斯坦福同步辐射光源的溶液相高重复率激光泵浦x射线探针皮秒硬x射线光谱。

IF 2.3 2区 物理与天体物理 Q3 CHEMISTRY, PHYSICAL Structural Dynamics-Us Pub Date : 2023-10-27 eCollection Date: 2023-09-01 DOI:10.1063/4.0000207
Marco Reinhard, Dean Skoien, Jacob A Spies, Angel T Garcia-Esparza, Benjamin D Matson, Jeff Corbett, Kai Tian, James Safranek, Eduardo Granados, Matthew Strader, Kelly J Gaffney, Roberto Alonso-Mori, Thomas Kroll, Dimosthenis Sokaras
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引用次数: 0

摘要

我们在斯坦福同步辐射光源的光束线15-2上提出了一个用于溶液相高重复率(MHz)皮秒硬x射线光谱的专用终端站。用高功率超快掺镱光纤激光器以640的重复频率对样品进行了光激发 kHz,而数据采集工作在1.28 以交替开关模式记录数据的存储环的MHz重复率。时间分辨x射线测量是通过20 SPEAR3的mA/70ps凸轮轴束,这是斯坦福同步加速器辐射光源常规操作期间可用的模式。作为一项基准研究,旨在证明该终端站的优势能力,我们在水性[FeII(phen)3]2+上进行了皮秒Fe K边x射线吸收光谱,这是一种典型的自旋交叉复合物,经过光诱导的激发自旋态捕获,形成0.6-0.7的电子激发态 ns寿命。此外,我们报道了瞬态Fe Kβ主线和价核x射线发射光谱,分别显示出独特的探测灵敏度和与模型光谱和密度泛函理论计算的良好一致性。值得注意的是,所实现的信噪比、整体性能和所开发的终端站的常规可用性使斯坦福同步辐射光源能够使用单色光束进行系统的时间分辨科学计划。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource.

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6-0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

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来源期刊
Structural Dynamics-Us
Structural Dynamics-Us CHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
CiteScore
5.50
自引率
3.60%
发文量
24
审稿时长
16 weeks
期刊介绍: Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods. The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as: Time-resolved X-ray and electron diffraction and scattering, Coherent diffractive imaging, Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.), Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy, Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.), Multidimensional spectroscopies in the infrared, the visible and the ultraviolet, Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains, Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals. These new methods are enabled by new instrumentation, such as: X-ray free electron lasers, which provide flux, coherence, and time resolution, New sources of ultrashort electron pulses, New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources, New sources of ultrashort infrared and terahertz (THz) radiation, New detectors for X-rays and electrons, New sample handling and delivery schemes, New computational capabilities.
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