Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission
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arXiv
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| Auteurs principaux: | , , , , , , , |
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| Format: | Preprint |
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2026
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| _version_ | 1866912810741530624 |
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| author | Morin, Kerwan Chakrabarti, Poulab Lagarde, Delphine Mauguet, Maxime Raczyńska, Sylwia Zielińska - Ziemkiewicz, David Marie, Xavier Boulier, Thomas |
| author_facet | Morin, Kerwan Chakrabarti, Poulab Lagarde, Delphine Mauguet, Maxime Raczyńska, Sylwia Zielińska - Ziemkiewicz, David Marie, Xavier Boulier, Thomas |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2601_05372 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission Morin, Kerwan Chakrabarti, Poulab Lagarde, Delphine Mauguet, Maxime Raczyńska, Sylwia Zielińska - Ziemkiewicz, David Marie, Xavier Boulier, Thomas Quantum Gases Quantum Physics 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. |
| title | Emission Dynamics of Rydberg Excitons in $\mathbf{\mathrm{Cu_2O}}$: Distinguishing Second Harmonic Generation from Secondary Emission |
| topic | Quantum Gases Quantum Physics |
| url | https://arxiv.org/abs/2601.05372 |