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arXiv:2401.02868 · Light Science & Applications

Nonlinear Rydberg exciton-polaritons in Cu2O microcavities

M. N. Makhonin, Anthonin Delphan, Kok Wee Song, Paul M. Walker, Tommi Isoniemi, Peter Claronino, Konstantinos Orfanakis, Sai Kiran Rajendran, Hamid Ohadi, Julian Heckötter, Marc Aßmann, M. Bayer, A. I. Tartakovskii, Maurice S. Skolnick, Oleksandr Kyriienko, Dmitry N. Krizhanovskii

Published Feb 6, 2024• 22 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/s41377-024-01382-9

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Mapping the strong interaction between Rydberg excitations in ultra-cold atomic ensembles onto single photons enables the realization of optical nonlinearities which can modify light on the level of individual photons.This novel approach forms the basis of a growing Rydberg quantum optics toolbox, which already contains photonic logic building-blocks such as single-photon sources, switches, transistors, and conditional π-phase shifts.This thesis reports on two experiments investigating strong photon-photon interactions mediated by Rydberg interactions.First, applying a ladder-type EIT scheme to Rydberg atoms in D-states with high principal quantum number results in the Rydberg interaction mediated nonlinearity accompanied by a time-dependent decay of transmission of probe light through the medium.In a joint experimental and theoretical analysis, this effect is attributed to the dephasing of propagating polaritons into stationary Rydberg excitations caused by the state mixing interaction occurring with Rydberg D-state atoms.Second, via a two-photon Raman excitation scheme Rydberg atoms are efficiently excited in a small atomic cloud.As the size of the Rydberg blockade exceeds the dimension of the medium, only a single Rydberg excitation can be present at a time.By fast engineered dephasing this Rydberg excitation is decoupled from the light field.Measurement of the transmitted light and the amount of excited Rydberg atoms gives evidence for the realization of a deterministic single-photon absorber.

