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Stochastic stimulated electronic x-ray Raman spectroscopy

DOI:10.1063/1.4940916 期刊:Structural Dynamics 出版年份:2016 更新时间:2025-09-04 15:30:14
摘要: Resonant inelastic x-ray scattering (RIXS) is a well-established tool for studying electronic, nuclear, and collective dynamics of excited atoms, molecules, and solids. An extension of this powerful method to a time-resolved probe technique at x-ray free electron lasers (XFELs) to ultimately unravel ultrafast chemical and structural changes on a femtosecond time scale is often challenging, due to the small signal rate in conventional implementations at XFELs that rely on the usage of a monochromator setup to select a small frequency band of the broadband, spectrally incoherent XFEL radiation. Here, we suggest an alternative approach, based on stochastic spectroscopy, which uses the full bandwidth of the incoming XFEL pulses. Our proposed method is relying on stimulated resonant inelastic x-ray scattering, where in addition to a pump pulse that resonantly excites the system a probe pulse on a specific electronic inelastic transition is provided, which serves as a seed in the stimulated scattering process. The limited spectral coherence of the XFEL radiation defines the energy resolution in this process and stimulated RIXS spectra of high resolution can be obtained by covariance analysis of the transmitted spectra. We present a detailed feasibility study and predict signal strengths for realistic XFEL parameters for the CO molecule resonantly pumped at the O1s ! p(cid:2) transition. Our theoretical model describes the evolution of the spectral and temporal characteristics of the transmitted x-ray radiation, by solving the equation of motion for the electronic and vibrational degrees of freedom of the system self consistently with the propagation by Maxwell equations.
作者: Victor Kimberg,Nina Rohringer
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Investigating the feasibility of using stochastic stimulated electronic x-ray Raman spectroscopy as a high-resolution probe for studying ultrafast chemical and structural changes in molecules, specifically the CO molecule, using x-ray free electron lasers.

The study demonstrates the potential of stochastic stimulated electronic x-ray Raman spectroscopy as a high-resolution probe for molecular dynamics, with specific predictions for the CO molecule. It highlights the importance of achieving sufficient Raman gain and the challenges posed by the stochastic nature of XFEL pulses. The method offers a promising alternative to conventional RIXS for studying ultrafast chemical and structural changes.

The study is theoretical and relies on simulations, which may not fully capture all experimental conditions. The feasibility of observing high-resolution spectra is contingent on the ability to achieve sufficient Raman gain and the technical capabilities of XFEL facilities, including pulse energy jitter, pulse durations, and spectrometer resolution.

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