Colors of entangled two-photon absorption

Author:

Varnavski Oleg1,Giri Sajal Kumar2,Chiang Tse-Min2,Zeman Charles J.2ORCID,Schatz George C.2ORCID,Goodson Theodore13

Affiliation:

1. Department of Chemistry, University of Michigan, Ann Arbor, MI 48109

2. Department of Chemistry, Northwestern University, Evanston, IL 60208-3113

3. Applied Physics, University of Michigan, Ann Arbor, MI 48109

Abstract

Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light–based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes.

Funder

DOD | USAF | AMC | Air Force Office of Scientific Research

National Science Foundation

U.S. Department of Energy

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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