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  Stochastic stimulated electronic x-ray Raman spectroscopy

Kimberg, V., & Rohringer, N. (2016). Stochastic stimulated electronic x-ray Raman spectroscopy. Structural Dynamics, 3(3): 034101. doi:10.1063/1.4940916.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0029-2323-8 Version Permalink: http://hdl.handle.net/21.11116/0000-0004-93FC-A
Genre: Journal Article

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http://arxiv.org/abs/1511.00481 (Preprint)
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http://dx.doi.org/10.1063/1.4940916 (Publisher version)
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 Creators:
Kimberg, Victor1, 2, Author              
Rohringer, Nina1, 3, 4, Author              
Affiliations:
1Max Planck Institute for the Physics of Complex Systems, Max Planck Society, ou_2117288              
2Theoretical Chemistry and Biology, Royal Institute of Technology, 10691 Stockholm, Sweden, ou_persistent22              
3Quantum Optics with X-Rays, Independent Research Groups, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938291              
4Center for Free-Electron Laser Science, Luruper Chaussee 149, 22761 Hamburg, Germany, ou_persistent22              

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Free keywords: Chemical Physics; Atomic and Molecular Clusters; Photons X-ray optics; X-ray spectra; X-ray spectroscopy; Absorption spectra
 Abstract: 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-rayfree 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.

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Language(s): eng - English
 Dates: 2015-11-022015-10-302016-01-152016-02-092016-05
 Publication Status: Published in print
 Pages: 20
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: arXiv: 1511.00481
DOI: 10.1063/1.4940916
 Degree: -

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Title: Structural Dynamics
Source Genre: Journal
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Publ. Info: Melville, NY : American Institute of Physics
Pages: - Volume / Issue: 3 (3) Sequence Number: 034101 Start / End Page: - Identifier: Other: 2329-7778
CoNE: /journals/resource/2329-7778