Spatial Properties of Entangled Two-Photon Absorption

Phys Rev Lett. 2022 Oct 28;129(18):183601. doi: 10.1103/PhysRevLett.129.183601.

Abstract

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.