Optical cavities hold great promise to manipulate and control the photochemistry of molecules.

Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both linear and the nonlinear interferences can provide information regarding the light statistics and underlying detail of the light-matter interactions. Here we demonstrate how interferometric detection of nonlinear spectroscopic signals may be used to improve the measurement accuracy of matter susceptibilities. Light-matter interactions change the photon statistics of quantum light, which are encoded in the field correlation functions. Application is made to the Hong-Ou-Mandel two-photon interferometer that reveals entanglement-enhanced resolution that can be achieved with existing optical technology.

Quantum decoherence arises due to uncontrollable entanglement between a system and its environment. However, the effects of decoherence are often thought of and modeled through a simpler picture in which the role of the environment is to introduce classical noise in the system’s degrees of freedom. Here, we establish necessary conditions that the classical noise models need to satisfy to quantitatively model the decoherence. Specifically, for pure-dephasing processes, we identify well-defined statistical properties for the noise that are determined by the quantum many-point time correlation function of the environmental operators that enter into the system-bath interaction. In particular, for the exemplifying spin-boson problem with a Lorentz-Drude spectral density, we show that the high-temperature quantum decoherence is quantitatively mimicked by colored Gaussian noise. In turn, for dissipative environments, we show that classical noise models cannot describe decoherence effects due to relaxation through spontaneous emission of photons/phonons. These developments provide a rigorous platform to assess the validity of classical noise models of decoherence.

Placing aromatic molecules in a chiral optical cavity can break time-reversal symmetry and generate polariton ring currents with a linearly polarized pump. Such currents can be probed by circular dichroism, with one order of magnitude enhancement.