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arXiv:2211.16658 · Physical Review Letters

Quantum Light from Lossy Semiconductor Rydberg Excitons

Valentin Walther, Anders Søndberg Sørensen

Published Jul 21, 2023• 3 citations
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Abstract

The emergence of photonic quantum correlations is typically associated with emitters strongly coupled to a photonic mode. Here, we show that semiconductor Rydberg excitons, which are only weakly coupled to a free-space light mode can produce strongly antibunched fields, i.e., quantum light. This effect is fueled by a micron-scale excitation blockade between Rydberg excitons inducing pair-wise polariton scattering events. Photons incident on an exciton resonance are scattered into blue- and red-detuned pairs, which enjoy relative protection from absorption and thus dominate the transmitted light. We demonstrate that this effect persists in the presence of additional phonon coupling, strong nonradiative decay, and across a wide range of experimental parameters. Our results pave the way for the observation of quantum statistics from weakly coupled semiconductor excitons.

DOI
10.1103/physrevlett.131.033607

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The emergence of photonic quantum correlations is typically associated with emitters strongly coupled to a photonic mode. Here, we show that semiconductor Rydberg excitons, which are only weakly coupled to a free-space light mode can produce strongly antibunched fields, i.e., quantum light. This effect is fueled by a micron-scale excitation blockade between Rydberg excitons inducing pair-wise polariton scattering events. Photons incident on an exciton resonance are scattered into blue- and red-detuned pairs, which enjoy relative protection from absorption and thus dominate the transmitted light. We demonstrate that this effect persists in the presence of additional phonon coupling, strong nonradiative decay, and across a wide range of experimental parameters. Our results pave the way for the observation of quantum statistics from weakly coupled semiconductor excitons.
The quantum correlations between the beams generated by polariton pair scattering in a semiconductor microcavity above the parametric oscillation threshold are computed analytically. The influence of various parameters, including the cavity-exciton detuning, the intensity mismatch between the signal and idler beams, and the amount of spurious noise, is analyzed. We show that very strong quantum correlations between the signal and idler polaritons can be achieved. However, the quantum effects in the outgoing light fields are strongly reduced due to the large mismatch in the coupling of the signal and idler polaritons to the external photons.
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Abstract Rydberg excitons (analogues of Rydberg atoms in condensed matter systems) are highly excited bound electron-hole states with large Bohr radii. The interaction between them as well as exciton coupling to light may lead to strong optical nonlinearity, with applications in sensing and quantum information processing. Here, we achieve strong effective photon–photon interactions (Kerr-like optical nonlinearity) via the Rydberg blockade phenomenon and the hybridisation of excitons and photons forming polaritons in a Cu2O-filled microresonator. Under pulsed resonant excitation polariton resonance frequencies are renormalised 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 experimentally observed scaling of the polariton nonlinearity coefficient as ∝ n4.4±1.8 for principal quantum numbers up to n = 7. Such high principal quantum numbers studied in a polariton system for the first time are essential for realisation of high Rydberg optical nonlinearities, which paves the way towards quantum optical applications and fundamental studies of strongly correlated photonic (polaritonic) states in a solid state system.
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.
Investigations of quantum effects in semiconductor quantum-well microcavities interacting with laser light in the strong-coupling regime are presented. Modifications of quantum fluctuations of the outgoing light are expected due to the non-linearity originating from coherent exciton–exciton scattering. In the strong-coupling regime, this scattering translates into a four-wave mixing interaction between the mixed exciton–photon states, the polaritons. Squeezing and giant amplification of the polariton field and of the outgoing light field fluctuations are predicted. However, polariton–phonon scattering is shown to yield excess noise in the output field, which may destroy the non-classical effects. Experiments demonstrate evidence for giant amplification due to coherent four-wave mixing of polaritons. Noise reduction below the thermal noise level was also observed.
Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly nonclassical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditions of electromagnetically induced transparency and thereby provides an efficient mechanism for single-photon switching between high transmission and reflectance of the monolayer, with a tunable dynamical timescale of the emerging photon-photon interactions. Remarkably, it turns out that the resulting high degree of photon correlations remains virtually unaffected by Rydberg-state decoherence, in excess of nonradiative decoherence observed for ground-state excitons in two-dimensional semiconductors. This robustness to imperfections suggests a promising approach to quantum photonics at the level of individual photons.