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arXiv:2007.07076 · Physical Review Letters

Controlling Exciton-Phonon Interactions via Electromagnetically Induced Transparency

Valentin Walther, P. Grünwald, Thomas Pohl

Published Oct 20, 2020• 23 citations
arXivHTMLPDF

Abstract

Highly excited Rydberg states of excitons in Cu_{2}O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate that two-photon excitation of Rydberg excitons under conditions of electromagnetically induced transparency (EIT) can be used to control this background. Based on a microscopic theory that describes the known single-photon absorption spectrum, we analyze the conditions under which two-photon EIT permits separating the optical Rydberg excitation from the phonon-induced absorption background, and even suppressing it entir7ely. Our findings thereby pave the way for the exploitation of Rydberg blockade with Cu_{2}O excitons in nonlinear optics and other applications.

DOI
10.1103/physrevlett.125.173601

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Highly excited Rydberg states of excitons in Cu_{2}O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate that two-photon excitation of Rydberg excitons under conditions of electromagnetically induced transparency (EIT) can be used to control this background. Based on a microscopic theory that describes the known single-photon absorption spectrum, we analyze the conditions under which two-photon EIT permits separating the optical Rydberg excitation from the phonon-induced absorption background, and even suppressing it entir7ely. Our findings thereby pave the way for the exploitation of Rydberg blockade with Cu_{2}O excitons in nonlinear optics and other applications.
Abstract Bound states of electron–hole pairs in semiconductors demonstrate a hydrogen-like behavior in their high-lying excited states that are also known as Rydberg exciton states. The strong interaction between excitons in levels with high principal quantum numbers prevents the creation of more than one exciton in a small crystal; resulting in the Rydberg blockade effect. Here, we propose a new kind of solid-state single-photon source based on the recently observed Rydberg blockade effect for excitons in cuprous oxide. Our quantitative estimates based on single and double excitation probability dynamics indicate that GHz rates and values of the second-order correlation function g 2 ( 0 ) below the percent level can be simultaneously achievable. These results should pave the way to explore applications of Rydberg excitons in photonic quantum information processing.
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.
Electromagnetically induced transparency (EIT) in quantum dot exciton systems in which the exciton behaves as a two-level system is investigated theoretically. It is shown that due to strong exciton–phonon coupling EIT can occur in such a quantum dot system and ultraslow light can propagate. The nonlinear optical absorption and Kerr coefficient based on EIT are also calculated. The numerical results show that giant nonlinear optical effects can be obtained while the frequency of the signal field differs only by an amount of LO phonon frequency from the exciton frequency in quantum dot systems.
We analyze several implementations of all-optical single-photon transistors (SPTs) operating in the continuous-wave (cw) regime, as presented in the companion paper []. The devices rely on ensembles of Rydberg atoms interacting via van der Waals interactions. Under electromagnetically induced transparency (EIT), a weak probe field is fully transmitted through the atomic ensemble in the absence of control photons. Exciting a collective Rydberg state with a single control photon breaks the EIT condition, thereby strongly suppressing the probe transmission. We show how collective Rydberg interactions in an atomic ensemble, confined either in an optical cavity or in free space, give rise to two distinct probe-induced dephasing mechanisms. These processes localize the control excitations, extend their lifetimes, and increase the device efficiency. We characterize the SPTs in terms of control-photon absorption probability and probe gain, supported by numerical simulations of realistic one- and three-dimensional ensembles. The proposed cw devices complement previously demonstrated SPTs and broaden the toolbox of quantum light manipulation circuitry.
We investigate facilitation-induced transparency (FIT) enabled by strong and long-range Rydberg atom interactions between two spatially separated optical channels. In this setting, the resonant two-photon excitation of Rydberg states in a target channel is conditioned by a single Rydberg excitation in a control channel. Through the contactless coupling enabled by the Rydberg interaction, the optical transparency of the target channel can be actively manipulated by steering the optical detuning in the control channel. By adopting a dressed-state picture, we identify two different interference pathways, in which one corresponds to Rydberg blockade and an emergent one results from facilitation. We show that the FIT is originated from the Rydberg interaction and the quantum interference effect between the two pathways, which is different from conventional electromagnetically induced transparency realized by single-body laser-atom coupling. We find that the FIT in such a dual-channel setting is rather robust, insensitive to changes of systemic parameters, and can be generalized to multichannel settings. Moreover, we demonstrate that such a FIT permits the realization of controllable single-photon switches, which also paves a route to detect Rydberg facilitation by using optical absorption spectra. Our study contributes to current efforts in probing correlated many-body dynamics and developing single-photon quantum devices based on Rydberg atom ensembles.
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.