光谱分辨激子-激子相互作用泵浦-探测光谱的模拟
Simulating spectrally resolved exciton--exciton-interaction pump--probe spectroscopy
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中文总结 AI 辅助
本文提出光谱分辨激子-激子相互作用泵浦-探测光谱的微观理论描述，可用于大分子体系，能区分单激子与多激子动力学，便于与实验光谱对比。
中文摘要 AI 辅助
激子-激子相互作用泵浦-探测光谱（EEI-PP）可捕捉光与物质相互作用的五阶信号，直接探测激子-激子湮灭，即便在扩展、近等能的环境中也能用于研究激发能传输。尽管光谱分辨的五阶信号已在简化案例中被探究，但在更大体系中仅分析过光谱积分信号。本文提出一种带实际线形的光谱分辨EEI-PP响应的微观理论描述，揭示单激子与多激子态结构如何塑造光谱特征与动力学；该描述适用于方酸聚合物等大分子体系，便于与实验光谱直接对比。通过将总信号分解为各激发路径，本文证明需借助光谱分辨区分原本相互交织的单激子与多激子动力学，如单激子弛豫和激子-激子湮灭。
英文摘要
Exciton--exciton-interaction pump--probe spectroscopy (EEI--PP) captures the fifth-order signal of light-matter interaction, directly probing exciton--exciton annihilation. This allows studying excitation energy transport even in extended, nearly isoenergetic landscapes. Although spectrally resolved fifth-order signals have already been explored in simplified cases, in larger systems only spectrally integrated signals have been analyzed. We present a microscopic theoretical description for spectrally resolved EEI--PP response with realistic lineshapes, revealing how single- and multi-exciton state structure shape the spectral features and dynamics. The description is applicable to large molecular systems such as squaraine polymers, facilitating a direct comparison with experimental spectra. By a decomposition of the total signal into individual excitation pathways, we demonstrate that the spectral resolution is needed to distinguish otherwise intertwined single- and multi-exciton dynamics, such as single-exciton relaxation and exciton--exciton annihilation.
发表机构
- Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院）
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