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Физик сэтгүүл

Spectroscopy with Polarization Controlled Entangled Photons for Detecting Orbital Excitation in Solids

P Munkhbaatar, Duger Ulam-Orgikh, J Vanchinkhuu

Published Mar 13, 2022• 0 citations
Publisher

Abstract

We propose an excitation-probe measurement method utilizing entangled photon pulses. The excitation-probe signal is dominated by stimulated Raman scattering as well as two-photon absorption when the time delay between the excitation pulse and the probe pulse is shorter than the pulseduration. This paper demonstrates that the two-photon-absorption signal can be suppressed when the photons of the pulses are entangled. The stimulated Raman scattering signal can be composed of many peaks distributed over broad photon energies owing to the transitions between numerous quantum states in complex materials. We also show that the desired peaks among the many peaks can be selected by controlling the thickness of the nonlinear crystal, the pump pulse center frequency,and the polarization of the excitation pulse and probe pulse.

DOI
10.22353/physics.v22i449.593

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Quantum entanglement offers an incredible resource for enhancing the sensing and spectroscopic probes. Here we develop a microscopic theory for the stimulated Raman scattering (SRS) using entangled photons. We demonstrate that the time-energy correlation of the photon pairs can optimize the signal for polyatomic molecules. Our results show that the spectral-line intensity of the entangled-photon SRS (ESRS) is of the same order of magnitude as the one for the entangled two-photon absorption (ETPA); the parameter window is thus identified to do so. Moreover, the vibrational coherence is found to play an important role for enhancing the ESRS against the ETPA intensity. Our work paves a firm road for extending the schemes of molecular spectroscopy with quantum light, based on the observation of the ETPA in experiments.
Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of incoming photons. Pathway-selectivity opens up new avenues for mapping photon into material entanglement. New material information, otherwise erased by interferences among pathways, is revealed.
Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by entangled photons. We demonstrate that the time-energy correlation of the photon pairs can optimize the signal for polyatomic molecules. Our results show that the spectral-line intensity of the entangled-photon SRS (ESRS) is of the same order of magnitude as the one for the entangled two-photon absorption (ETPA); the parameter window is thus identified to do so. Moreover, the vibrational coherence is found to play an important role for enhancing the ESRS against the ETPA intensity. Our work paves a firm road for extending the schemes of molecular spectroscopy with quantum light, based on the observation of the ETPA in experiments.
We find that stimulated Raman excitation of an atom by a two-photon pulse can be enhanced by orders of magnitude if the photons are simultaneously frequency correlated and spatially anticorrelated. That is, a correlated photon pair must have an inherent time delay between its constituent photons. This counterintuitive feature is a manifestation of the uncertainty principle, which yields that frequency-correlated photons cannot be time (spatially) correlated. This is opposite to two-photon absorption by a three-level atom, for which the enhancement occurs if photons in the pulse are frequency anticorrelated and spatially correlated, that is, photons in the pair simultaneously interact with the atom. Our findings can be useful for imaging and spectroscopy of biological samples which demand low illumination intensity.