论文标题

通过瞬时共振增强了超快X射线衍射

Enhanced ultrafast X-ray diffraction by transient resonances

论文作者

Kuschel, Stephan, Ho, Phay J., Haddad, Andre Al, Zimmermann, Felix, Flueckiger, Leonie, Ware, Matthew R., Duris, Joseph, MacArthur, James P., Lutman, Alberto, Lin, Ming-Fu, Li, Xiang, Nakahara, Kazutaka, Aldrich, Jeff W., Walter, Peter, Young, Linda, Bostedt, Christoph, Marinelli, Agostino, Gorkhover, Tais

论文摘要

单个Ultrastort X射线脉冲的衍射成像在纳米级,在纳米级,在本机环境中具有亚前分辨率的衍射成像,例如化学反应等非平衡过程,而无需结晶。在这里,在样本损伤发生之前,纳米式射击会部分衍射。样品的结构信息可以从相干X射线干扰图像中重建。从单个重元素纳米颗粒中的此类快照的最新空间分辨率仅限于几纳米。空间分辨率的进一步改进需要更高的图像亮度,这最终受样品的漂白效果的限制。我们比较了来自单个100 nm Xe纳米颗粒的快照,这是XE M-shell共振附近X射线脉冲持续时间和传入的X射线强度的函数。令人惊讶的是,录制的图像很少有飞秒和次秒脉冲的脉冲比静态线性模型预测的高10倍。我们对整个数据集的蒙特卡洛模拟和统计分析证实了这些发现,并将效果归因于瞬态共振。我们的仿真表明,在暴露期间,超快的外形变化可以增加X射线图像的亮度,数量级。我们的研究指导了纳米级空间和时间分辨率的前所未有组合的成像之道。

Diffraction-before-destruction imaging with single ultrashort X-ray pulses has the potential to visualise non-equilibrium processes, such as chemical reactions, at the nanoscale with sub-femtosecond resolution in the native environment without the need of crystallization. Here, a nanospecimen partially diffracts a single X-ray flash before sample damage occurs. The structural information of the sample can be reconstructed from the coherent X-ray interference image. State-of-art spatial resolution of such snapshots from individual heavy element nanoparticles is limited to a few nanometers. Further improvement of spatial resolution requires higher image brightness which is ultimately limited by bleaching effects of the sample. We compared snapshots from individual 100 nm Xe nanoparticles as a function of the X-ray pulse duration and incoming X-ray intensity in the vicinity of the Xe M-shell resonance. Surprisingly, images recorded with few femtosecond and sub-femtosecond pulses are up to 10 times brighter than the static linear model predicts. Our Monte-Carlo simulation and statistical analysis of the entire data set confirms these findings and attributes the effect to transient resonances. Our simulation suggests that ultrafast form factor changes during the exposure can increase the brightness of X-ray images by several orders of magnitude. Our study guides the way towards imaging with unprecedented combination of spatial and temporal resolution at the nanoscale.

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