Correlation-induced phase shifts and time delays in resonance enhanced high harmonic generation from Cr+
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| Main Authors: | , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866915562593976320 |
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| author | Aharon, Yoad Pick, Adi Hen, Amir Marcus, Gilad Neufeld, Ofer |
| author_facet | Aharon, Yoad Pick, Adi Hen, Amir Marcus, Gilad Neufeld, Ofer |
| contents | We investigate resonance-enhanced high harmonic generation (rHHG) in Cr+ by comparing a 1D shape-resonant model, time-dependent density functional theory (TDDFT), and independent particle approximation (IPA) simulations. Previous studies linked rHHG to the 3p -> 3d giant resonance, suggesting a modified four-step model where recolliding electrons are first captured in the autoionizing state before recombining into the ground state, potentially leading to an emission delay associated with the resonance lifetime. While both the 1D-model and TDDFT reproduce experimental spectra, TDDFT reveals that rHHG counterintuitively originates from spin-down 3p states, while spin-up 3d electrons negligibly contribute. The IPA fails to reproduce rHHG, highlighting the significance of electron correlations. Furthermore, TDDFT revealed a correlation induced ~480 attosecond time delay, accompanied by a strong phase shift across the resonance, potentially explaining earlier RABBIT measurements. Our work sheds light on long-standing open questions in rHHG and should advance novel ultrafast spectroscopies of electron correlations and resonances. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2507_00526 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Correlation-induced phase shifts and time delays in resonance enhanced high harmonic generation from Cr+ Aharon, Yoad Pick, Adi Hen, Amir Marcus, Gilad Neufeld, Ofer Atomic Physics We investigate resonance-enhanced high harmonic generation (rHHG) in Cr+ by comparing a 1D shape-resonant model, time-dependent density functional theory (TDDFT), and independent particle approximation (IPA) simulations. Previous studies linked rHHG to the 3p -> 3d giant resonance, suggesting a modified four-step model where recolliding electrons are first captured in the autoionizing state before recombining into the ground state, potentially leading to an emission delay associated with the resonance lifetime. While both the 1D-model and TDDFT reproduce experimental spectra, TDDFT reveals that rHHG counterintuitively originates from spin-down 3p states, while spin-up 3d electrons negligibly contribute. The IPA fails to reproduce rHHG, highlighting the significance of electron correlations. Furthermore, TDDFT revealed a correlation induced ~480 attosecond time delay, accompanied by a strong phase shift across the resonance, potentially explaining earlier RABBIT measurements. Our work sheds light on long-standing open questions in rHHG and should advance novel ultrafast spectroscopies of electron correlations and resonances. |
| title | Correlation-induced phase shifts and time delays in resonance enhanced high harmonic generation from Cr+ |
| topic | Atomic Physics |
| url | https://arxiv.org/abs/2507.00526 |