类胡萝卜素二聚体中的单线态裂变——交换和偶极相互作用的作用

IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL Physical Chemistry Chemical Physics Pub Date : 2025-01-13 DOI:10.1039/d4cp04445b
Alexandru G. Ichert, William Barford
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引用次数: 0

摘要

单线态裂变理论在类胡萝卜素二聚体提出,其目的是解释背后的机制创造两个不相关的三胞胎。在类胡萝卜素链“亮”的n1B+u态激发后,有超快的内部转换到链内“暗”的11B−u三对态。这种强交换耦合状态演变成一对在独立链和自旋退相干上的三重态,形成一对单一的、不纠缠的三重态,对应于完全的单重态裂变。二聚体中平行番茄红素单体(即h -聚集体)的模拟EPR光谱显示出明显的光谱信号,这是由于在不同的类胡萝卜素链上的三联体对之间存在残留的交换偶联。
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Singlet fission in carotenoid dimers – the role of the exchange and dipolar interactions
A theory of singlet fission in carotenoid dimers is presented which aims to explain the mechanism behind the creation of two uncorrelated triplets. Following the excitation of a carotenoid chain “bright” n1B+u state, there is ultrafast internal conversion to the intrachain “dark” 11Bu triplet-pair state. This strongly exchange-coupled state evolves into a pair of triplets on separate chains and spin-decoheres to form a pair of single, unentangled triplets, corresponding to complete singlet fission. The simulated EPR spectrum for parallel lycopene monomers in a dimer (i.e., H-aggregate) shows a distinct spectral signal due to the residual exchange coupling between the triplet-pairs on seperate carotenoid chains.
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来源期刊
Physical Chemistry Chemical Physics
Physical Chemistry Chemical Physics 化学-物理:原子、分子和化学物理
CiteScore
5.50
自引率
9.10%
发文量
2675
审稿时长
2.0 months
期刊介绍: Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.
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