Quantum-Light Multidimensional Spectroscopy of Molecules

Quantum states of the light, e.g., single photons, entanglement and squeezing, opens up a new avenue for spectroscopy by utilizing the parameters of quantum optical fields as novel control knobs and through the variation of photon statistics. With the advance of cavity quantum electrodynamics and light source technology, imaging and controlling the electron and vibrational motions of molecules can be achieved, towards unprecedented resolution and precision, not accessible by the classical light pulses [1]. In this talk, I will present our recent works on multidimensional spectroscopy using quantum states of light. Several schemes will be discussed: multidimensional coherent probe and Raman spectra with quantum optical fields [2,3,4]. Microscopic models for molecular relaxation using density matrix will be incorporated for a unified understanding of the signals.