Solvent Driving Force Ensures Fast Formation of a Persistent and Well-Separated Radical Pair in Plant Cryptochrome
Solvent Driving Force Ensures Fast Formation of a Persistent and Well-Separated Radical Pair in Plant Cryptochrome
复制标题
溶剂驱动力确保在植物隐色素中快速形成持久且分离良好的自由基对
DOI：
10.1021/ja510550g
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发表时间：
2015-01-28
影响因子：
15
通讯作者：
Elstner, Marcus
中科院分区：
文献类型：
--
作者：
Luedemann, Gesa;Solov'yov, Ilia A.;Elstner, Marcus
光感受器蛋白质隐花色素被认为是光吸收后，对非常弱的磁场敏感的自由基对的宿主，赋予候鸟一种磁罗盘感觉。导致形成稳定的、磁场敏感的自由基对的分子机制，尽管有各种理论和实验努力，但仍未明确确定。我们通过一种独特的量子力学分子动力学方法来挑战这种明确的方法，在这种方法中，我们进行电子转移动力学模拟，考虑到蛋白质在电子转移时的运动。这种方法使我们能够以一种无偏的方式跟踪电子转移的时间演变，并揭示确保隐色素中快速电子转移的分子驱动力，从而确保形成适合于磁接收的持久自由基对。我们认为，这种解开的分子机制是隐色素/光解酶家族所有蛋白质固有的一般原理，因此，隐色素被定制为潜在地作为有效的化学磁受体发挥作用。
The photoreceptor protein cryptochrome is thought to host, upon light absorption, a radical pair that is sensitive to very weak magnetic fields, endowing migratory birds with a magnetic compass sense. The molecular mechanism that leads to formation of a stabilized, magnetic field sensitive radical pair has despite various theoretical and experimental efforts not been unambiguously identified yet. We challenge this unambiguity through a unique quantum mechanical molecular dynamics approach where we perform electron transfer dynamics simulations taking into account the motion of the protein upon the electron transfer. This approach allows us to follow the time evolution of the electron transfer in an unbiased fashion and to reveal the molecular driving force that ensures fast electron transfer in cryptochrome guaranteeing formation of a persistent radical pair suitable for magnetoreception. We argue that this unraveled molecular mechanism is a general principle inherent to all proteins of the cryptochrome/photolyase family and that cryptochromes are, therefore, tailored to potentially function as efficient chemical magnetoreceptors.