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

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/1.5109258 · OSTI ID:1609513

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.

Research Organization:
Univ. of California, Irvine, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
FG02-04ER15571; SC0019484; CHE-1663822
OSTI ID:
1609513
Alternate ID(s):
OSTI ID: 1568912; OSTI ID: 1864803
Journal Information:
Journal of Chemical Physics, Vol. 151, Issue 4; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

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Figures / Tables (10)