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Title: Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light

Abstract

Homodyne X-ray diffraction signals produced by classical light and classical detectors are given by the modulus square of the charge density in momentum space |σ(q)|2, missing its phase, which is required in order to invert the signal to real space. We show that quantum detection of the radiation field yields a linear diffraction pattern that reveals σ(q) itself, including the phase. We further show that repeated diffraction measurements with variable delays constitute a novel multidimensional measure of spontaneous charge-density fluctuations. Classical diffraction, in contrast, only reveals a subclass of even-order correlation functions. Simulations of two-dimensional signals obtained by two diffraction events are presented for the amino acid cysteine.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. East China Normal Univ., Shanghai (China)
  2. Univ. of California, Irvine, CA (United States)
  3. École Polytechnique Fédérale de Lausanne (Switzerland); Paul Scherrer Inst. (Switzerland)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1922844
Grant/Contract Number:  
SC0019484; FG02-04ER15571; CHE-1663822
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 4; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electrical properties; Light; Molecules; Phase transitions; Physical and chemical processes

Citation Formats

Dorfman, Konstantin E., Asban, Shahaf, Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, and Mukamel, Shaul. Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.9b00071.
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Dorfman, Konstantin E., Asban, Shahaf, Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, & Mukamel, Shaul. Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light. United States. https://doi.org/10.1021/acs.jpclett.9b00071
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Dorfman, Konstantin E., Asban, Shahaf, Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, and Mukamel, Shaul. Thu . "Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light". United States. https://doi.org/10.1021/acs.jpclett.9b00071. https://www.osti.gov/servlets/purl/1922844.
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@article{osti_1922844,
title = {Monitoring Spontaneous Charge-Density Fluctuations by Single-Molecule Diffraction of Quantum Light},
author = {Dorfman, Konstantin E. and Asban, Shahaf and Ye, Lyuzhou and Rouxel, Jérémy R. and Cho, Daeheum and Mukamel, Shaul},
abstractNote = {Homodyne X-ray diffraction signals produced by classical light and classical detectors are given by the modulus square of the charge density in momentum space |σ(q)|2, missing its phase, which is required in order to invert the signal to real space. We show that quantum detection of the radiation field yields a linear diffraction pattern that reveals σ(q) itself, including the phase. We further show that repeated diffraction measurements with variable delays constitute a novel multidimensional measure of spontaneous charge-density fluctuations. Classical diffraction, in contrast, only reveals a subclass of even-order correlation functions. Simulations of two-dimensional signals obtained by two diffraction events are presented for the amino acid cysteine.},
doi = {10.1021/acs.jpclett.9b00071},
journal = {Journal of Physical Chemistry Letters},
number = 4,
volume = 10,
place = {United States},
year = {Thu Jan 24 00:00:00 EST 2019},
month = {Thu Jan 24 00:00:00 EST 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.jpclett.9b00071
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