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Physical review. B./Physical review. B

Quantum interference of Rydberg excitons in Cu 2 O : Quantum beats

Sylwia Zielińska‐Raczyńska, David Ziemkiewicz

Published May 1, 2025• 3 citations
Publisher

Abstract

A density matrix formalism is employed to calculate the emission of multilevel Rydberg excitonic system, highlighting picosecond-scale dynamics and coherent effects such as quantum beats. The theoretical results for one- and two-photon excitations of various Rydberg excitons and configurations providing the insight into their dynamics are compared with recent experimental data. In particular, the effect of Rydberg blockade on the quantum beat phenomenon is discussed.

DOI
10.1103/physrevb.111.205201

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Rydberg states of excitons are promising quantum objects to engineer giant nonlinearities in a solid-state system. For this purpose, a deeper understanding of the dynamics of Rydberg excitons and of their potential for coherent manipulation becomes important. We report experimental results where two-photon absorption is resonant with various Rydberg states of excitons in copper oxide and we detect their emission dynamics on a streak camera with subpicosecond resolution. This technique enables the direct measurement of the Rydberg states lifetimes, which are in good agreement with the expected Rydberg scaling law. Moreover, we observe several intriguing dynamics including the presence of long-lived coherent oscillations. Finally, we independently measure the coherence time of the Rydberg states using a modified Michelson interferometer and find a good agreement with the coherent oscillations detected in the exciton emission dynamics. The lifetimes also reveal the absence of inhomogeneous broadening in the current high-precision spectroscopic data for the S series, which together with the presence of significant coherence time confirms the suitability of the system for coherent engineering.
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.