Single-Photon Scattering Can Account for the Discrepancies among Entangled Two-Photon Measurement Techniques
Abstract
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.
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.Attached Files
Supplemental Material - jz2c00865_si_001.pdf
Supplemental Material - jz2c00865_si_002.pdf
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Additional details
- Eprint ID
- 114969
- Resolver ID
- CaltechAUTHORS:20220531-843956000
- Department of Energy (DOE)
- DE-SC0020151
- Created
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2022-06-01Created from EPrint's datestamp field
- Updated
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2022-06-30Created from EPrint's last_modified field