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arXiv:1904.02959 · Physical review. B./Physical review. B

Nonlinear optical properties and self-Kerr effect of Rydberg excitons

Sylwia Zielińska‐Raczyńska, G. Czajkowski, Karol Karpiński, David Ziemkiewicz

Published Jun 25, 2019• 21 citations
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Abstract

We show how to compute the nonlinear optical functions (absorption, reflection, and transmission) for a medium with Rydberg excitons (REs), including the effect of the coherence between the electron-hole pair and the electromagnetic field. Using the real density-matrix approach the analytical expressions for nonlinear optical functions are obtained and numerical calculations are performed for ${\mathrm{Cu}}_{2}\mathrm{O}$ crystal where REs have been observed. We report a good agreement with recently published experimental data. Propagation of the electromagnetic waves in Rydberg exciton media with nonlinear effect is also discussed and the possibility of obtaining self-phase modulation due to Kerr nonlinearity is investigated.

DOI
10.1103/physrevb.99.245206

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We show how to compute the nonlinear optical functions (absorption, reflection, and transmission) for a medium with Rydberg excitons (REs), including the effect of the coherence between the electron-hole pair and the electromagnetic field. Using the real density-matrix approach the analytical expressions for nonlinear optical functions are obtained and numerical calculations are performed for Cu2O{\mathrm{Cu}}_{2}\mathrm{O}Cu2​O crystal where REs have been observed. We report a good agreement with recently published experimental data. Propagation of the electromagnetic waves in Rydberg exciton media with nonlinear effect is also discussed and the possibility of obtaining self-phase modulation due to Kerr nonlinearity is investigated.
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We show how to compute the optical functions when Rydberg Excitons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. We use the Real Density Matrix Approach (RDMA), which, combined with Green's function method, enables one to derive analytical expressions for the optical functions. Choosing the susceptibility, we performed numerical calculations appropriate to a Cu$_2$0 crystal. The effect of the coherence is displayed in the line shape. We also examine in details and explain the dependence of the oscillator strength and the resonance placement on the state number. We report a good agreement with recently published experimental data.
By mapping photons into the sample of cuprous oxide with Rydberg excitons, it is possible to obtain a significant optical phase shift due to third-order cross-Kerr nonlinearities realized under the conditions of electromagnetically induced transparency. The optimum conditions for observation of the phase shift over π in Rydberg excitons media are examined. A discussion of the application of the cross-phase modulations in the field of all-optical quantum information processing in solid-state systems is presented.
Dynamics of Cu2_22​O Rydberg excitons -- real density matrix approach
Basing on recent reliable measurements of the life- and coherence time of Cu2_22​O Rydberg excitons, we present an analytical method which enables to describe the experimental results. The real-density matrix approach (RDMA) is applied to describe two-photon absorption in Cu2_22​O through the excitonic response to the exciting fields. This approach produces an analytical expression for the emission intensity time evolution, and can be used to explain trends in reported experimental data. Our approach takes into account the effect of the coherence between the electron-hole pair and the electromagnetic fields, the quantum beats and the life- and coherence time dependence on the applied laser power. Adding a separation of slow- and rapid dynamics components we find excellent agreement with the experimental data.
We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a nonlinear manner. We explore this mechanism theoretically and determine its effects on the optical properties of a semiconductor for the case of degenerate pair-state asymptotes of Rydberg excitons in Cu_{2}O. Upon analyzing the additional effects of a dilute residual electron-hole plasma, we find quantitative agreement with previous transmission measurements, which provides strong indications for the enhancement of Rydberg-induced nonlinearities by surrounding free charges.
Light propagation through an ensemble of ultracold Rydberg atoms in an electromagnetically-induced-transparency (EIT) configuration is studied. In strongly interacting Rydberg EIT media, nonlinear optical effects lead to a nontrivial dependence of the degree of probe-beam attenuation on the medium density and on its initial intensity. We develop a Monte Carlo rate equation model that self-consistently includes the effect of the probe-beam attenuation to investigate the steady state of the Rydberg medium driven by two laser fields. We compare our results to recent experimental data and to results of other state-of-the-art models for light propagation in Rydberg EIT media. We find that for low probe field intensities, our results match the experimental data best if a density-dependent dephasing rate is included in the model. At higher probe intensities, our model deviates from other theoretical approaches, because it predicts a spectral asymmetry together with line broadening. These are likely due to off-resonant excitation channels, which, however, have not been observed in recent experiments. Atomic motion and coupling to additional Rydberg levels are discussed as possible origins for these deviations.