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arXiv:2105.07942 · Physical review. B./Physical review. B

Giant Rydberg excitons in Cu2O probed by photoluminescence excitation spectroscopy

Marijn A. M. Versteegh, Stephan Steinhauer, Josip Bajo, Thomas Lettner, Ariadna Soro, Alena Romanova, Samuel Gyger, Lucas Schweickert, A. Mysyrowicz, Val Zwiller

Published Dec 20, 2021• 44 citations
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Abstract

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 $T=38$ mK with principal quantum numbers up to $n=30$, corresponding to a calculated diameter of $3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}$.

DOI
10.1103/physrevb.104.245206

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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\ensuremathμm3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}3\ensuremathμm.
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.
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.
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.
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.
Over the past decade, Rydberg excitons in bulk Cu 2 O have emerged as a solid-state analog to atomic Rydberg systems, exhibiting exaggerated quantum optical properties including large dipole moments, strong dipole–dipole interactions, and enhanced nonlinear susceptibilities. High-resolution absorption spectroscopy has revealed elegant scaling laws with principal quantum number across temperatures from tens of mK to above 100 K. While many features follow a hydrogen-like model, non-hydrogenic effects arise from complex bandstructures and many-body interactions. This review summarizes experimental advances in accessing high- n Rydberg states and quantum phenomena arising from diverse exciton interaction mechanisms. It also discusses prospective quantum and nonlinear optical applications.