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Title: Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light

Abstract

Covariance spectroscopy signals based on the transmission of broadband stochastic probe light undergoing a nonlinear optical process with matter are studied. The resulting signal depends on intensity correlation functions of the probe pulse. Application is made to transient absorption and stimulated Raman signals, where an ultraviolet pump and a delayed stochastically modulated infrared or optical Raman probe are used for monitoring vibrational excitations. We show that the stochastic properties of light can be exploited to circumvent the limitations on the joint temporal and spectral resolution of the signal. We study a model system with a time-dependent frequency and show that the dynamical information can be fully extracted from the covariance signal. Finally, this information is heavily suppressed upon averaging of noisy signals and practically inaccessible in conventional stimulated Raman measurements.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1609513
Alternate Identifier(s):
OSTI ID: 1568912; OSTI ID: 1864803
Grant/Contract Number:  
FG02-04ER15571; SC0019484; CHE-1663822
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 4; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; physics

Citation Formats

Osipov, V. Al., Asban, S., and Mukamel, S. Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light. United States: N. p., 2019. Web. doi:10.1063/1.5109258.
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Osipov, V. Al., Asban, S., & Mukamel, S. Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light. United States. https://doi.org/10.1063/1.5109258
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Osipov, V. Al., Asban, S., and Mukamel, S. Tue . "Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light". United States. https://doi.org/10.1063/1.5109258. https://www.osti.gov/servlets/purl/1609513.
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@article{osti_1609513,
title = {Time and frequency resolved transient-absorption and stimulated-Raman signals of stochastic light},
author = {Osipov, V. Al. and Asban, S. and Mukamel, S.},
abstractNote = {Covariance spectroscopy signals based on the transmission of broadband stochastic probe light undergoing a nonlinear optical process with matter are studied. The resulting signal depends on intensity correlation functions of the probe pulse. Application is made to transient absorption and stimulated Raman signals, where an ultraviolet pump and a delayed stochastically modulated infrared or optical Raman probe are used for monitoring vibrational excitations. We show that the stochastic properties of light can be exploited to circumvent the limitations on the joint temporal and spectral resolution of the signal. We study a model system with a time-dependent frequency and show that the dynamical information can be fully extracted from the covariance signal. Finally, this information is heavily suppressed upon averaging of noisy signals and practically inaccessible in conventional stimulated Raman measurements.},
doi = {10.1063/1.5109258},
journal = {Journal of Chemical Physics},
number = 4,
volume = 151,
place = {United States},
year = {Tue Jul 30 00:00:00 EDT 2019},
month = {Tue Jul 30 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5109258
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Cited by: 3 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) Schematic layout of the TA setup. The actinic pulse Ea excites the sample (S.) at time t = 0 and prepares it in the superposition |ν⟩⟨ν′|, the stochastic probe pulse arrives at time T, and the transmitted light is measured by detector (D.) at time t; levelmore » schemes [(b) and (c)] and loop diagrams [(d) and (e)] contributing to TA signal, ξ is the stochastic phase.« less
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