通过纳米等离子体激元在捕光蛋白质中塑造激子
Shaping excitons in light-harvesting proteins through nanoplasmonics
摘要：
纳米等离子体已被用于增强分子光谱信号，具有精确到亚分子尺度的空间分辨率。通过一个严格的，最先进的多尺度模型的基础上的量子化学描述，在这里，我们表明，最佳调谐的尖端形状的金属纳米粒子可以选择性地激发典型的相干系统的局部区域，最终缩小到探测一个单一的色素。紫色细菌的主要捕光复合物LH 2由于其独特的性质而被研究，因为它在色素子簇之间呈现出高和弱的离域性。这一发现开辟了直接光谱调查的量子为基础的过程，如量子扩散的激发之间的发色团，和他们的外部操纵
英文摘要：
Nanoplasmonics has been used to enhance molecular spectroscopic signals, with exquisite spatial resolution down to the sub-molecular scale. By means of a rigorous, state-of-the-art multiscale model based on a quantum chemical description, here we show that optimally tuned tip-shaped metal nanoparticles can selectively excite localized regions of typically coherent systems, eventually narrowing down to probing one single pigment. The well-known major light-harvesting complex LH2 of purple bacteria has been investigated because of its unique properties, as it presents both high and weak delocalization among subclusters of pigments. This finding opens the way to the direct spectroscopic investigation of quantum-based processes, such as the quantum diffusion of the excitation among the chromophores, and their external manipulation
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