Physical and Theoretical Chemistry Laboratory, University of Oxford, South Parks Road, Oxford OX1 3QZ, United Kingdom.
Department of Biochemistry, Biomembrane Structure Unit, University of Oxford, Oxford OX1 3QU, United Kingdom.
Phys Rev Lett. 2014 Jun 13;112(23):238301. doi: 10.1103/PhysRevLett.112.238301. Epub 2014 Jun 9.
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 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-out-of-plane wagging and backbone torsional modes that were replaced by unreactive coordinates in the solution environment, concomitant with a deactivation of the reactive relaxation pathway.
分子如何将光能转化为特定的转化是光物理中的一个基本问题。超快光谱揭示了与电子能量流动相关的动力学,但对于吸收的光子能量如何驱动核运动知之甚少。在这里,我们使用超宽带瞬态吸收光谱来监测视黄醛发色团光激发后相干振动能量的流动。在质子泵菌视紫红质中,我们观察到氢出平面摇摆和骨架扭转模式的相干激活,这些模式在溶液环境中被无反应的坐标取代,同时反应性弛豫途径失活。