Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy.

Autor:	Yadalam HK; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States., Kizmann M; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States., Rouxel JR; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Nam Y; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States., Chernyak VY; Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, Michigan 48202, United States.; Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202, United States., Mukamel S; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States.
Jazyk:	angličtina
Zdroj:	The journal of physical chemistry letters [J Phys Chem Lett] 2023 Dec 07; Vol. 14 (48), pp. 10803-10809. Date of Electronic Publication: 2023 Nov 28.
DOI:	10.1021/acs.jpclett.3c02341
Abstrakt:	Even-order spectroscopies such as sum-frequency generation (SFG) and difference-frequency generation (DFG) can serve as direct probes of molecular chirality. Such signals are usually given by the sum of several interaction pathways that carry different information about matter. Here we focus on DFG, involving impulsive optical-optical-IR interactions, where the last IR pulse probes vibrational transitions in the ground or excited electronic state manifolds, depending on the interaction pathway. Spectroscopy with classical light can use phase matching to select the two pathways. In this theoretical study, we propose a novel quantum interferometric protocol that uses entangled photons to isolate individual pathways. This additional selectivity originates from engineering the state of light using a Zou-Wang-Mandel interferometer combined with coincidence detection.
Databáze:	MEDLINE
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