Franson-Interferometric Bounds on Entangled Two-Photon Absorption

Abstract

Entangled photons offer quantum correlations with no classical analogue. In entangled pair two-photon absorption (ETPA), absorption rate is predicted to scale linearly rather than quadratically with photon flux, promising molecular excitation at fluxes far below the classical threshold. Reported ETPA cross sections nevertheless vary widely across experiments, largely since the observable, the differential of the transmitted flux or weak fluorescence, is difficult to separate from scattering and linear losses. We present a method which uses Franson interference to study entangled two-photon absorption through delay-dependent coincidence measurements on dye molecules. Applying the method to Rhodamine 6G, we observe a small asymmetry in the Franson interference envelope and obtain a model-derived effective cross section of approximately 2.1 E(-21) centimeter squared for Rhodamine 6G. However, the estimated systematic uncertainty does not allow a definitive ETPA assignment. Instead, the experiment establishes a quantitative bound on the ETPA response and provides a background-free benchmark for future measurements.