Populations and coherence in femtosecond time resolved X-ray crystallography of the photoactive yellow protein

IF 2.5 2区 化学 Q3 CHEMISTRY, PHYSICAL
C. Hutchison, J. V. van Thor
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引用次数: 12

Abstract

Abstract Ultrafast X-ray crystallography of the photoactive yellow protein with femtosecond delays using an X-ray free electron laser has successfully probed the dynamics of an early Franck-Condon species. The femtosecond pump-probe application of protein crystallography represents a new experimental regime that provides an X-ray structural probe for coherent processes that were previously accessible primarily using ultrafast spectroscopy. We address how the optical regime of the visible pump, that is necessary to successfully resolve ultrafast structural differences, affects the motions that are measured using the technique. The sub-picosecond photochemical dynamics in PYP involves evolution of a mixture of electronic ground and excited state populations. Additional to photoisomerisation that is considered to proceed through activated barrier crossing, within the dephasing time structural motion include vibrational coherence arising from excited states, the ground state and a ground state intermediate under experimental conditions used for ultrafast crystallography. Intense optical pulses are required to convert population levels in PYP crystals that allow detection by X-ray crystallography, but the compromise currently needed for the optical bandwidth and power has consequences with regard to the contributions to the motions that are experimentally measured with femtosecond delays. We briefly review the ultrafast spectroscopy literature of the primary photoreactions of PYP and discuss relevant physical models taken from coherent control and femtosecond coherence spectroscopy literature that address both the population transfer as well as the vibrational coherences. We apply linear response theory, with the additional use of a high power approximation, of on-resonance impulsive vibrational coherence in the ground state and the non-impulsive coherence in the excited state and discuss experimental approaches to manipulate the coherence contributions. The results are generalised and extended to discuss the future capabilities of high repetition rate X-ray free electron laser instruments providing enhanced sensitivity to perform the crystallographic equivalent of an impulsive Raman measurement of vibrational coherence.
光活性黄色蛋白飞秒时间分辨x射线晶体学的居群和相干性
利用x射线自由电子激光器对具有飞秒延迟的光活性黄色蛋白进行了超快x射线晶体学研究,成功地探测了早期Franck-Condon物质的动力学。蛋白质晶体学的飞秒泵浦探针应用代表了一种新的实验体制,它为先前主要使用超快光谱的相干过程提供了x射线结构探针。我们讨论了成功解决超快结构差异所必需的可见泵浦的光学状态如何影响使用该技术测量的运动。PYP中的亚皮秒光化学动力学涉及电子基态和激发态种群混合的演化。除了光异构化被认为是通过激活的势垒穿越进行,在脱相时间内,结构运动包括由激发态、基态和实验条件下用于超快晶体学的基态中间体产生的振动相干性。在PYP晶体中,需要强烈的光脉冲来转换允许x射线晶体学检测的种群水平,但是目前需要的光带宽和功率的折衷对于用飞秒延迟实验测量的运动的贡献有影响。我们简要回顾了PYP初级光反应的超快光谱文献,并讨论了从相干控制和飞秒相干光谱文献中获取的相关物理模型,这些模型既解决了人口转移问题,也解决了振动相干问题。我们应用线性响应理论,并额外使用高功率近似,对基态的非共振脉冲振动相干性和激发态的非脉冲相干性进行分析,并讨论了操纵相干性贡献的实验方法。这些结果被推广和扩展,以讨论高重复率x射线自由电子激光仪器的未来能力,提供更高的灵敏度,以执行振动相干性的脉冲拉曼测量的晶体学等效。
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来源期刊
CiteScore
14.20
自引率
1.60%
发文量
5
审稿时长
1 months
期刊介绍: International Reviews in Physical Chemistry publishes review articles describing frontier research areas in physical chemistry. Internationally renowned scientists describe their own research in the wider context of the field. The articles are of interest not only to specialists but also to those wishing to read general and authoritative accounts of recent developments in physical chemistry, chemical physics and theoretical chemistry. The journal appeals to research workers, lecturers and research students alike.
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