Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer

• URL: http://arxiv.org/abs/2603.23427v1
• Date: Tue, 24 Mar 2026 16:57:00 GMT
• Title: Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer
• Abstract summary: Exciton transport in molecular aggregates is a fundamental process governing the performance of organic optoelectronics and light-harvesting systems.<n>Recent advances in ultrafast spectroscopy have brought into focus the short-time regime, in which exciton motion remains ballistic on femtosecond-to-picosecond timescales.<n>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 fluctuations.
• Score: 6.900133159039129
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: 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.

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