Asban Shahaf, Cho Daeheum, Mukamel Shaul
Department of Chemistry and Physics and Astronomy , University of California , Irvine , California 92697-2025 , United States.
J Phys Chem Lett. 2019 Oct 3;10(19):5805-5814. doi: 10.1021/acs.jpclett.9b00924. Epub 2019 Sep 19.
We study theoretically incoherent time-resolved X-ray diffraction of fluctuating sources such as free electron lasers, as well as coherent sources with controllably added randomness. We find that the temporal resolution is strongly eroded by the noise. By considering frequency resolution of the signal, we find that the statistical properties of the noise carry important information allowing us to restore the temporal resolution. We propose a multidimensional stochastic resonance treatment to shape the optical window and extract this information from signals. Using the frequency-dependent stochastic phase as a frequency marker allows to improve the spectral resolution as well via intensity correlations. Frequency-tuned field correlation functions are used to modify the effective frequency gating and extract specific charge density contributions to the diffraction pattern while maintaining temporal resolution.
我们从理论上研究了诸如自由电子激光等波动源以及具有可控添加随机性的相干源的非相干时间分辨X射线衍射。我们发现噪声会严重侵蚀时间分辨率。通过考虑信号的频率分辨率,我们发现噪声的统计特性携带了重要信息,使我们能够恢复时间分辨率。我们提出了一种多维随机共振处理方法来塑造光学窗口并从信号中提取此信息。使用频率相关的随机相位作为频率标记也可以通过强度相关性提高光谱分辨率。频率调谐场相关函数用于修改有效频率门控,并在保持时间分辨率的同时提取对衍射图案的特定电荷密度贡献。