Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy

Yadalam, Hari Kumar; Kizmann, Matthias; Rouxel, Jérémy R.; Nam, Yeonsig; Chernyak, Vladimir Y.; Mukamel, Shaul

doi:10.1021/acs.jpclett.3c02341

Title: Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy

Journal Article · 28 November 2023 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.3c02341 · OSTI ID:2350694

^[1]; Kizmann, Matthias ^[1];

^[2];

^[1]; Chernyak, Vladimir Y. ^[3];

^[1]

Univ. of California, Irvine, CA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Wayne State Univ., Detroit, MI (United States)

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. Importantly, this additional selectivity originates from engineering the state of light using a Zou–Wang–Mandel interferometer combined with coincidence detection.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; SC0022134

OSTI ID:: 2350694

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 48 Vol. 14; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy

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