4.6 Article

Vibrational Hyper-Raman Molecular Spectroscopy with Entangled Photons

Journal

ACS PHOTONICS
Volume 8, Issue 9, Pages 2722-2727

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.1c00777

Keywords

entangled photons; hyper-Raman spectroscopy; Liouville-space pathways; one-photon resonances

Funding

  1. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0020168]
  2. NSF [CHE-1953045]

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Time-energy entangled photons are used to calculate vibrational hyper-Raman signals of the organic chromophore Wu112. Compared to classical light, entangled-photon HR signal scales linearly with the SPDC pump field intensity, providing selectivity and allowing weak-field measurements on fragile samples.
Time-energy entangled photons produced by spontaneous parametric down-conversion (SPDC) are employed to calculate vibrational hyper-Raman (HR) signals of the conjugated organic chromophore Wu112. Compared with classical light, time-energy entanglement can provide selectivity of Liouville-space pathways and thus suppress the strong broad electronic-Raman background arising from one-photon resonances of the intermediate states. The entangled-photon HR signal scales linearly with the SPDC pump field intensity rather than quadratically for classical light, which allows weak-field measurements on fragile samples.

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