Erić Vesna, Castro Jorge Luis, Li Xinmeng, Dsouza Lolita, Frehan Sean K, Huijser Annemarie, Holzwarth Alfred R, Buda Francesco, Sevink G J Agur, de Groot Huub J M, Jansen Thomas L C
Zernike Institute for Advanced Materials, University of Groningen, 9747 AG Groningen, The Netherlands.
Department of Chemistry and Hylleraas Centre for Quantum Molecular Sciences, University of Oslo, Sem Sælands vei 26, 0315 Oslo, Norway.
J Phys Chem B. 2023 Aug 31;127(34):7487-7496. doi: 10.1021/acs.jpcb.3c04719. Epub 2023 Aug 18.
Chlorosomes from green bacteria perform the most efficient light capture and energy transfer, as observed among natural light-harvesting antennae. Hence, their unique functional properties inspire developments in artificial light-harvesting and molecular optoelectronics. We examine two distinct organizations of the molecular building blocks as proposed in the literature, demonstrating how these organizations alter light capture and energy transfer, which can serve as a mechanism that the bacteria utilize to adapt to changes in light conditions. Spectral simulations of polarization-resolved two-dimensional electronic spectra unravel how changes in the helicity of chlorosomal aggregates alter energy transfer. We show that ultrafast anisotropy decay presents a spectral signature that reveals contrasting energy pathways in different chlorosomes.
正如在自然光捕获天线中所观察到的那样，绿细菌的叶绿体执行着最有效的光捕获和能量转移。因此，它们独特的功能特性激发了人工光捕获和分子光电子学的发展。我们研究了文献中提出的分子构建块的两种不同组织方式，展示了这些组织方式如何改变光捕获和能量转移，这可以作为细菌用来适应光照条件变化的一种机制。偏振分辨二维电子光谱的光谱模拟揭示了叶绿体聚集体螺旋度的变化如何改变能量转移。我们表明，超快各向异性衰减呈现出一种光谱特征，揭示了不同叶绿体中对比鲜明的能量路径。
