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Title: Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs

Abstract

Two techniques that employ equally spaced trains of optical pulses to map an optical high frequency into a low frequency modulation of the signal that can be detected in real time are compared. The development of phase-stable optical frequency combs has opened up new avenues to metrology and spectroscopy. The ability to generate a series of frequency spikes with precisely controlled separation permits a fast, highly accurate sampling of the material response. Recently, pairs of frequency combs with slightly different repetition rates have been utilized to down-convert material susceptibilities from the optical to microwave regime where they can be recorded in real time. We show how this one-dimensional dual comb technique can be extended to multiple dimensions by using several combs. We demonstrate how nonlinear susceptibilities can be quickly acquired using this technique. In a second class of techniques, sequences of ultrafast mode locked laser pulses are used to recover pathways of interactions contributing to nonlinear susceptibilities by using a photo-acoustic modulation varying along the sequences. We show that these techniques can be viewed as a time-domain analog of the multiple frequency comb scheme.

Authors:
 [1];  [1];  [1]
  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)
OSTI Identifier:
1535342
Alternate Identifier(s):
OSTI ID: 1400011
Grant/Contract Number:  
FG02-04ER15571
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 9; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Chemistry; Physics

Citation Formats

Bennett, Kochise, Rouxel, Jeremy R., and Mukamel, Shaul. Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs. United States: N. p., 2017. Web. doi:10.1063/1.5000375.
Bennett, Kochise, Rouxel, Jeremy R., & Mukamel, Shaul. Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs. United States. doi:10.1063/1.5000375.
Bennett, Kochise, Rouxel, Jeremy R., and Mukamel, Shaul. Tue . "Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs". United States. doi:10.1063/1.5000375. https://www.osti.gov/servlets/purl/1535342.
@article{osti_1535342,
title = {Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs},
author = {Bennett, Kochise and Rouxel, Jeremy R. and Mukamel, Shaul},
abstractNote = {Two techniques that employ equally spaced trains of optical pulses to map an optical high frequency into a low frequency modulation of the signal that can be detected in real time are compared. The development of phase-stable optical frequency combs has opened up new avenues to metrology and spectroscopy. The ability to generate a series of frequency spikes with precisely controlled separation permits a fast, highly accurate sampling of the material response. Recently, pairs of frequency combs with slightly different repetition rates have been utilized to down-convert material susceptibilities from the optical to microwave regime where they can be recorded in real time. We show how this one-dimensional dual comb technique can be extended to multiple dimensions by using several combs. We demonstrate how nonlinear susceptibilities can be quickly acquired using this technique. In a second class of techniques, sequences of ultrafast mode locked laser pulses are used to recover pathways of interactions contributing to nonlinear susceptibilities by using a photo-acoustic modulation varying along the sequences. We show that these techniques can be viewed as a time-domain analog of the multiple frequency comb scheme.},
doi = {10.1063/1.5000375},
journal = {Journal of Chemical Physics},
number = 9,
volume = 147,
place = {United States},
year = {2017},
month = {9}
}

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