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When a low flux of time-frequency-entangled photon pairs (EPP) illuminates atwo-photon transition, the rate of two-photon absorption (TPA) can be enhancedconsiderably by the quantum nature of photon number correlations and frequencycorrelations. We present a quantum-theoretic derivation of entangled TPA (ETPA)and calculate an upper bound on the amount of quantum enhancement that ispossible in such systems. The derived bounds indicate that in order to observeETPA the experiments would need to operate at a combination of significantlyhigher rates of EPP illumination, molecular concentrations, and conventionalTPA cross sections than are achieved in typical experiments.

Quantifying the enhancement of two-photon absorption due to spectral-temporal entanglement