalene). It was found our ability detect vibrational coherence via state Ox1 diminishes population is lost by transfer. However, wavepacket not damped process been observed previously detecting radical transient absorption. The presented here indicates "addition" an photoexcited acceptor does significantly perturb coherence, suggesting its presence as a spectator, consistent with Born-Oppenheimer separation degrees freedom.
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