Two-photon absorption (TPA) is a nonlinear optical process with wide applications in fluorescence microscopy and spectroscopy of organic molecules and compounds, as it enables atoms or molecules to transition into states that may otherwise be inaccessible by a single photon, either because of selection rules or energy conservation. Despite its common use, TPA is a rather inefficient process, often requiring very large photon numbers to produce significant results. It has been demonstrated and analytically described [1,2], that using frequency entangled pairs of photons can in some cases enhance the efficiency of TPA. For this to occur, the joint spectral amplitude (JSA) of the photon-pair state, which describes the spectral entanglement between the pair, must be engineered according to the spectral properties of the TPA response-function of the specific system in question. In this work, we consider different cases for the spectral functionality of TPA and propose that the control of the group indices of the modes involved in the pair-generation process is a key property in the design of photon-pair sources for optimized TPA.
We present a source of near-infrared photon pairs based on the process of spontaneous parametric downconversion (SPDC), for which the joint signal-idler quantum state is designed to be factorable in the frequency-time and in the transverse position-momentum degrees of freedom. Our technique is based on the use of a broadband pump and vector group velocity matching between the pump, signal, and idler waves. We show experimentally that a source based on this technique can be configured for the generation of: i) pure heralded single photons, and ii) polarization-entangled photon pairs which are free from spectral correlations, in both cases without resorting to spectral filtering. While critical for many applications in optical quantum information processing, such a source has not previously been demonstrated.