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Title: Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4986069· OSTI ID:1393442

Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We also explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picture that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. Our simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.

Research Organization:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0002162; FG02-09ER46664
OSTI ID:
1393442
Alternate ID(s):
OSTI ID: 1377970
Journal Information:
Journal of Chemical Physics, Vol. 147, Issue 8; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

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