光子吸收后相干核响应的直接观测
Direct observation of the coherent nuclear response after the absorption of a photon
摘要：
分子如何将光能转化为特定的转换是光物理学中的一个基本问题。超快光谱揭示了与电子能量流相关的动力学，但对吸收的光子能量如何驱动核或电子运动知之甚少。在这里，我们使用超宽带瞬态吸收光谱监测相干振动能量流光激发后的视网膜生色团。在质子泵细菌视紫红质中，我们观察到氢摇摆和主链扭转模式的相干激活，这些模式在溶液环境中被非反应性坐标所取代，伴随着反应性弛豫途径的失活。
英文摘要：
How molecules convert light energy to perform a specific transformation is a fundamental question in photophysics. Ultrafast spectroscopy reveals the kinetics associated with electronic energy flow, but little is known about how absorbed photon energy drives nuclear or electronic motion. Here, we used ultrabroadband transient absorption spectroscopy to monitor coherent vibrational energy flow after photoexcitation of the retinal chromophore. In the proton pump bacteriorhodopsin we observed coherent activation of hydrogen wagging and backbone torsional modes that were replaced by unreactive coordinates in the solution environment, concomitant with a deactivation of the reactive relaxation pathway.
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