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arXiv:2508.05806

Rydberg Exciton Dynamics in the Blockade Regime of Cu2O

Gillian E. Minarik, Eric A. Arsenault, Vinicius da Silveira Lanza Avelar, Taketo Handa, Xiaoyang Zhu

Published Aug 7, 2025• 0 citations
arXivHTMLPDF

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.

DOI
10.48550/arxiv.2508.05806

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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.
The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and molecular physics to quantum optics and technology. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up to a micrometer have indeed been observed in cuprous oxide semiconductors. Here, we demonstrate the generation and control of strong exciton interactions in this material by optically producing two distinct quantum states of Rydberg excitons. This is made possible by two-color pump-probe experiments that allow for a detailed probing of the interactions. Our experiments reveal the emergence of strong spatial correlations and an inter-state Rydberg blockade that extends over remarkably large distances of several micrometers. The generated many-body states of semiconductor excitons exhibit universal properties that only depend on the shape of the interaction potential and yield clear evidence for its vastly extended-range and power-law character.
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.
Rydberg excitons are, with their ultrastrong mutual interactions, giant optical nonlinearities, and very high sensitivity to external fields, promising for applications in quantum sensing and nonlinear optics at the single-photon level. To design quantum applications it is necessary to know how Rydberg excitons and other excited states relax to lower-lying exciton states. Here, we present photoluminescence excitation spectroscopy as a method to probe transition probabilities from various excitonic states in cuprous oxide. We show giant Rydberg excitons at T=38T=38T=38 mK with principal quantum numbers up to n=30n=30n=30, corresponding to a calculated diameter of $3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}$.
Abstract The recent observation of high-lying Rydberg states of excitons in semiconductors with relatively high binding energy motivates exploring their applications in quantum nonlinear optics and quantum information processing. Here, we study Rydberg excitation dynamics of a mesoscopic array of excitons to demonstrate its application in simulation of quantum many-body dynamics. We show that the Z 2 -ordered phase can be reached using physical parameters available for cuprous oxide (Cu 2 O) by optimizing driving laser parameters such as duration, intensity, and frequency. In an example, we study the application of our proposed system to solving the maximum independent set problem based on the Rydberg blockade effect.
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.
Cuprous oxide ([Formula: see text]) has recently emerged as a promising material in solid-state quantum technology, specifically for its excitonic Rydberg states characterized by large principal quantum numbers (n). The significant wavefunction size of these highly-excited states (proportional to [Formula: see text]) enables strong long-range dipole-dipole (proportional to [Formula: see text]) and van der Waals interactions (proportional to [Formula: see text]). Currently, the highest-lying Rydberg states are found in naturally occurring [Formula: see text]. However, for technological applications, the ability to grow high-quality synthetic samples is essential. The fabrication of thin-film [Formula: see text] samples is of particular interest as they hold potential for observing extreme single-photon nonlinearities through the Rydberg blockade. Nevertheless, due to the susceptibility of high-lying states to charged impurities, growing synthetic samples of sufficient quality poses a substantial challenge. This study successfully demonstrates the CMOS-compatible synthesis of a [Formula: see text] thin film on a transparent substrate that showcases Rydberg excitons up to [Formula: see text] which is readily suitable for photonic device fabrications. These findings mark a significant advancement towards the realization of scalable and on-chip integrable Rydberg quantum technologies.