Photon Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany;
The Hamburg Centre for Ultrafast Imaging, 22761 Hamburg, Germany.
Proc Natl Acad Sci U S A. 2020 Sep 29;117(39):24110-24116. doi: 10.1073/pnas.2003337117. Epub 2020 Sep 15.
Dynamics and kinetics in soft matter physics, biology, and nanoscience frequently occur on fast (sub)microsecond but not ultrafast timescales which are difficult to probe experimentally. The European X-ray Free-Electron Laser (European XFEL), a megahertz hard X-ray Free-Electron Laser source, enables such experiments via taking series of diffraction patterns at repetition rates of up to 4.5 MHz. Here, we demonstrate X-ray photon correlation spectroscopy (XPCS) with submicrosecond time resolution of soft matter samples at the European XFEL. We show that the XFEL driven by a superconducting accelerator provides unprecedented beam stability within a pulse train. We performed microsecond sequential XPCS experiments probing equilibrium and nonequilibrium diffusion dynamics in water. We find nonlinear heating on microsecond timescales with dynamics beyond hot Brownian motion and superheated water states persisting up to 100 μs at high fluences. At short times up to 20 μs we observe that the dynamics do not obey the Stokes-Einstein predictions.
软物质物理、生物和纳米科学中的动力学和动力学经常发生在快速(亚微秒)但不是超快时间尺度上,这很难在实验中探测到。欧洲 X 射线自由电子激光(欧洲 XFEL)是一种兆赫兹硬 X 射线自由电子激光源,通过在高达 4.5 MHz 的重复率下采集一系列衍射图案来实现这些实验。在这里,我们在欧洲 XFEL 上演示了具有亚微秒时间分辨率的软物质样品的 X 射线光子相关光谱(XPCS)。我们表明,由超导加速器驱动的 XFEL 在脉冲串内提供了前所未有的光束稳定性。我们进行了微秒级顺序 XPCS 实验,探测水中的平衡和非平衡扩散动力学。我们发现,在微秒时间尺度上存在非线性加热,动力学超出了热布朗运动,过热状态在高通量下持续长达 100 μs。在短时间内,直到 20 μs,我们观察到动力学不遵守斯托克斯-爱因斯坦预测。