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Conference on Lasers and Electro-Optics

Experimental Bounds on Entangled Two Photon Absorption in Rhodamine 6G

Tiemo S. Landes, Markus Allgaier, Sofiane Merkouche, Brian J. Smith, Andrew H. Marcus, Michael G. Raymer

Published Jan 1, 2021• 2 citations
Publisher

Abstract

Entangled photons have been reported to enhance two-photon absorption by many orders of magnitude. Recent theoretical work predicts smaller increases for common molecular dyes. We present experimental results supporting this claim in Rhodamine 6G.
DOI
10.1364/cleo_qels.2021.fm3n.3

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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.
We experimentally study entangled two-photon absorption in rhodamine 6G as a function of the spatial properties of a high flux of broadband entangled photon pairs. We first demonstrate a key signature dependence of the entangled two-photon absorption rate on the type of entangled pair flux attenuation: linear, when the laser pump power is attenuated, and quadratic, when the pair flux itself experiences linear loss. We then perform a fluorescence-based Z-scan measurement to study the influence of beam waist size on the entangled two-photon absorption process and compare this to classical single- and two-photon absorption processes. We demonstrate that the entangled two-photon absorption shares a beam waist dependence similar to that of classical two-photon absorption. This result presents an additional argument for the wide range of contrasting values of quoted entangled two-photon absorption cross sections of dyes in literature.
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Nonlinear spectroscopy and microscopy techniques are ubiquitous in a wide range of applications across physics and biology. However, these usually rely on high-powered pulsed laser systems. A promising alternative is to exploit entangled two-photon absorption (ETPA), which can lead to tens of orders of magnitude lower incident fluxes than in conventional two-photon absorption schemes. However, the role of different entangled degrees of freedom in ETPA was unclear following recent experimental studies, when compared to earlier theoretical works. Here, we first demonstrate a linear dependence of the ETPA rate with the photon-pair rate, a clear signature of ETPA, and estimate the values for the concentration-dependent ETPA cross section for Rhodamine 6G. We then investigate the signature of energy-time entanglement and polarization dependence in the ETPA fluorescence rate and demonstrate a strong dependence of the signal on the interphoton delay that reflects the coherence time of the entangled two-photon wave packet.