Quantum Ghost Spectroscopy Reveals Hidden Electronic Coherence in Molecular Aggregates
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arXiv
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| Autores principales: | , , , |
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| Formato: | Preprint |
| Publicado: |
2026
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| _version_ | 1866914592381206528 |
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| author | Zhang, Mingran Xu, Yihe Yakovlev, Vladislav V. Zhang, Zhedong |
| author_facet | Zhang, Mingran Xu, Yihe Yakovlev, Vladislav V. Zhang, Zhedong |
| contents | Ultrafast spectroscopy of molecular systems is fundamentally constrained by the Fourier uncertainty principle: high temporal resolution smears out electronic state signatures, while high spectral resolution obscures dynamic information. Here we overcome this limitation using time-resolved quantum ghost spectroscopy (tr-QGS) with entangled photon pairs, which enables independent control of temporal and spectral scales. We apply this approach to perylene bismide (PBI-1) trimers for energy transfer,by combining a quantum description of light-molecule interaction with time-dependent density matrix renormalization group (TD-DMRG) simulations. This explicitly includes five vibrational modes and nonadiabatic coupling between electronic states. Our simulations reveal that tr-QGS uniquely captures electronic coherence oscillating at 0.7 eV for >50 fs, a signature of nonadiabatic coupling that was obscured in conventional time-resolved fluorescence due to Fourier-limited broadening. Moreover, we observe a direct transfer from electronic to vibrational coherence at 200 fs, providing real-time visualization of vibronic relaxation pathways. The entangled photon correlation enables a sensitivity below the shot-noise limit and suppresses photobleaching artifacts that plague classical measurements. These results establish tr-QGS as a transformative tool for interrogating nonadiabatic dynamics in molecular aggregates, light-harvesting complexes, and photocatalysts, offering a route to reveal quantum coherence in chemistry with unprecedented time-energy precision. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2605_23639 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Quantum Ghost Spectroscopy Reveals Hidden Electronic Coherence in Molecular Aggregates Zhang, Mingran Xu, Yihe Yakovlev, Vladislav V. Zhang, Zhedong Quantum Physics Ultrafast spectroscopy of molecular systems is fundamentally constrained by the Fourier uncertainty principle: high temporal resolution smears out electronic state signatures, while high spectral resolution obscures dynamic information. Here we overcome this limitation using time-resolved quantum ghost spectroscopy (tr-QGS) with entangled photon pairs, which enables independent control of temporal and spectral scales. We apply this approach to perylene bismide (PBI-1) trimers for energy transfer,by combining a quantum description of light-molecule interaction with time-dependent density matrix renormalization group (TD-DMRG) simulations. This explicitly includes five vibrational modes and nonadiabatic coupling between electronic states. Our simulations reveal that tr-QGS uniquely captures electronic coherence oscillating at 0.7 eV for >50 fs, a signature of nonadiabatic coupling that was obscured in conventional time-resolved fluorescence due to Fourier-limited broadening. Moreover, we observe a direct transfer from electronic to vibrational coherence at 200 fs, providing real-time visualization of vibronic relaxation pathways. The entangled photon correlation enables a sensitivity below the shot-noise limit and suppresses photobleaching artifacts that plague classical measurements. These results establish tr-QGS as a transformative tool for interrogating nonadiabatic dynamics in molecular aggregates, light-harvesting complexes, and photocatalysts, offering a route to reveal quantum coherence in chemistry with unprecedented time-energy precision. |
| title | Quantum Ghost Spectroscopy Reveals Hidden Electronic Coherence in Molecular Aggregates |
| topic | Quantum Physics |
| url | https://arxiv.org/abs/2605.23639 |