•Jan 1, 2017•2 citations
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.
Abstract Within the last few years, Rydberg excitons, bound electron–hole pairs in highly excited states, have emerged as a promising technology platform for quantum nonlinear optics, quantum information processing, and quantum sensing. The advanced device designs and sensing concepts in these fields require strong nonlinearities at the few-photon or few-carrier level. Rydberg states offer the required strong nonlinearities as the relevant physical quantities at the heart of such nonlinear effects scale strongly with the principal quantum number, n, of the excited state: For example, their polarizability scales as n7n^7n7 n 7 , resulting in an enormous sensitivity to external fields. We review recent experimental and theoretical results that pave the way toward quantum sensing of the electric fields originating from static charge carriers and strongly diluted electron–hole plasmas. We also discuss the strong nonlinear optical properties of Rydberg excitons and how they could be utilized in terms of sensing. Graphical abstract
Hosting giant Rydberg excitons with principal quantum numbers up to n = 30, cuprous oxide (Cu2O) provides a rare solid-state setting for exploring Rydberg physics, as exemplified by the blockade effect. Here we access the strongly interaction regime at high excitation densities (10^14-10^16/cm^3) and resolve the corresponding blockade dynamics for n = 2-7 using time-resolved spectroscopy. We find that Rydberg blockades are primarily governed by resonant dipolar interactions and that exciton recombination is coupled to the blockade itself. These findings demonstrate the potential for manipulating Rydberg exctions in the strongly interacting blockade regime in a solid state system.
Photons are ideal carriers of quantum information: they are fast, low-loss, and compatible with mature photonic infrastructure.Linear optical quantum computing exploits these properties but relies on probabilistic measurements and post-selection, incurring an exponential resource overhead that limits scalability [1].Circumventing this bottleneck requires deterministic quantum logic gates, which in turn demand strong, controllable interactions between individual photons.Photons do not interact in free space or in linear optical media.The standard route to attain effective photonphoton interactions is to hybridise photons with interacting matter excitations, forming polaritons.The matter component introduces an interaction-induced anharmonic level shift U into the ladder of polariton states: when one polariton occupies a mode, the next photon sees a shifted resonance (Fig. 1a).The key figure of merit is U/γ, where γ is the total polariton decoherence rate.For U/γ ≪ 1 the nonlinearity is classical; for U/γ ≳ 1 the system enters the quantum nonlinear regime, enabling photon blockade, large conditional phase shifts, and deterministic photonic gates.Atomic Rydberg systems have provided the clearest demonstration of this regime.Atoms excited to Rydberg states -electronic states with large principal quantum numbers n ≫ 1 -possess unique properties [2].Their lifetimes scale as 1/γ ∝ n 3 and transition dipole moments as µ ∝ n 2 , leading to strong dipole-dipole (U ∝ n 4 /r 3 ) or van der Waals (U ∝ n 11 /r 6 ) interactions over long distances r.These interactions can be imprinted onto photons via electromagnetically induced transparency (EIT) [3]: photons hybridise with collective atomic excitations to form slowly propagating Rydberg polaritons that strongly interact with each other over distances of up to tens of micrometres [4].This mechanism has produced photon blockade [5]
Microwave–optical conversion is key to future networks of quantum devices, such as those based on superconducting technology. Conversion at the single quantum level requires strong nonlinearity, high bandwidth, and compatibility with a millikelvin environment. A large nonlinearity is observed in Rydberg atoms, but combining atomic gases with dilution refrigerators is technically challenging. Here, we demonstrate a strong microwave–optical nonlinearity in a cryogenic, solid-state system by exploiting Rydberg states of excitons in Cu2O. We measure a microwave–optical cross-Kerr coefficient of B0 = 0.022 ± 0.008 m V−2 at 4 K, which is several orders of magnitude larger than other solid-state systems. The results are in quantitative agreement with a nonlinear susceptibility model based on the giant microwave dipole moment between nearby excitonic states. Our results highlight the potential of Rydberg excitons for nonlinear optics and form the basis for a microwave–optical frequency converter based on Cu2O.
The quantum confinement of Rydberg excitons (REs) in quantum structures opens the way towards considering nonlinear interactions in such systems. We present a theoretical calculation of optical functions in the case of a nonlinear coupling between REs in a quantum well with an electromagnetic wave. Using the real density matrix approach (RDMA), the analytical expressions for a linear and nonlinear absorption are derived and numerical calculations for Cu2O{\mathrm{Cu}}_{2}\mathrm{O}Cu2​O quantum wells are performed. The results indicate the conditions in which quantum well confinement states can be observed in linear and nonlinear optical spectra. The Kerr nonlinearity and self-phase modulation in such a system are studied. The effect of the Rydberg blockade and the associated optical bleaching are also discussed and confronted with available experimental data.
Mapping the strong interaction between Rydberg excitations in ultra-cold atomic ensembles onto single photons enables the realization of optical nonlinearities which can modify light on the level of individual photons.This novel approach forms the basis of a growing Rydberg quantum optics toolbox, which already contains photonic logic building-blocks such as single-photon sources, switches, transistors, and conditional π-phase shifts.This thesis reports on two experiments investigating strong photon-photon interactions mediated by Rydberg interactions.First, applying a ladder-type EIT scheme to Rydberg atoms in D-states with high principal quantum number results in the Rydberg interaction mediated nonlinearity accompanied by a time-dependent decay of transmission of probe light through the medium.In a joint experimental and theoretical analysis, this effect is attributed to the dephasing of propagating polaritons into stationary Rydberg excitations caused by the state mixing interaction occurring with Rydberg D-state atoms.Second, via a two-photon Raman excitation scheme Rydberg atoms are efficiently excited in a small atomic cloud.As the size of the Rydberg blockade exceeds the dimension of the medium, only a single Rydberg excitation can be present at a time.By fast engineered dephasing this Rydberg excitation is decoupled from the light field.Measurement of the transmitted light and the amount of excited Rydberg atoms gives evidence for the realization of a deterministic single-photon absorber.