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arXiv:2605.05171

Plasma effects on lifetimes and screening of Rydberg excitons

AbdAlGhaffar Amer, V. Walther, Francis Robicheaux

quant-phSubmitted May 6, 2026• Announced May 7, 2026
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Abstract

We simulate the effects of a neutral electron--hole plasma on Rydberg excitons in cuprous oxide (Cu$_2$O), focusing on the validity of Debye screening and the role of plasma-induced thermalization. Unlike atomic Rydberg states, excitons in Cu$_2$O consist of quasiparticles with comparable effective masses whose orbital frequencies can exceed the plasma frequency, invalidating the assumption of a stationary screened charge. Using two complementary approaches, a classical orbit model and a harmonic-oscillator representation evolved via the truncated Wigner approximation, we study exciton lifetimes and interaction screening under realistic plasma conditions. We find numerically that plasma-induced scattering induces finite exciton lifetimes with specific scaling relations with plasma density, principal quantum number $n$ and temperature, possibly providing an explanation for experimentally observed deviations from the $n^3$ scaling at high principal quantum numbers. By explicitly computing time-averaged electric fields, we show that Debye screening overestimates the screening of the exciton's internal field, especially for high angular momentum states. Furthermore, we demonstrate that exciton-exciton interactions are not Debye screened at separations comparable to the Debye length for Rydberg excitons that are well resolvable in absorption measurements.

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•Jan 1, 2013•0 citations
We simulate the effects of a neutral electron--hole plasma on Rydberg excitons in cuprous oxide (Cu2_22​O), focusing on the validity of Debye screening and the role of plasma-induced thermalization. Unlike atomic Rydberg states, excitons in Cu2_22​O consist of quasiparticles with comparable effective masses whose orbital frequencies can exceed the plasma frequency, invalidating the assumption of a stationary screened charge. Using two complementary approaches, a classical orbit model and a harmonic-oscillator representation evolved via the truncated Wigner approximation, we study exciton lifetimes and interaction screening under realistic plasma conditions. We find numerically that plasma-induced scattering induces finite exciton lifetimes with specific scaling relations with plasma density, principal quantum number nnn and temperature, possibly providing an explanation for experimentally observed deviations from the n3n^3n3 scaling at high principal quantum numbers. By explicitly computing time-averaged electric fields, we show that Debye screening overestimates the screening of the exciton's internal field, especially for high angular momentum states. Furthermore, we demonstrate that exciton-exciton interactions are not Debye screened at separations comparable to the Debye length for Rydberg excitons that are well resolvable in absorption measurements.
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.
We report experimental and theoretical investigations of interacting excitons of the yellow series in cuprous oxide (Cu2_22​O) with principal quantum numbers up to by means of second harmonic generation (SHG). Using picosecond pulsed laser excitation up to 10 GW/cm2^22 peak intensity we observe a pronounced change of the spectra with increasing pump laser intensity: an energetic shift to lower absolute energies and a spectral broadening. The absolute intensities of the spectral lines scale for low powers with the square of the pump power, but saturates at higher powers. At still higher powers the SHG intensity is actually reduced. To explain these results quantitively, we developed a semi-classical theory of resonant SHG where the process of SHG is fully coherent. The excitons are assumed to be bosons interacting by a distance dependent potential giving rise to both the changes in spectral line shape and the saturation by a Rydberg\it{Rydberg}Rydberg blockade. The concomitant measurement of two-photon absorption allows to derive quantitative values for the exciton-exciton interaction. While the results agree in order of magnitude with those calculated by state-of-the art atomic-like van der Waals interaction theory, the scaling with principle quantum number is quite different. As a possible screening by an electron-hole plasma created by three-photon absorption into blue and violet band states could be ruled out, our results point toward fundamental differences between excitons and atoms.
The recent observation of excitons in highly excited states has allowed the study of Rydberg physics in cuprous oxide crystals. This opens the unique possibility to elaborate on similarities and differences between Rydberg atoms and Rydberg excitons, as done here experimentally and theoretically for quantities related to the splitting of multiplets with particular principal quantum number nnn in zero and finite electric or magnetic fields. The authors find characteristic scaling laws with nnn with some discrepancies between excitons and atoms, but surprisingly, they find mostly similarities, even though the underlying physics, such as the complex valence band structure, are quite different.
We investigate the interaction between highly excited Rydberg excitons and charged impurities in the semiconductor Cuprous Oxide. We find that it is long-ranged and based on charge-induced dipole interactions. We demonstrate that we can utilize this interaction to neutralize impurities throughout the whole crystal - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We find 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. 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.
Ultracold neutral plasmas (UNPs) are highly correlated, charged-particle systems studied in standard atomic-molecular optical physics laboratories. Advances in ultracold physics techniques have led to the development of magneto-optical traps that permit the localization of micro-Kelvin temperature atomic samples (10⁸ - 10¹⁰ cm -³ that can be photoionized with a defined excess laser energy. Magneto-optical trapping of molecules proves difficult, and to date, lags in reaching conditions attainable for atoms. Molecules possess additional degrees of freedom where energy can flow during laser trapping and cooling. Alternatively, elastic collisions with inert gases offer another route to low temperatures. Super-sonic expansions of target molecules seeded in a noble gas can reduced the translational temperature to values as low as 0.1 K. Here I report on the formation of a molecular ultracold plasma in a molecular beam of nitric oxide seeded in an inert gas. Our method does not directly form a plasma, but instead, I create a Rydberg gas that spontaneously evolves to a plasma. I have verified the transition to a collective plasma state by applying pulsed-fields to the field-free flight region, and observe a signal that persists well beyond classical field amplitudes required to ionize individual Rydberg states. Electric field screening is a collective effect occurring over a characteristic distance, quantified by the Debye length, λ_D. Molecular ultracold plasmas described here exhibit Debye lengths smaller than the overall size, λ_D<<σ. Plasmas of this nature offer an exotic environment for which to study fundamental phenomena. While plasmas are generally thought of as hot, UNPs exist at low enough temperatures that electrostatic interaction energy between particles is greater than their kinetic energy. At this point, charged particles begin to find themselves in local potential energy minima. Over the entire sample this translates to long-range order, or correlation. It is of great interest for researchers studying UNPs to maximize particle correlation, which requires UNPs to remain very cold, and dense through their lifetime.