Orientational Dynamics of Transition Dipoles and Exciton Relaxation in LH2 from Ultrafast Two-Dimensional Anisotropy.
Orientational Dynamics of Transition Dipoles and Exciton Relaxation in LH2 from Ultrafast Two-Dimensional Anisotropy.
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超快二维各向异性 LH2 中跃迁偶极子的取向动力学和激子弛豫。
DOI：
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发表时间：
2019
影响因子：
5.7
通讯作者：
G. Engel
中科院分区：
文献类型：
--
作者：
Sara C. Massey;Po;Shu;Shu;P. Dahlberg;Sara H Sohail;M. A. Allodi;E. C. Martin;S. Kais;C. Hunter;G. Engel
光合生物中的捕光复合物显示出快速有效的能量传递动力学，这关键取决于复合物内耦合发色团的电子结构及其与环境的相互作用。我们提出了超快各向异性动力学，解决在时间和频率，跨膜捕光复合物LH2从Rhodobacter sphaeroides在其原生膜环境中使用偏振控制的二维电子光谱。从实验和改进的Redfield模拟获得的随时间变化的各向异性揭示了激发态吸收和超快平衡在LH2的B850带内的取向偏好。这种超快平衡有利于随后向反应中心的能量转移。我们的研究结果还表明，激发态吸收各向异性之间的直接激发的B850人口和人口，最初在800 nm处激发的动态差异，这表明从B850状态的吸收更高的激发态的能量转移从B850 *。这些结果提供了洞察细菌光捕获的超快动力学和LH2在天然膜环境中的激发态能量景观。
Light-harvesting complexes in photosynthetic organisms display fast and efficient energy transfer dynamics, which depend critically on the electronic structure of the coupled chromophores within the complexes and their interactions with their environment. We present ultrafast anisotropy dynamics, resolved in both time and frequency, of the transmembrane light-harvesting complex LH2 from Rhodobacter sphaeroides in its native membrane environment using polarization-controlled two-dimensional electronic spectroscopy. Time-dependent anisotropy obtained from both experiment and modified Redfield simulation reveals an orientational preference for excited state absorption and an ultrafast equilibration within the B850 band in LH2. This ultrafast equilibration is favorable for subsequent energy transfer toward the reaction center. Our results also show a dynamic difference in excited state absorption anisotropy between the directly excited B850 population and the population that is initially excited at 800 nm, suggesting absorption from B850 states to higher-lying excited states following energy transfer from B850*. These results give insight into the ultrafast dynamics of bacterial light harvesting and the excited state energy landscape of LH2 in the native membrane environment.
球形红杆菌 B850 天线复合体中的超快激子弛豫。
DOI：
10.1073/pnas.93.24.13774
发表时间：
1996
影响因子：
11.1
作者：
Nagarajan,V;Alden,RG;Williams,JC;Parson,WW
通讯作者：
Parson,WW
DOI：
10.1063/1.4921324
发表时间：
2015
期刊：
The Journal of chemical physics
影响因子：
--
作者：
Singh,VP;Westberg,M;Wang,C;Dahlberg,PD;Gellen,T;Gardiner,AT;Cogdell,RJ;Engel,GS
通讯作者：
Engel,GS
通讯：光捕获复合物 1 中广泛的激子态促进体内有效的单向能量转移。
DOI：
10.1063/1.4999057
发表时间：
2017
期刊：
The Journal of chemical physics
影响因子：
--
作者：
Sohail,SaraH;Dahlberg,PeterD;Allodi,MarcoA;Massey,SaraC;Ting,Po-Chieh;Martin,ElizabethC;Hunter,CNeil;Engel,GregoryS
通讯作者：
Engel,GregoryS