Tight inner ring architecture and quantum motion of nuclei enable efficient energy transfer in bacterial light harvesting.
Tight inner ring architecture and quantum motion of nuclei enable efficient energy transfer in bacterial light harvesting.
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DOI：
10.1126/sciadv.add0023
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发表时间：
2022-10-28
期刊：
影响因子：
13.6
通讯作者：
中科院分区：
文献类型：
--
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吸收的太阳能在光合作用捕光复合体之间的高效、定向转移仍然是一个有趣的问题。在这项工作中，我们用全量子力学路径积分方法确定了红假单胞菌LH2复合体中B800和B850环之间的能量流动路径，模拟了24个细菌叶绿素分子的激发态动力学及其与每个发色团中50个简正模振动的耦合。虽然所有颜料都是相同的，但B850内环的更紧密的堆积是内环的热力学稳定的原因。分子振动使1-ps的能量流到B850态，否则在动力学上是无法到达的。对振动的经典处理导致了激发的均匀平衡分布，只有67%转移到内环。然而，与原子核的量子运动相关的自发涨落将转移效率提高到90%。路径积分模拟揭示了光合细菌环间激发能量传递的机制途径。
The efficient, directional transfer of absorbed solar energy between photosynthetic light-harvesting complexes continues to pose intriguing questions. In this work, we identify the pathways of energy flow between the B800 and B850 rings in the LH2 complex of Rhodopseudomonas molischianum using fully quantum mechanical path integral methods to simulate the excited-state dynamics of the 24 bacteriochlorophyll molecules and their coupling to 50 normal mode vibrations in each chromophore. While all pigments are identical, the tighter packing of the inner B850 ring is responsible for the thermodynamic stabilization of the inner ring. Molecular vibrations enable the 1-ps flow of energy to the B850 states, which would otherwise be kinetically inaccessible. A classical treatment of the vibrations leads to uniform equilibrium distribution of the excitation, with only 67% transferred to the inner ring. However, spontaneous fluctuations associated with the quantum motion of the nuclei increase the transfer efficiency to 90%. Path integral simulations reveal the mechanistic pathway of inter-ring excitation energy transfer in photosynthetic bacteria.
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影响因子：
4.4
作者：
Abramavicius, Darius;Mukamel, Shaul
通讯作者：
Mukamel, Shaul
DOI：
10.1098/rspa.1950.0184
发表时间：
1950-01-01
影响因子：
--
作者：
HUANG, K;RHYS, A
通讯作者：
RHYS, A
影响因子：
3
作者：
FEYNMAN, RP;VERNON, FL
通讯作者：
VERNON, FL
DOI：
10.1073/pnas.0908989106
发表时间：
2009-10-13
影响因子：
11.1
作者：
Ishizaki, Akihito;Fleming, Graham R.
通讯作者：
Fleming, Graham R.
影响因子：
3.3
作者：
Jang, Seogjoo;Newton, Marshall D.;Silbey, Robert J.
通讯作者：
Silbey, Robert J.