Two-photon absorption cross sections of pulsed entangled beams

Abstract: Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to overlap temporally, accidental coincidences are thought to give rise to a 'classical' quadratic scaling which dominates the signal at large photon fluxes and thus recovers a supposedly classical regime, where any quantum advantage is thought to be lost. Here we scrutinize this assumption and demonstrate that quantum-enhanced absorption cross sections can persist even to very large photon numbers. To this end, we use a minimal model for quantum light, which can interpolate continuously between the entangled pair and a high-photon-flux limit, to derive analytically ETPA cross sections and the intensity crossover regime. We investigate the interplay between spectral and spatial degrees of freedom, how linewidth broadening of the sample impacts the experimentally achievable enhancement.