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Single-Photon Scattering Can Account for the Discrepancies among Entangled Two-Photon Measurement Techniques

Hickam, Bryce P. and He, Manni and Harper, Nathan and Szoke, Szilard and Cushing, Scott K. (2022) Single-Photon Scattering Can Account for the Discrepancies among Entangled Two-Photon Measurement Techniques. Journal of Physical Chemistry Letters, 13 (22). pp. 4934-4940. ISSN 1948-7185. doi:10.1021/acs.jpclett.2c00865.

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Entangled photon pairs are predicted to linearize and increase the efficiency of two-photon absorption, allowing continuous wave laser diodes to drive ultrafast time-resolved spectroscopy and nonlinear processes. Despite a range of theoretical studies and experimental measurements, inconsistencies in the value of the entanglement-enhanced interaction cross section persist. A spectrometer that can temporally and spectrally characterize the entangled photon state before, during, and after any potential two-photon excitation event is constructed. For the molecule rhodamine 6G, which has a virtual state pathway, any entangled two-photon interaction is found to be equal to or weaker than classical, single-photon scattering events. This result can account for the discrepancies among the wide variety of entangled two-photon absorption cross sections reported from different measurement techniques. The reported instrumentation can unambiguously separate classical and entangled effects and therefore is important for the growing field of nonlinear and multiphoton entangled spectroscopy.

Item Type:Article
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Hickam, Bryce P.0000-0003-2120-4769
Cushing, Scott K.0000-0003-3538-2259
Additional Information:© 2022 American Chemical Society. Received: March 24, 2022; Accepted: May 25, 2022; Published: May 30, 2022. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Grant DE-SC0020151 (S.K.C.). This report was prepared as an account of work sponsored by an agency of the U.S. Government. Neither the U.S. Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the U.S. Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the U.S. Government or any agency thereof. Author Contributions. B.P.H. and M.H. contributed equally to this work. The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0020151
Subject Keywords:Absorption spectroscopy, Fluorescence, Mass spectrometers, Molecules, Scattering
Issue or Number:22
Record Number:CaltechAUTHORS:20220531-843956000
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Official Citation:Single-Photon Scattering Can Account for the Discrepancies among Entangled Two-Photon Measurement Techniques. Bryce P. Hickam, Manni He, Nathan Harper, Szilard Szoke, and Scott K. Cushing. The Journal of Physical Chemistry Letters 2022 13 (22), 4934-4940; DOI: 10.1021/acs.jpclett.2c00865
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114969
Deposited By: George Porter
Deposited On:01 Jun 2022 17:27
Last Modified:30 Jun 2022 16:14

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