Singlet fission in carotenoid dimers – the role of the exchange and dipolar interactions

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

引用次数: 0

Abstract

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” 1¹B⁻_u 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 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.