Hutchison Christopher D M, Perrett Samuel, van Thor Jasper J
Department of Life Sciences, Faculty of Natural Sciences, Imperial College London, London SW7 2AZ, United Kingdom.
J Phys Chem B. 2024 Sep 19;128(37):8855-8868. doi: 10.1021/acs.jpcb.4c01492. Epub 2024 Aug 1.
Free electron lasers operating in the soft and hard X-ray regime provide capabilities for ultrafast science in many areas, including X-ray spectroscopy, diffractive imaging, solution and material scattering, and X-ray crystallography. Ultrafast time-resolved applications in the picosecond, femtosecond, and attosecond regimes are often possible using single-shot experimental configurations. Aside from X-ray pump and X-ray probe measurements, all other types of ultrafast experiments require the synchronized operation of pulsed laser excitation for resonant or nonresonant pumping. This Perspective focuses on the opportunities for the optical control of structural dynamics by applying techniques from nonlinear spectroscopy to ultrafast X-ray experiments. This typically requires the synthesis of two or more optical pulses with full control of pulse and interpulse parameters. To this end, full characterization of the femtosecond optical pulses is also highly desirable. It has recently been shown that two-color and two-pulse femtosecond excitation of fluorescent protein crystals allowed a Tannor-Rice coherent control experiment, performed under characterized conditions. Pulse shaping and the ability to synthesize multicolor and multipulse conditions are highly desirable and would enable XFEL facilities to offer capabilities for structural dynamics. This Perspective will give a summary of examples of the types of experiments that could be achieved, and it will additionally summarize the laser, pulse shaping, and characterization that would be recommended as standard equipment for time-resolved XFEL beamlines, with an emphasis on ultrafast time-resolved serial femtosecond crystallography.
工作在软X射线和硬X射线波段的自由电子激光器为许多领域的超快科学研究提供了能力,包括X射线光谱学、衍射成像、溶液和材料散射以及X射线晶体学。使用单次实验配置,通常可以在皮秒、飞秒和阿秒时间尺度上进行超快时间分辨应用。除了X射线泵浦和X射线探测测量外,所有其他类型的超快实验都需要脉冲激光激发的同步操作,用于共振或非共振泵浦。本展望重点关注通过将非线性光谱技术应用于超快X射线实验来实现结构动力学光学控制的机会。这通常需要合成两个或更多的光脉冲,并完全控制脉冲和脉冲间参数。为此,对飞秒光脉冲进行全面表征也是非常必要的。最近的研究表明,荧光蛋白晶体的双色和双脉冲飞秒激发能够在特定条件下进行坦诺尔-赖斯相干控制实验。非常需要脉冲整形以及合成多色和多脉冲条件的能力,这将使X射线自由电子激光设施能够提供结构动力学研究的能力。本展望将总结可以实现的实验类型的示例,并额外总结作为时间分辨X射线自由电子激光光束线标准设备推荐的激光器、脉冲整形和表征技术,重点是超快时间分辨串行飞秒晶体学。