Time-and-frequency-gated photon coincidence counting; a novel multidimensional spectroscopy tool

Coherent multidimensional optical spectroscopy is broadly applied across the electromagnetic spectrum ranging from NMR to UV. These techniques reveal the properties of matter through the correlation plots of signal fields generated in response to sequences of short pulses with variable delays. Here we discuss a new class of multidimensional techniques obtained by the time-and-frequency-resolved photon coincidence counting measurements of N photons, which constitute a dimensional spectrum. A compact description of these signals is developed based on time-ordered superoperators rather than the normally ordered ordinary operators used in Glauber's photon counting formalism. The independent control of the time and frequency gate parameters reveals fine details of matter dynamics not available otherwise. These signal are illustrated for application to an anharmonic oscillator model with fluctuating energy and anharmonicity.