Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission

• URL: http://arxiv.org/abs/2601.05372v1
• Date: Thu, 08 Jan 2026 20:53:30 GMT
• Title: Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission
• Authors: Kerwan Morin, Poulab Chakrabarti, Delphine Lagarde, Maxime Mauguet, Sylwia Zielińska - Raczyńska, David Ziemkiewicz, Xavier Marie, Thomas Boulier,
• Abstract summary: Rydberg excitons give rise to two very different optical responses under resonant two-photon excitation.<n>We map how each depends on $n$, temperature, excitation power, and crystal quality.<n>Our results provide a unified framework for interpreting emission from Rydberg excitons.
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• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Rydberg excitons in $\mathrm{Cu_2O}$ simultaneously give rise to two very different optical responses under resonant two-photon excitation: a coherent second-harmonic signal mediated by the excitonic second order susceptibility tensor $χ^{(2)}$, and a secondary emission originating from the radiative decay of real exciton populations. Distinguishing these two channels is essential for interpreting nonlinear and quantum-optical experiments based on high-$n$ states, yet their temporal, spectral, and power-dependent signatures often overlap. Here we use time-resolved resonant two-photon excitation to cleanly separate SHG and SE and to map how each depends on $n$, temperature, excitation power, and crystal quality. This approach reveals the markedly different sensitivities of the two processes to phonons, defects, and many-body effects, and establishes practical criteria for identifying SE and SHG in a wide range of experimental conditions. Our results provide a unified framework for interpreting emission from Rydberg excitons and offer guidelines for future studies aiming to exploit their nonlinear response and long-range interactions.

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