14 Mar 2024 | Maxim Makhonin, Anthonin Delphan, Kok Wee Song, Paul Walker, Tommi Isoniemi, Peter Claronino, Konstantinos Orfanakis, Sai Kiran Rajendran, Hamid Ohadi, Julian Heckötter, Marc Assmann, Manfred Bayer, Alexander Tartakovskii, Maurice Skolnick, Oleksandr Kyriienko and Dmitry Krizhanovskii
The study investigates the nonlinear optical properties of Rydberg exciton-polaritons in Cu₂O microcavities. Rydberg excitons, highly excited bound electron-hole states with large Bohr radii, exhibit strong optical nonlinearity due to their interaction and coupling to light. The researchers achieve strong effective photon-photon interactions (Kerr-like optical nonlinearity) through the Rydberg blockade phenomenon and the hybridization of excitons and photons forming polaritons in Cu₂O-filled microresonators. Under pulsed resonant excitation, the polariton resonance frequencies are renormalized due to the reduction of the photon-exciton coupling with increasing exciton density. Theoretical analysis shows that the Rydberg blockade plays a major role in the observed scaling of the polariton nonlinearity coefficient as ∝ n⁴.⁴±1.⁸ for principal quantum numbers up to n = 7. This high principal quantum number is essential for realizing high Rydberg optical nonlinearities, paving the way for quantum optical applications and fundamental studies of strongly-correlated photonic (polaritonic) states in a solid-state system. The study also reports strong and ultra-fast nonlinear optical responses, with the nonlinearity scaling highly superlinearly with the principal quantum number. The nonlinear indices n₂ are found to be in the range from 10⁻¹⁷ m²/W to 4 × 10⁻¹⁵ m²/W for n = 3 to n = 7. Single-pulse experiments reveal picosecond rise and fall times for the nonlinearity, followed by additional dynamics on density-dependent timescales of order 100 ps to 2 ns. Theoretical models are developed to explain the observed experimental behavior, considering contributions from Rydberg and Pauli blockade. The study concludes that Rydberg polaritons in Cu₂O are a suitable platform for quantum polaritonics with nonlinearities scaling strongly with Rydberg exciton quantum numbers, reaching single-polariton nonlinearity.The study investigates the nonlinear optical properties of Rydberg exciton-polaritons in Cu₂O microcavities. Rydberg excitons, highly excited bound electron-hole states with large Bohr radii, exhibit strong optical nonlinearity due to their interaction and coupling to light. The researchers achieve strong effective photon-photon interactions (Kerr-like optical nonlinearity) through the Rydberg blockade phenomenon and the hybridization of excitons and photons forming polaritons in Cu₂O-filled microresonators. Under pulsed resonant excitation, the polariton resonance frequencies are renormalized due to the reduction of the photon-exciton coupling with increasing exciton density. Theoretical analysis shows that the Rydberg blockade plays a major role in the observed scaling of the polariton nonlinearity coefficient as ∝ n⁴.⁴±1.⁸ for principal quantum numbers up to n = 7. This high principal quantum number is essential for realizing high Rydberg optical nonlinearities, paving the way for quantum optical applications and fundamental studies of strongly-correlated photonic (polaritonic) states in a solid-state system. The study also reports strong and ultra-fast nonlinear optical responses, with the nonlinearity scaling highly superlinearly with the principal quantum number. The nonlinear indices n₂ are found to be in the range from 10⁻¹⁷ m²/W to 4 × 10⁻¹⁵ m²/W for n = 3 to n = 7. Single-pulse experiments reveal picosecond rise and fall times for the nonlinearity, followed by additional dynamics on density-dependent timescales of order 100 ps to 2 ns. Theoretical models are developed to explain the observed experimental behavior, considering contributions from Rydberg and Pauli blockade. The study concludes that Rydberg polaritons in Cu₂O are a suitable platform for quantum polaritonics with nonlinearities scaling strongly with Rydberg exciton quantum numbers, reaching single-polariton nonlinearity.