ABSTRACT
The detailed analysis of the sum-over-state formula for the entanglement-induced two-photon absorption (ETPA) transition moment shows that the magnitude of the ETPA cross-section is expected to vary significantly depending on the coherence time Te and the relative position of just two electronic states. Moreover, the dependency on Te is periodic. These predictions are confirmed by molecular quantum mechanical calculations for several chromophores.
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.