Quantum theory of single-photon nonlinearities generated by ensembles of emitters

The achievement of sufficiently fast interactions between two optical fields at the few-photon level would provide a key enabler for a broad range of quantum technologies. One critical hurdle in this endeavor is the lack of a comprehensive quantum theory of the generation of nonlinearities by ensembles of emitters. Distinct approaches applicable to different regimes have yielded important insights: i) a semiclassical approach reveals that, for many-photon coherent fields, the contributions of independent emitters add independently allowing ensembles to produce strong optical nonlinearities via EIT; ii) a quantum analysis has shown that in the few-photon regime collective coupling effects prevent ensembles from inducing these strong nonlinearities. Rather surprisingly, experimental results with around twenty photons are in line with the semi-classical predictions. Theoretical analysis has been fragmented due to the difficulty of treating nonlinear many-body quantum systems. Here we are able to solve this problem by constructing a powerful theory of the generation of optical nonlinearities by single emitters and ensembles. The key to this construction is the application of perturbation theory to perturbations generated by subsystems. This theory reveals critical properties of ensembles that have long been obscure. The most remarkable of these is the discovery that quantum effects prevent ensembles generating single-photon nonlinearities only within the rotating-wave regime; outside this regime single-photon nonlinearities scale as the number of emitters. The theory we present here also provides an efficient way to calculate nonlinearities for arbitrary multi-level driving schemes, and we expect that it will prove a powerful foundation for further advances in this area.Comment: 21 pages, Revtex4-2, 4 png figures, 1 supplement fil