Probing excited-state dynamics with quantum entangled photons: Correspondence to coherent multidimensional spectroscopy

Abstract: Quantum light is a key resource for promoting quantum technology. One such class of technology aims to improve the precision of optical measurements using engineered quantum states of light. In this study, we investigate transmission measurement of frequency-entangled broadband photon pairs generated via parametric down-conversion with a monochromatic laser. It is observed that state-to-state dynamics in the system under study are temporally resolved by adjusting the path difference between the entangled twin beams when the entanglement time is sufficiently short. The non-classical photon correlation enables time-resolved spectroscopy with monochromatic pumping. It is further demonstrated that the signal corresponds to the spectral information along anti-diagonal lines of, for example, two-dimensional Fourier-transformed photon echo spectra. This correspondence inspires us to anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.