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Stochastic stimulated electronic x-ray Raman spectroscopy
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology. Max Planck Institute for the Physics of Complex Systems, Germany.ORCID iD: 0000-0003-1269-8760
2016 (English)In: Structural Dynamics, ISSN 2329-7778, Vol. 3, no 3, 34101Article in journal (Refereed) PublishedText
Abstract [en]

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→π* 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.

Place, publisher, year, edition, pages
American Association of Physicists in Medicine , 2016. Vol. 3, no 3, 34101
National Category
Physical Sciences
URN: urn:nbn:se:kth:diva-186978DOI: 10.1063/1.4940916ISI: 000379177700002ScopusID: 2-s2.0-84958749894OAI: diva2:929904

QC 20160520

Available from: 2016-05-20 Created: 2016-05-16 Last updated: 2016-08-12Bibliographically approved

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Kimberg, Victor
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