钌基光敏剂与脂质膜结合诱导的激子局域化
Exciton Localization on Ru-based Photosensitizers Induced by Binding to Lipid Membranes
摘要：
表征嵌入膜环境中的金属配合物的电子性质对于开发光遗传学应用中的高效光敏剂至关重要。分子动力学和QM/MM模拟以及定量波函数分析揭示了嵌入在脂质双层和水中的[Ru（bpy）2（bpy-C17）]2+激发后形成的激子之间的不可预见的差异，尽管介质不影响吸收光谱的电荷转移特性和激发能。在水中，激子主要是离域的两个配体和非极性取代基的存在下诱导的电子跃迁的方向性。相反，当光敏剂嵌入到脂质膜中时，激子尺寸减小，并且由于与双层的带正电荷表面的静电相互作用而更局限于一个bypyridyl位点。这些差异表明，金属络合物的电子结构可以通过与外部物质的结合来控制，强调了环境在激发时引导电子流的关键作用，从而有助于合理调整光遗传学试剂。
英文摘要：
The characterization of electronic properties of metal complexes embedded in membrane environments is of paramount importance to develop efficient photosensitizers in optogenetic applications. Molecular dynamics and QM/MM simulations together with quantitative wavefunction analysis reveal an unforeseen difference between the exciton formed upon excitation of [Ru(bpy)2(bpy-C17)]2+ embedded in a lipid bilayer and in water, despite the media does not influence the charge-transfer character and the excitation energy of the absorption spectra. In water the exciton is mainly delocalized over two ligands and the presence of non-polar substituents induces directionality of the electronic transition. Instead, when the photosensitizer is embedded into a lipid membrane, the exciton size diminishes and is more localized at one bypyridyl site due to electrostatic interactions with the positively charged surface of the bilayer. These differences show that the electronic structure of metal complexes can be controlled through the binding to external species, underscoring the crucial role of the environment in directing the electronic flow upon excitation and thus helping rational tuning of optogenetic agents.
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