High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses

The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty through correlation signals averaged over indep...

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Autores principales:	Stefano M. Cavaletto, Daniel Keefer, Shaul Mukamel
Formato:	article
Lenguaje:	EN
Publicado:	American Physical Society 2021
Materias:	Physics QC1-999
Acceso en línea:	https://doaj.org/article/97d112dddfc34b9dbd932ac2bd63262a
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spelling	oai:doaj.org-article:97d112dddfc34b9dbd932ac2bd63262a2021-12-02T14:23:07ZHigh Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses10.1103/PhysRevX.11.0110292160-3308https://doaj.org/article/97d112dddfc34b9dbd932ac2bd63262a2021-02-01T00:00:00Zhttp://doi.org/10.1103/PhysRevX.11.011029http://doi.org/10.1103/PhysRevX.11.011029https://doaj.org/toc/2160-3308The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty through correlation signals averaged over independent pulse realizations. No control is required over the spectral phase of the pulse, enabling immediate application of existing, noisy x-ray free-electron-laser pulses. The proposed stimulated Raman technique provides the combined broad observation bandwidth and high time-frequency resolution needed for the observation of elementary molecular events. A model is used to simulate chaotic free-electron-laser pulses and calculate their correlation properties. The resulting joint temporal and spectral resolution is exemplified for a molecular model system with time-dependent frequencies and for the RNA base uracil passing through a conical intersection. Ultrafast coherences, which constitute a direct signature of the nonadiabatic dynamics, are resolved. The detail and depth of physical information accessed by the proposed stochastic signal are virtually identical to those obtained by phase-controlled pulses.Stefano M. CavalettoDaniel KeeferShaul MukamelAmerican Physical SocietyarticlePhysicsQC1-999ENPhysical Review X, Vol 11, Iss 1, p 011029 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Physics QC1-999
spellingShingle	Physics QC1-999 Stefano M. Cavaletto Daniel Keefer Shaul Mukamel High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
description	The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty through correlation signals averaged over independent pulse realizations. No control is required over the spectral phase of the pulse, enabling immediate application of existing, noisy x-ray free-electron-laser pulses. The proposed stimulated Raman technique provides the combined broad observation bandwidth and high time-frequency resolution needed for the observation of elementary molecular events. A model is used to simulate chaotic free-electron-laser pulses and calculate their correlation properties. The resulting joint temporal and spectral resolution is exemplified for a molecular model system with time-dependent frequencies and for the RNA base uracil passing through a conical intersection. Ultrafast coherences, which constitute a direct signature of the nonadiabatic dynamics, are resolved. The detail and depth of physical information accessed by the proposed stochastic signal are virtually identical to those obtained by phase-controlled pulses.
format	article
author	Stefano M. Cavaletto Daniel Keefer Shaul Mukamel
author_facet	Stefano M. Cavaletto Daniel Keefer Shaul Mukamel
author_sort	Stefano M. Cavaletto
title	High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
title_short	High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
title_full	High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
title_fullStr	High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
title_full_unstemmed	High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
title_sort	high temporal and spectral resolution of stimulated x-ray raman signals with stochastic free-electron-laser pulses
publisher	American Physical Society
publishDate	2021
url	https://doaj.org/article/97d112dddfc34b9dbd932ac2bd63262a
work_keys_str_mv	AT stefanomcavaletto hightemporalandspectralresolutionofstimulatedxrayramansignalswithstochasticfreeelectronlaserpulses AT danielkeefer hightemporalandspectralresolutionofstimulatedxrayramansignalswithstochasticfreeelectronlaserpulses AT shaulmukamel hightemporalandspectralresolutionofstimulatedxrayramansignalswithstochasticfreeelectronlaserpulses
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High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses

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