Pathway Selectivity in 2D Electronic‐Vibrational Spectroscopy with Quantum Light

Jadoun, Deependra [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA] (ORCID:0000000333059140); Yadalam, Hari K. [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]; Harbola, Upendra [Department of Inorganic and Physical Chemistry Indian Institute of Science Bangalore 560012 India]; Chernyak, Vladimir Y. [Department of Chemistry Wayne State University 5101 Cass Ave Detroit MI 48202 USA, Department of Mathematics Wayne State University 656 W. Kirby Detroit MI 48202 USA]; Kizmann, Matthias [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]; Mukamel, Shaul [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]

doi:10.1002/lpor.202401576

DOE OSTI · 2500929

Pathway Selectivity in 2D Electronic‐Vibrational Spectroscopy with Quantum Light

Jadoun, Deependra [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA] (ORCID:0000000333059140)·Yadalam, Hari K. [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]·Harbola, Upendra [Department of Inorganic and Physical Chemistry Indian Institute of Science Bangalore 560012 India]·Chernyak, Vladimir Y. [Department of Chemistry Wayne State University 5101 Cass Ave Detroit MI 48202 USA, Department of Mathematics Wayne State University 656 W. Kirby Detroit MI 48202 USA]·Kizmann, Matthias [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]·Mukamel, Shaul [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]

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Abstract

Abstract Pathway selectivity in quantum spectroscopy with entangled photons is a powerful spectroscopic tool. Phase‐matched signals involving classical light contain contributions from multiple material pathways, whereas quantum spectroscopy may allow the selection of individual pathways. 2D electronic‐vibrational spectroscopy (2DEVS) is a four‐wave mixing technique which employs visible and infrared entangled photons. It is showed how the three contributing pathways—ground state bleach, excited state absorption, and excited state emission—can be separated by photon‐number‐resolved coincidence measurements. Entangled photons thus reveal spectral features not visible in the classical signal, with an enhanced spectral resolution.

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Jadoun, Deependra [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA] (ORCID:0000000333059140), Yadalam, Hari K. [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA], Harbola, Upendra [Department of Inorganic and Physical Chemistry Indian Institute of Science Bangalore 560012 India], Chernyak, Vladimir Y. [Department of Chemistry Wayne State University 5101 Cass Ave Detroit MI 48202 USA, Department of Mathematics Wayne State University 656 W. Kirby Detroit MI 48202 USA], Kizmann, Matthias [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA], Mukamel, Shaul [Department of Chemistry University of California Irvine CA 92614 USA, Department of Physics and Astronomy University of California Irvine CA 92614 USA]. 2025-01-15. Pathway Selectivity in 2D Electronic‐Vibrational Spectroscopy with Quantum Light. https://doi.org/10.1002/lpor.202401576

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