受限空间中的分子光开关。,Accounts of Chemical Research

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受限空间中的分子光开关。
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2020-09-24 , DOI: 10.1021/acs.accounts.0c00434
Angela B Grommet ₁ , Lucia M Lee ₁ , Rafal Klajn ₁

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在自然界中，光敏蛋白收集光以驱动一系列生物过程，包括光合作用，趋光性，视觉和最终生命。例如，细菌视紫红质是一种嵌入在古细菌细胞膜中的蛋白质，可与疏水性口袋内的发色团视网膜结合。暴露于光中会触发受限视网膜的区域选择性光异构化，继而引发蛋白质内一系列构象变化，从而触发质子通量对抗浓度梯度，从而为微生物提供了生存所需的能量。自然界中的这些功能激发了我们在有限的条件下使用合成光电开关来利用光能的灵感。像视网膜一样，合成光电开关需要一定程度的构象灵活性才能异构化。在自然界，视蛋白宿主的结构柔韧性可以适应与视网膜异构化相关的构象变化，但它会导致生色团与蛋白质之间发生空间连通。类似地，我们努力设计这样的系统，其中受限的光开关的异构化导致光开关与其封闭环境之间的空间连通。为了达到这个目的，必须在限制状态下在分子拥挤和构象自由之间取得平衡：过多的拥挤会阻止切换，而太多的自由则类似于溶液中孤立分子的切换，从而阻止了交流。我们努力设计这样的系统，其中受限的光开关的异构化会导致光开关与其封闭环境之间的空间连通。为了达到这个目的，必须在限制状态下在分子拥挤和构象自由之间取得平衡：过多的拥挤会阻止切换，而太多的自由则类似于溶液中孤立分子的切换，从而阻止了交流。我们努力设计这样的系统，其中受限的光开关的异构化会导致光开关与其封闭环境之间的空间连通。为了达到这个目的，必须在限制状态下在分子拥挤和构象自由之间取得平衡：过多的拥挤会阻止切换，而太多的自由则类似于溶液中孤立分子的切换，从而阻止了交流。

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Molecular Photoswitching in Confined Spaces.

In nature, light is harvested by photoactive proteins to drive a range of biological processes, including photosynthesis, phototaxis, vision, and ultimately life. Bacteriorhodopsin, for example, is a protein embedded within archaeal cell membranes that binds the chromophore retinal within its hydrophobic pocket. Exposure to light triggers regioselective photoisomerization of the confined retinal, which in turn initiates a cascade of conformational changes within the protein, triggering proton flux against the concentration gradient, providing the microorganisms with the energy to live. We are inspired by these functions in nature to harness light energy using synthetic photoswitches under confinement. Like retinal, synthetic photoswitches require some degree of conformational flexibility to isomerize. In nature, the conformational change associated with retinal isomerization is accommodated by the structural flexibility of the opsin host, yet it results in steric communication between the chromophore and the protein. Similarly, we strive to design systems wherein isomerization of confined photoswitches results in steric communication between a photoswitch and its confining environment. To achieve this aim, a balance must be struck between molecular crowding and conformational freedom under confinement: too much crowding prevents switching, whereas too much freedom resembles switching of isolated molecules in solution, preventing communication.

更新日期：2020-11-17

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