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This content will become publicly available on August 31, 2018

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

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.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ;  [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
SC0002162; FG02-09ER46664
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 8; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE
OSTI Identifier:
1393442
Alternate Identifier(s):
OSTI ID: 1377970