Experimental feasibility of molecular two-photon absorption with isolated time-frequency-entangled photon pairs

Landes, Tiemo; Allgaier, Markus; Merkouche, Sofiane; Smith, Brian J.; Marcus, Andrew H.; Raymer, Michael G.

doi:10.1103/PhysRevResearch.3.033154

We investigate the interaction of weak light fields with two-dimensional lattices of atoms with high lying atomic Rydberg states. This system features different interactions that act on disparate length scales, from zero-range defect scattering of atomic excitations and finite-range dipole exchange processes to long-range Rydberg-state interactions, which span the entire array and can block multiple Rydberg excitations. Analyzing their interplay, we identify conditions that yield a nonlinear quantum mirror which coherently splits incident fields into correlated photon-pairs in a single transverse mode, while transmitting single photons unaffected. In particular, we find strong anti-bunching of the transmitted light with equal-time pair correlations that decrease exponentially with an increasing range of the Rydberg blockade. Such strong photon-photon interactions in the absence of photon losses open up promising avenues for the generation and manipulation of quantum light, and the exploration of many-body phenomena with interacting photons.

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