A Liquid-Core Fiber Platform for Classical and Entangled Two-Photon Absorption Measurements

We introduce a toluene-filled fiber platform for two-photon absorption measurements. By confining both the light and molecular sample inside the 5 μm hollow core of the fiber, we increase the distance over which the nonlinear light-matter interaction occurs. With only a 7.3 nL excitation volume, we measure classical two-photon absorption (C2PA) at an average laser power as low as 1.75 nW, which is a 45-fold improvement over a conventional free-space technique. We use this platform to attempt to measure entangled two-photon absorption (E2PA), a process with a limited regime where the quantum advantage is large. This regime arises due to a crossover from linear to quadratic scaling with photon flux as photon flux is increased. Recently, several teams of researchers have reported that E2PA cross-sections are much smaller than previously claimed. As a result, the linear scaling dominates at photon fluxes so low that it is extremely difficult or impossible to measure using conventional free-space techniques. In this report, we implement the first E2PA measurement using a waveguide. We see no evidence of E2PA, and we set an upper bound on the cross-section consistent with these recent reports.