Entangled Two-Photon Absorption Spectroscopy with Varying Pump Wavelength

In virtual-state spectroscopy, information about the energy-level structure of an arbitrary sample is retrieved by Fourier transforming sets of measured two-photon absorption probabilities of entangled photon pairs where the degree of entanglement and the delay time between the photons have been varied. This works well for simple systems but quickly becomes rather difficult when many intermediate states are involved. We propose and discuss an extension of entangled two-photon absorption spectroscopy that solves this problem by means of repeated measurements at different pump wavelengths. Specifically, we demonstrate that our extension works well for a variety of realistic experimental setups.