Rydberg Excitons In Cuprous Oxide Research Articles

Giant microwave–optical Kerr nonlinearity via Rydberg excitons in cuprous oxide

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.

Microwave-optical coupling via Rydberg excitons in cuprous oxide

We report exciton-mediated coupling between microwave and optical fields in cuprous oxide (Cu$_2$O) at low temperatures. Rydberg excitonic states with principal quantum number up to $n=12$ were observed at 4~K using both one-photon (absorption) and two-photon (second harmonic generation) spectroscopy. Near resonance with an excitonic state, the addition of a microwave field significantly changed the absorption lineshape, and added sidebands at the microwave frequency to the coherent second harmonic. Both effects showed a complex dependence on $n$ and angular momentum, $l$. All of these features are in semi-quantitative agreement with a model based on intraband electric dipole transitions between Rydberg exciton states. With a simple microwave antenna we already reach a regime where the microwave coupling (Rabi frequency) is comparable to the nonradiatively broadened linewidth of the Rydberg excitons. The results provide a new way to manipulate excitonic states, and open up the possibility of a cryogenic microwave to optical transducer based on Rydberg excitons.

Coherent transfer matrix analysis of the transmission spectra of Rydberg excitons in cuprous oxide

In this study we analyze the transmission spectrum of a thin plate of Cuprous Oxide in the range of the absorption of the yellow exciton states with the coherent transfer matrix method. We demonstrate that, in contrast to the usual analysis using Beer's law, which turns out to be a rather good approximation only in the spectral region of high principal quantum numbers, a consistent quantitative description over the whole spectral range under consideration is possible. This leads to new and more accurate parameters not only for the Rydberg exciton states, but also for the strengths of indirect transitions. Furthermore, the results have consequences on the determination of the density of electron-hole pairs after optical excitation.

Quantum many-body effects on Rydberg excitons in cuprous oxide

We investigate quantum many-body effects on Rydberg excitons in cuprous oxide induced by the surrounding electron-hole plasma. Line shifts and widths are calculated by full diagonalisation of the plasma Hamiltonian and compared to results in first order perturbation theory, and the oscillator strength of the exciton lines is analysed.

Polarized edge state emission from topological spin phases of trapped Rydberg excitons in Cu2O

In one dimensional chains of trapped Rydberg excitons in cuprous oxide semiconductor the topological spin phase has been recently predicted [Phys. Rev. Lett. 123, 126801 (2019); arXiv:1903.11951]. This phase is characterized by the diluted antiferromagnetic order of $p$-shell exciton angular momenta-$1$ and the edge states behaving akin spin-$1/2$ fermions. Here we study the properties of the ground state in the finite chains and its fine structure resulting from the effective interaction of the edge spins. We demonstrate that these edge states can detected optically via the enhancement of the circular polarization of the edge emission as compared with the emission from the bulk. We calculate the distribution of the exciton angular momentum vs. trap number in the chain numerically and analytically based on the variational ansatz.

Classical and semiclassical description of Rydberg excitons in cuprous oxide

Experimental and theoretical investigations of excitons in cuprous oxide have revealed a significant fine-structure splitting of the excitonic Rydberg states caused by a strong impact of the valence band structure. We provide a semiclassical interpretation of that splitting by investigating the classical dynamics of the excitonic electron-hole pair beyond the hydrogen-like model. Considering the slow motion of Rydberg excitons in coordinate space compared to the fast dynamics of quasispin and hole spin we use an adiabatic approach and energy surfaces in momentum space for the computation of the exciton dynamics. We observe quasi-periodic motion on near-integrable tori. Semiclassical torus quantization yields the energy regions of the fine-structure splitting of $n$-manifolds in agreement with quantum mechanical computations.

Interaction of charged impurities and Rydberg excitons in cuprous oxide

We investigate the influence of a static, uncorrelated distribution of charged impurities on the spectrum of bound excitons in the copper oxide Cu$_{\text{2}}$O. We show that the statistical distribution of Stark shifts and ionisation rates leads to the vanishing of Rydberg resonances into an apparent continuum. The appearance of additional absorption lines due to the broken rotational symmetry, together with spatially inhomogeneous Stark shifts, leads to a modification of the observed line shapes that agree qualitatively with the changes observed in the experiment.

Influence of electron-hole plasma on Rydberg excitons in cuprous oxide

We develop a many-body approach to the behavior of exciton bound states and the conduction electron band edge in a surrounding electron-hole plasma with a focus on the absorption spectrum of Rydberg excitons in cuprous oxide. The interplay of band edge and exciton levels is analyzed numerically, whereby the self-consistent solution is compared to the semiclassical Debye approximation. Our results provide criteria which allow to verify or rule out the different band edge models against future experimental data.

