Signatures of coherent energy transfer and exciton delocalization in time-resolved optical cross correlations
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| Format: | Preprint |
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2025
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| _version_ | 1866914288509124608 |
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| author | Gestsson, Hallmann Óskar Olaya-Castro, Alexandra |
| author_facet | Gestsson, Hallmann Óskar Olaya-Castro, Alexandra |
| contents | We investigate how optical second-order cross correlations witness the quantum features of a prototype donor-acceptor light-harvesting unit. By considering a pair of detuned two-level emitters electronically coupled and incoherently driven to a non-equilibrium steady-state, we gain insight into how electronic quantum properties such as exciton eigenstate delocalization, coherent energy transfer and steady-state electronic coherence, are manifested in the joint probability of emission or optical second-order cross correlation. Specifically, we show that the frequency associated with oscillations present in time-resolved second-order cross correlation functions quantifies not only the time scale of coherent energy transfer but also the degree of delocalization of the exciton eigenstates. Furthermore, we show that time-resolved cross correlations directly witness steady-state electronic coherence. Our work strengthens the idea that measurements of the intensity quantum cross correlations can provide distinctive signatures of the quantum behavior of biophysical emitters. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2512_17741 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Signatures of coherent energy transfer and exciton delocalization in time-resolved optical cross correlations Gestsson, Hallmann Óskar Olaya-Castro, Alexandra Chemical Physics Biological Physics Quantum Physics We investigate how optical second-order cross correlations witness the quantum features of a prototype donor-acceptor light-harvesting unit. By considering a pair of detuned two-level emitters electronically coupled and incoherently driven to a non-equilibrium steady-state, we gain insight into how electronic quantum properties such as exciton eigenstate delocalization, coherent energy transfer and steady-state electronic coherence, are manifested in the joint probability of emission or optical second-order cross correlation. Specifically, we show that the frequency associated with oscillations present in time-resolved second-order cross correlation functions quantifies not only the time scale of coherent energy transfer but also the degree of delocalization of the exciton eigenstates. Furthermore, we show that time-resolved cross correlations directly witness steady-state electronic coherence. Our work strengthens the idea that measurements of the intensity quantum cross correlations can provide distinctive signatures of the quantum behavior of biophysical emitters. |
| title | Signatures of coherent energy transfer and exciton delocalization in time-resolved optical cross correlations |
| topic | Chemical Physics Biological Physics Quantum Physics |
| url | https://arxiv.org/abs/2512.17741 |