Energy-time entanglement and intermediate state dynamics in two photon absorption

Abstract: It is well known that energy-time entanglement can enhance two photon absorption (TPA) by simultaneously optimizing the two photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between entanglement and the TPA rate depends on the coherences of intermediate states involved in the transition, making it a rather challenging task to identify universal features of TPA processes. In the present paper, we show that the theory can be simplified greatly by separating the two photon resonance from the temporal dynamics of the intermediate levels. The result is a description of the role of entanglement in the TPA process by a one-dimensional coherence in the Hilbert space defined by the arrival time difference of the two photons. Transformation into the frequency difference basis results in Kramers-Kronig relations for the TPA process, separating off-resonant contributions of virtual levels from resonant contributions. In particular, it can be shown that off-resonant contributions are insensitive to the frequencies of the associated virtual states, indicating that virtual-state spectroscopy of levels above the final two photon excited state is not possible.