Fine Structure of Rydberg Excitons in Cuprous Oxide

In 1952, E.F. Gross and N.A. Karryev discovered excitons of big radius also called the Wannier–Mott excitons. Their energy spectrum, response to external electric and magnetic fields, and also elastic deformations of a crystal were extensively studied in the 1960s–1970s. The second wave of interest to excitons in Cu2O crystals appeared comparatively recent, in 2014, after the “giant” highly excited exciton states had been observed in this material. A theoretical description of highly excited exciton states needs, as a rule, new approaches, because, for such states, a deviation from the exactly solved hydrogen-like model becomes substantial and a numerical solution of the Schrodinger equation with allowance made for the features of the crystal energy band structure becomes extremely resource consuming. This report is a brief review of recent theoretical and experimental studies of the fine structure of the exciton energy spectrum in copper protoxide.

Interaction of Rydberg excitons in cuprous oxide with phonons and photons: optical linewidth and polariton effect

We demonstrate that the optical linewidth of Rydberg excitons in Cu2O can be completely explained by scattering with acoustical and optical phonons, whereby the dominant contributions stems from the non-polar optical and modes. The consequences for the observation of polariton effects are discussed. We find that an anti-crossing of photon and exciton dispersions exists only for states with main quantum numbers n > 28, so polariton effects do not play any role in the experiments reported up to now.

Exciton-polaritons in cuprous oxide: Theory and comparison with experiment

The observation of giant Rydberg excitons in cuprous oxide $\left(\mathrm{Cu_{2}O}\right)$ up to a principal quantum number of $n=25$ by T.~Kazimierczuk \emph{et al.} [Nature \textbf{514}, 343, (2014)] inevitably raises the question whether these quasi-particles must be described within a multi-polariton framework since excitons and photons are always coupled in the solid. In this paper we present the theory of exciton-polaritons in $\mathrm{Cu_{2}O}$. To this end we extend the Hamiltonian which includes the complete valence band structure, the exchange interaction, and the central-cell corrections effects, and which has been recently deduced by F.~Schweiner \emph{et al.} [Phys.~Rev.~B \textbf{95}, 195201, (2017)], for finite values of the exciton momentum $\hbar K$. We derive formulas to calculate not only dipole but also quadrupole oscillator strengths when using the complete basis of F.~Schweiner \emph{et al.}. Very complex polariton spectra for the three orientations of $\boldsymbol{K}$ along the axes $[001]$, $[110]$, and $[111]$ of high symmetry are obtained and a strong mixing of exciton states is reported. The main focus is on the $1S$ ortho exciton-polariton, for which pronounced polariton effects have been measured in experiments. We set up a $5\times 5$ matrix model, which accounts for both the polariton effect and the $K$-dependent splitting, and which allows treating the anisotropic polariton dispersion for any direction of $\boldsymbol{K}$. We especially discuss the dispersions for $\boldsymbol{K}$ being oriented in the planes perpendicular to $[1\bar{1}0]$ and $[111]$, for which experimental transmission spectra have been measured. Furthermore, we compare our results with experimental values of the $K$-dependent splitting, the group velocity, and the oscillator strengths of this exciton-polariton.

Quantum chaos and breaking of all anti-unitary symmetries in Rydberg excitons.

Symmetries are the underlying principles of fundamental interactions in nature. Chaos in a quantum system may emerge from breaking these symmetries. Compared to vacuum, crystals are attractive for studying quantum chaos, as they not only break spatial isotropy, but also lead to novel quasiparticles with modified interactions. Here we study yellow Rydberg excitons in cuprous oxide which couple strongly to the vacuum light field and interact significantly with crystal phonons, leading to inversion symmetry breaking. In a magnetic field, time-reversal symmetry is also broken and the exciton states show a complex splitting pattern, resulting in quadratic level repulsion for small splittings. In contrast to atomic chaotic systems in a magnetic field, which show only a linear level repulsion, this is a signature of a system where all anti-unitary symmetries are broken simultaneously. This behaviour can otherwise be found only for the electro-weak interaction or engineered billiards.

Giant Rydberg excitons in the copper oxide Cu2O.

A highly excited atom having an electron that has moved into a level with large principal quantum number is a hydrogen-like object, termed a Rydberg atom. The giant size of Rydberg atoms leads to huge interaction effects. Monitoring these interactions has provided insights into atomic and molecular physics on the single-quantum level. Excitons--the fundamental optical excitations in semiconductors, consisting of an electron and a positively charged hole--are the condensed-matter analogues of hydrogen. Highly excited excitons with extensions similar to those of Rydberg atoms are of interest because they can be placed and moved in a crystal with high precision using microscopic energy potential landscapes. The interaction of such Rydberg excitons may allow the formation of ordered exciton phases or the sensing of elementary excitations in their surroundings on a quantum level. Here we demonstrate the existence of Rydberg excitons in the copper oxide Cu2O, with principal quantum numbers as large as n = 25. These states have giant wavefunction extensions (that is, the average distance between the electron and the hole) of more than two micrometres, compared to about a nanometre for the ground state. The strong dipole-dipole interaction between such excitons is indicated by a blockade effect in which the presence of one exciton prevents the excitation of another in its vicinity.