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Title: Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles

Nonlinear spectroscopy signals detected by fluorescence from dilute samples of N non-interacting molecules are usually adequately described by simply multiplying the single molecule response by N. Here, we show that signals that scale with higher powers of N are generated by the joint detection of several particles. This can be accomplished by phase sensitive detection such as phase cycling, photo-acoustic modulation, or by Hanbury-Brown Twiss photon coincidence. Such measurements can dissect the ensemble according to the number of excited particles.
Authors:
 [1]
  1. Univ. of California, Irvine, CA (United States). Dept. of Chemistry and Dept. of Physics and Astronomy
Publication Date:
Grant/Contract Number:
FG02-04ER15571; CHE-1361516
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 4; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Univ. of California, Irvine, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS; nonlinear optics; fluorescence; excited states; photons; optical coherence; fourier transforms; signal coherence; single molecule techniques; nonlinear spectroscopy; quantum coherence
OSTI Identifier:
1467860
Alternate Identifier(s):
OSTI ID: 1275975

Mukamel, Shaul. Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles. United States: N. p., Web. doi:10.1063/1.4960049.
Mukamel, Shaul. Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles. United States. doi:10.1063/1.4960049.
Mukamel, Shaul. 2016. "Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles". United States. doi:10.1063/1.4960049. https://www.osti.gov/servlets/purl/1467860.
@article{osti_1467860,
title = {Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles},
author = {Mukamel, Shaul},
abstractNote = {Nonlinear spectroscopy signals detected by fluorescence from dilute samples of N non-interacting molecules are usually adequately described by simply multiplying the single molecule response by N. Here, we show that signals that scale with higher powers of N are generated by the joint detection of several particles. This can be accomplished by phase sensitive detection such as phase cycling, photo-acoustic modulation, or by Hanbury-Brown Twiss photon coincidence. Such measurements can dissect the ensemble according to the number of excited particles.},
doi = {10.1063/1.4960049},
journal = {Journal of Chemical Physics},
number = 4,
volume = 145,
place = {United States},
year = {2016},
month = {7}
}