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| Auteurs principaux: | , , , , |
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| Format: | Preprint |
| Publié: |
2025
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| Sujets: | |
| Accès en ligne: | https://arxiv.org/abs/2503.00584 |
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| _version_ | 1866908342058745856 |
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| author | Gera, Tarun Hartzell, Alexia Chen, Lipeng Eisfeld, Alexander Raccah, Doran I. G. B. |
| author_facet | Gera, Tarun Hartzell, Alexia Chen, Lipeng Eisfeld, Alexander Raccah, Doran I. G. B. |
| contents | We present a size-invariant (i.e., $N^0$) scaling algorithm for simulating fluorescence spectroscopy in large molecular aggregates. We combine the dyadic adaptive hierarchy of pure states (DadHOPS) equation-of-motion with an operator decomposition scheme and an efficient Monte Carlo sampling algorithm to enable a formally exact, local description of the fluorescence spectrum in large molecular aggregates. Furthermore, we demonstrate that the ensemble average inverse participation ratio (IPR) of DadHOPS wave functions reproduces the delocalization extent extracted from fluorescence spectroscopy of J-aggregates with strong vibronic transitions. This work provides a computationally efficient framework for fluorescence simulations, offering a new tool for understanding the optical properties of mesoscale molecular systems. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2503_00584 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Formally exact fluorescence spectroscopy simulations for mesoscale molecular aggregates with $N^0$ scaling Gera, Tarun Hartzell, Alexia Chen, Lipeng Eisfeld, Alexander Raccah, Doran I. G. B. Chemical Physics We present a size-invariant (i.e., $N^0$) scaling algorithm for simulating fluorescence spectroscopy in large molecular aggregates. We combine the dyadic adaptive hierarchy of pure states (DadHOPS) equation-of-motion with an operator decomposition scheme and an efficient Monte Carlo sampling algorithm to enable a formally exact, local description of the fluorescence spectrum in large molecular aggregates. Furthermore, we demonstrate that the ensemble average inverse participation ratio (IPR) of DadHOPS wave functions reproduces the delocalization extent extracted from fluorescence spectroscopy of J-aggregates with strong vibronic transitions. This work provides a computationally efficient framework for fluorescence simulations, offering a new tool for understanding the optical properties of mesoscale molecular systems. |
| title | Formally exact fluorescence spectroscopy simulations for mesoscale molecular aggregates with $N^0$ scaling |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2503.00584 |