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arXiv:2604.27331

Low-Energy Purification of Crystal Defects by Rydberg Excitons

Shiva Kant Tiwari, Tijs Karman, Valentin Walther

Published Apr 30, 2026• 0 citations
arXivHTMLPDF

Abstract

Recent experiments show that optically generated Rydberg excitons in cuprous oxide can neutralize charged impurities, strongly reducing stray electric fields and effectively purifying the crystal. Here, we develop a multichannel theory of Rydberg exciton-impurity scattering that resolves the competing roles of capture, elastic scattering, and inelastic transitions between excitonic states. We find that at high collision energies, as effective under conventional single-photon excitation, purification is reduced relative to Langevin capture. These collisions are accompanied by inelastic redistribution and dominant elastic scattering, including pronounced glory scattering, which suppress purification efficiency. We identify a quantum regime at ultralow collision energies favorable for purification, where only the s-wave contributes: capture is enhanced while elastic and inelastic channels are strongly suppressed. This regime can be accessed via degenerate two-photon excitation of even-parity Rydberg excitons with tunable recoil, additionally enabling the systematic exploration of exciton-impurity scattering over a wide range of collision energies beyond what is readily achievable in atomic counterparts in atomic gas experiments.

DOI
10.48550/arxiv.2604.27331

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Recent experiments show that optically generated Rydberg excitons in cuprous oxide can neutralize charged impurities, strongly reducing stray electric fields and effectively purifying the crystal. Here, we develop a multichannel theory of Rydberg exciton-impurity scattering that resolves the competing roles of capture, elastic scattering, and inelastic transitions between excitonic states. We find that at high collision energies, as effective under conventional single-photon excitation, purification is reduced relative to Langevin capture. These collisions are accompanied by inelastic redistribution and dominant elastic scattering, including pronounced glory scattering, which suppress purification efficiency. We identify a quantum regime at ultralow collision energies favorable for purification, where only the s-wave contributes: capture is enhanced while elastic and inelastic channels are strongly suppressed. This regime can be accessed via degenerate two-photon excitation of even-parity Rydberg excitons with tunable recoil, additionally enabling the systematic exploration of exciton-impurity scattering over a wide range of collision energies beyond what is readily achievable in atomic counterparts in atomic gas experiments.
Improving the quantum coherence of solid-state systems is a decisive factor in realizing solid-state quantum technologies. The key to optimize quantum coherence lies in reducing the detrimental influence of noise sources such as spin noise and charge noise. Here we demonstrate that we can utilize highly-excited Rydberg excitons to neutralize charged impurities in the semiconductor Cuprous Oxide - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We observe that the absorption of the purified crystal increases by up to 25% and that the purification effect is long-lived and may persist for hundreds of microseconds or even longer. We investigate the interaction between Rydberg excitons and impurities and find that it is long-ranged and based on charge-induced dipole interactions. Using a time-resolved pump-probe technique, we can discriminate purification from Rydberg blockade, which has been a long-standing goal in excitonic Rydberg systems.
We investigate the interaction between highly excited Rydberg excitons and charged impurities in the semiconductor Cuprous Oxide. We find that it is long-ranged and based on charge-induced dipole interactions. We demonstrate that we can utilize this interaction to neutralize impurities throughout the whole crystal - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We find that the absorption of the purified crystal increases by up to 25 % and that the purification effect is long-lived and may persist for hundreds of microseconds or even longer. Using a time-resolved pump-probe technique, we can discriminate purification from Rydberg blockade, which has been a long-standing goal in excitonic Rydberg systems.
We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a nonlinear manner. We explore this mechanism theoretically and determine its effects on the optical properties of a semiconductor for the case of degenerate pair-state asymptotes of Rydberg excitons in Cu_{2}O. Upon analyzing the additional effects of a dilute residual electron-hole plasma, we find quantitative agreement with previous transmission measurements, which provides strong indications for the enhancement of Rydberg-induced nonlinearities by surrounding free charges.
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.
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.
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.