Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer
Fuente:
arXiv
Guardado en:
| Autores principales: | , , |
|---|---|
| Formato: | Preprint |
| Publicado: |
2026
|
| Materias: | |
| Acceso en línea: | |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| _version_ | 1866910069669494784 |
|---|---|
| author | Wang, Siwei Liu, Guangming Chen, Hsing-Ta |
| author_facet | Wang, Siwei Liu, Guangming Chen, Hsing-Ta |
| contents | Exciton transport in molecular aggregates is a fundamental process governing the performance of organic optoelectronics and light-harvesting systems. While most theoretical studies have emphasized long-time transport behavior, recent advances in ultrafast spectroscopy have brought into focus the short-time regime, in which exciton motion remains ballistic on femtosecond-to-picosecond timescales. In this work, we develop an analytical framework for short-time exciton dynamics in a one-dimensional lattice subject to both on-site energetic (diagonal) disorder and intermolecular coupling (off-diagonal) fluctuations. Utilizing the reciprocal-space analysis, we derive closed-form expressions for the first and second spatial moments considering both localized excitation and moving Gaussian initial conditions. Our analytical and numerical results show that, while the long-time dynamics are influenced by diagonal disorder, the short-time ballistic expansion is governed primarily by off-diagonal disorder. Crucially, we reveal a synergistic interplay between the average intermolecular coupling and the off-diagonal coupling disorder strength, demonstrating that they contribute equivalently to short-time exciton transport. Moreover, we integrate this generic disorder model with a realistic molecular system within the framework of macroscopic quantum electrodynamics, thereby providing a theoretical foundation for characterizing and optimizing ultrafast energy flow of disordered molecular aggregates in complex dielectric media. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2603_23427 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer Wang, Siwei Liu, Guangming Chen, Hsing-Ta Chemical Physics Quantum Physics Exciton transport in molecular aggregates is a fundamental process governing the performance of organic optoelectronics and light-harvesting systems. While most theoretical studies have emphasized long-time transport behavior, recent advances in ultrafast spectroscopy have brought into focus the short-time regime, in which exciton motion remains ballistic on femtosecond-to-picosecond timescales. In this work, we develop an analytical framework for short-time exciton dynamics in a one-dimensional lattice subject to both on-site energetic (diagonal) disorder and intermolecular coupling (off-diagonal) fluctuations. Utilizing the reciprocal-space analysis, we derive closed-form expressions for the first and second spatial moments considering both localized excitation and moving Gaussian initial conditions. Our analytical and numerical results show that, while the long-time dynamics are influenced by diagonal disorder, the short-time ballistic expansion is governed primarily by off-diagonal disorder. Crucially, we reveal a synergistic interplay between the average intermolecular coupling and the off-diagonal coupling disorder strength, demonstrating that they contribute equivalently to short-time exciton transport. Moreover, we integrate this generic disorder model with a realistic molecular system within the framework of macroscopic quantum electrodynamics, thereby providing a theoretical foundation for characterizing and optimizing ultrafast energy flow of disordered molecular aggregates in complex dielectric media. |
| title | Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer |
| topic | Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2603.23427 |