Excitonic and vibrational coherence in artificial photosynthetic systems studied by negative-time ultrafast laser spectroscopy
Literature Information
Dongjia Han, Bing Xue, Juan Du, Tomohiro Miyatake, Hitoshi Tamiaki, Xin Xing, Wei Yuan, Yanyan Li
Quantum coherences between excitonic states are believed to have a substantial impact on excitation energy transfer in photosynthetic systems. Here, the excitonic and vibrational coherence relaxation dynamics of artificially synthetic chlorosomes are studied by a sub 7 fs negative-time-delay laser spectroscopy at room temperature. The results provide direct evidence for the quantum coherence of the excitonic dephasing time of 23 ± 1 fs at physiologically relevant temperatures, which is significant in the initial step of energy transfer in chlorosome or chlorosome-like photosynthetic systems. Meanwhile, coherent molecular vibrations in the excited state are also detected without the effect of wave-packet motion in the ground state, which shows that the excited state wave-packet motion contributes greatly to the vibrational modes of ∼150 and ∼1340 cm−1 in artificial chlorosome systems.
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Physical Chemistry Chemical Physics

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.












![3,7-Di(1,1':3',1''-terphenyl-5'-yl)-10,11,12,13-tetrahydrodiindeno[7,1-de:1',7'-fg][1,3,2]dioxaphosphocin-5-ol 5-oxide structure 3,7-Di(1,1':3',1''-terphenyl-5'-yl)-10,11,12,13-tetrahydrodiindeno[7,1-de:1',7'-fg][1,3,2]dioxaphosphocin-5-ol 5-oxide structure](https://static.chemtradehub.com/structs/135/1352810-38-8-3f10.webp)
![3-[4-(difluoromethoxy)phenyl]-2-({[(9H-fluoren-9-yl)methoxy]carbonyl}amino)propanoic acid structure 3-[4-(difluoromethoxy)phenyl]-2-({[(9H-fluoren-9-yl)methoxy]carbonyl}amino)propanoic acid structure](https://static.chemtradehub.com/structs/149/1496564-27-2-952e.webp)
![(1S)-1,5-Anhydro-2-O-alpha-L-arabinopyranosyl-1-[5-hydroxy-7-({6-O-[3-(4-hydroxy-3-methoxyphenyl)propanoyl]-beta-D-glucopyranosyl}oxy)-2-(4-hydroxyphenyl)-4-oxo-4H-chromen-6-yl]-D-glucitol structure (1S)-1,5-Anhydro-2-O-alpha-L-arabinopyranosyl-1-[5-hydroxy-7-({6-O-[3-(4-hydroxy-3-methoxyphenyl)propanoyl]-beta-D-glucopyranosyl}oxy)-2-(4-hydroxyphenyl)-4-oxo-4H-chromen-6-yl]-D-glucitol structure](https://static.chemtradehub.com/structs/225/2252345-81-4-bcff.webp)