Pathway selectivity in time-resolved spectroscopy using two-photon coincidence counting with quantum entangled photons

Fuente: arXiv
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Hauptverfasser: Fujihashi, Yuta, Ishizaki, Akihito, Shimizu, Ryosuke
Format: Preprint
Veröffentlicht: 2023
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author Fujihashi, Yuta
Ishizaki, Akihito
Shimizu, Ryosuke
author_facet Fujihashi, Yuta
Ishizaki, Akihito
Shimizu, Ryosuke
contents Ultrafast optical spectroscopy is a powerful technique for studying the dynamic processes of molecular systems in condensed phases. However, in molecular systems containing many dye molecules, the spectra can become crowded and difficult to interpret owing to the presence of multiple nonlinear optical contributions. In this work, we theoretically propose time-resolved spectroscopy based on the coincidence counting of two entangled photons generated via parametric down-conversion with a monochromatic laser. We demonstrate that the use of two-photon counting detection of entangled photon pairs enables the selective elimination of the excited-state absorption signal. This selective elimination cannot be realized with classical coherent light. We anticipate that the proposed spectroscopy will help to simplify the spectral interpretation in complex molecular and materials systems comprising multiple molecules.
format Preprint
id arxiv_https___arxiv_org_abs_2311_16408
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Pathway selectivity in time-resolved spectroscopy using two-photon coincidence counting with quantum entangled photons
Fujihashi, Yuta
Ishizaki, Akihito
Shimizu, Ryosuke
Chemical Physics
Ultrafast optical spectroscopy is a powerful technique for studying the dynamic processes of molecular systems in condensed phases. However, in molecular systems containing many dye molecules, the spectra can become crowded and difficult to interpret owing to the presence of multiple nonlinear optical contributions. In this work, we theoretically propose time-resolved spectroscopy based on the coincidence counting of two entangled photons generated via parametric down-conversion with a monochromatic laser. We demonstrate that the use of two-photon counting detection of entangled photon pairs enables the selective elimination of the excited-state absorption signal. This selective elimination cannot be realized with classical coherent light. We anticipate that the proposed spectroscopy will help to simplify the spectral interpretation in complex molecular and materials systems comprising multiple molecules.
title Pathway selectivity in time-resolved spectroscopy using two-photon coincidence counting with quantum entangled photons
topic Chemical Physics
url https://arxiv.org/abs/2311.16408