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arXiv:2210.16416 · Scientific Reports

Highly-excited Rydberg excitons in synthetic thin-film cuprous oxide

Jacob DeLange, Kinjol Barua, Anindya Sundar Paul, Hamid Ohadi, Val Zwiller, Stephan Steinhauer, Hadiseh Alaeian

Published Oct 6, 2023• 19 citations

Abstract

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.

DOI: 10.1038/s41598-023-41465-y

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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.

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.

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.

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.

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 $3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}$.

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.

Due to their quantum nature, single-photon emitters generate individual photons in bursts or streams. They are paramount in emerging quantum technologies such as quantum key distribution, quantum repeaters, and measurement-based quantum computing. Many such systems have been reported in the last three decades, from Rubidium atoms coupled to cavities to semiconductor quantum dots and color centers implanted in waveguides. This review article highlights different material systems with deterministic and controlled single photon generation. We discuss and compare the performance metrics, such as purity and indistinguishability, for these sources and evaluate their potential for different applications. Finally, a new potential single-photon source, based on the Rydberg exciton in solid state metal oxide thin films, is introduced, briefly discussing its promising qualities and advantages in fabricating quantum chips for quantum photonic applications.