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MRS Bulletin

Rydberg excitons and quantum sensing

Julian Heckötter, Marc Aßmann, M. Bayer

Published Aug 28, 2024• 9 citations
Publisher

Abstract

Abstract Within the last few years, Rydberg excitons, bound electron–hole pairs in highly excited states, have emerged as a promising technology platform for quantum nonlinear optics, quantum information processing, and quantum sensing. The advanced device designs and sensing concepts in these fields require strong nonlinearities at the few-photon or few-carrier level. Rydberg states offer the required strong nonlinearities as the relevant physical quantities at the heart of such nonlinear effects scale strongly with the principal quantum number, n, of the excited state: For example, their polarizability scales as $$n^7$$ n 7 , resulting in an enormous sensitivity to external fields. We review recent experimental and theoretical results that pave the way toward quantum sensing of the electric fields originating from static charge carriers and strongly diluted electron–hole plasmas. We also discuss the strong nonlinear optical properties of Rydberg excitons and how they could be utilized in terms of sensing. Graphical abstract

DOI
10.1557/s43577-024-00775-w

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Introduction

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This introductory chapter presents the scope of this book: namely that the book is devoted to Rydberg (i.e., highly-excited) atoms and molecules They have striking distinctions to atoms and molecules in the ground or low-excited states. For Rydberg atoms, with the increase of the principal quantum number n, their characteristic size and the electric dipole moment scales as n 2 (which is why they are extremely sensitive to even weak electric fields and electromagnetic radiation) and their radiative lifetime scales as n 3. They strongly interact not only with an electric field, but also with each other: their dipole–dipole interaction scales as n 4/R 3 and their van der Waals interaction scales as n 11/R 6, where R is their separation from each other. In laboratory conditions experimentalists deal with Rydberg atoms having the quantum number of several tens. In the Universe, in H II regions, the principal quantum number of Rydberg atoms can reach n ~ 1000. In the latter case, the Rydberg atoms cannot be considered anymore as microscopic objects: the diameter of their electron orbit is ~ 0.1 mm, i.e., twice the diameter of human hair. Studies of Rydberg atoms and molecules have numerous applications. Examples are highly-responsive sensing, quantum optics (where the light is manipulated at the level of a single photon), quantum computing, quantum chaos, ultracold Rydberg gases and plasmas, anti-hydrogen formation, and plasma diagnostics.

Institute of Physics eBooks•Nov 1, 2021•0 citations
Abstract Within the last few years, Rydberg excitons, bound electron–hole pairs in highly excited states, have emerged as a promising technology platform for quantum nonlinear optics, quantum information processing, and quantum sensing. The advanced device designs and sensing concepts in these fields require strong nonlinearities at the few-photon or few-carrier level. Rydberg states offer the required strong nonlinearities as the relevant physical quantities at the heart of such nonlinear effects scale strongly with the principal quantum number, n, of the excited state: For example, their polarizability scales as n7n^7n7 n 7 , resulting in an enormous sensitivity to external fields. We review recent experimental and theoretical results that pave the way toward quantum sensing of the electric fields originating from static charge carriers and strongly diluted electron–hole plasmas. We also discuss the strong nonlinear optical properties of Rydberg excitons and how they could be utilized in terms of sensing. Graphical abstract
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.
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.
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 $3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}$.
Rydberg atoms are neutral atoms excited to high principal quantum number states, which endows them with exaggerated properties such as large electric dipole moments, long lifetimes, and extreme sensitivity to external electromagnetic fields. These characteristics form the foundation of Rydberg atom-based sensors, an emerging class of quantum devices capable of optically detecting electric fields across frequencies from DC to the terahertz regime. Rydberg-based electrometry operates through both Autler–Townes (AT) splitting of resonant Rydberg transitions and Stark-shift measurements for high-frequency or far-detuned fields, enabling broadband field sensing from DC to the THz regime. Using ladder-type electromagnetically induced transparency (EIT) and AT splitting, these sensors enable non-invasive, SI-traceable measurements of field amplitude, frequency, phase, and polarization. Recent developments have demonstrated broadband electric field probes, voltage calibration standards, and compact RF receivers based on thermal vapor cells and integrated photonic architectures. Furthermore, innovations in multi-photon EIT, superheterodyne readout, and multi wave mixing have expanded the dynamic range and bandwidth of Rydberg-based electrometry. Despite challenges related to environmental perturbations, linewidth broadening, and laser stabilization, ongoing advances in atomic control, hybrid photonic integration, and EIT-based readout promise scalable, chip-compatible sensors. This review summarizes the physical principles, experimental progress, and emerging applications of Rydberg atom-based sensing, emphasizing their potential for next generation quantum metrology, wireless communication, and precision field mapping.
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.
This introductory chapter presents the scope of this book: namely that the book is devoted to Rydberg (i.e., highly-excited) atoms and molecules They have striking distinctions to atoms and molecules in the ground or low-excited states. For Rydberg atoms, with the increase of the principal quantum number n, their characteristic size and the electric dipole moment scales as n 2 (which is why they are extremely sensitive to even weak electric fields and electromagnetic radiation) and their radiative lifetime scales as n 3. They strongly interact not only with an electric field, but also with each other: their dipole–dipole interaction scales as n 4/R 3 and their van der Waals interaction scales as n 11/R 6, where R is their separation from each other. In laboratory conditions experimentalists deal with Rydberg atoms having the quantum number of several tens. In the Universe, in H II regions, the principal quantum number of Rydberg atoms can reach n ~ 1000. In the latter case, the Rydberg atoms cannot be considered anymore as microscopic objects: the diameter of their electron orbit is ~ 0.1 mm, i.e., twice the diameter of human hair. Studies of Rydberg atoms and molecules have numerous applications. Examples are highly-responsive sensing, quantum optics (where the light is manipulated at the level of a single photon), quantum computing, quantum chaos, ultracold Rydberg gases and plasmas, anti-hydrogen formation, and plasma diagnostics.