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European Light Microscopy Initiative Meeting (ELMI)

Entangled Two-Photon Absorption in Commercial Fluorophores

Nitish Jain

Published Jun 22, 2021• 0 citations
Publisher
DOI
10.22443/rms.elmi2021.66

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We present an ongoing experiment to investigate the potential enhancement of the two-photon absorption (TPA) rate of an atom using time–frequency-entangled photon pairs, a process known as entangled two-photon absorption (ETPA). There has been significant debate in the literature regarding the existence and magnitude of such enhancement. Previous studies have primarily focused on ETPA in molecular fluorophores, which are relevant for biological imaging applications but typically exhibit relatively low two-photon cross sections, often not exceeding 10⁻⁵⁰ cm⁴s/photon. In this work, we sacrifice broad applicability for experimental practicality, and instead probe ETPA in rubidium vapor, which has a comparatively large two-photon cross section (∼10⁻¹⁸ cm⁴s/photon) relative to most molecular fluorophores used in prior studies. We have developed and characterized an entangled photon-pair source, and have observed two-photon absorption in rubidium vapor. We have also reproduced previous theoretical models of ETPA. Preliminary results are presented, along with a discussion of the future direction of the experiment.
Excitation with entangled photon pairs may lead to an increase in the efficiency of two-photon absorption at low photon flux. The corresponding process, entangled two-photon absorption (E2PA), has been investigated in numerous theoretical and experimental studies. However, significant ambiguity and inconsistency remain in the literature about the absolute values of E2PA cross sections. Here, we use a fluorescence-based registration scheme to experimentally determine upper bounds on the cross sections for six fluorophores. These bounds are up to 4 orders of magnitude lower than the smallest published cross section. For two samples that have been studied by others, Rhodamine 6G and 9R-S, we measure upper bounds 4 and 5 orders of magnitude lower than the previously reported cross sections.