Enhancing entangled two-photon absorption of Nile Red via temperature-controlled SPDC

Abstract: Entangled two-photon absorption can enable a linear scaling of fluorescence emission with the excitation power. In comparison to classical two-photon absorption with a quadratic scaling, this can allow fluorescence imaging or photolithography with high axial resolution at minimal exposure intensities. However, most experimental studies on two-photon absorption were not able to show an unambiguous proof of fluorescence emission driven by entangled photon pairs. On the other hand, existing theoretical models struggle to accurately predict the entangled two-photon absorption behavior of chemically complex dyes. In this paper, we introduce an approach to simulate entangled two-photon absorption in common fluorescence dyes considering their chemical properties. Our theoretical model allows a deeper understanding of experimental results and thus the occurrence of entangled two-photon absorption. In particular, we found a remarkable dependency of the absorption probability on the phase-matching temperature of the nonlinear material. Further, we compared results of our theoretical approach to experimental data for Nile Red.