标题： 对映选择性自由基反应可通过电子自旋极化诱导：自然界出现的均一手性的一种量子机制？ 显示英文标题

标题： Enantioselective radical reactions can be induced by electron spin polarization: A quantum mechanism for Nature's emergent homochirality?

摘要： 构成地球生命的生物分子具有手性，但同源手性出现的精确机制仍然是一个谜。 在本研究中，展示了当自由基对中一个自由基的电子自旋被极化时，其反应可以具有对映选择性。 这种现象源于自由基对电子自旋的瞬时光学量子动力学，这种现象即使在温暖且嘈杂的凝聚相环境中也会发生，其中比热能小得多的能量扰动会对反应性产生重大影响。 提出了一种定量理论，该理论基于手性诱导自旋选择性（CISS）的分子理论，其中电子交换相互作用和与手性相关的自旋-轨道耦合效应控制对映选择性。 该理论为这些反应的最大对映体过量提供了有用的界限，这些界限与先前的实验结果一致。 这里提出的对映选择性自由基对机制为最近的一项提议提供了另一种机制基础，即磁铁矿产生的自旋极化光电子提供了自然中同源手性起源所需的初始手性对称性破缺，同时也建议了一种使用自旋极化电子进行不对称合成的新策略。 显示英文摘要

摘要： Biomolecules that constitute life on Earth are chiral, but the precise mechanism by which homochirality emerged remains a mystery. In this work it is demonstrated that reactions of radical pairs, where one of the radical electron spins is polarised, can be enantioselective. This phenomenon arises from transient coherent quantum dynamics of the radical pair electron spins, which is known to occur even in warm and noisy condensed phase environments, where energetic perturbations much smaller than thermal energy can have large effects on reactivity. A quantitative theory is presented based on the molecular theory of chirality induced spin selectivity (CISS), where electron exchange interactions and chirality-dependent spin-orbit coupling effects control enantioselectivity. This theory provides useful bounds on the maximum enantiomeric excess for these reactions, which are found to be consistent with previous experiments. The enantioseletive radical pair mechanism presented here provides an alternative mechanistic basis to a recent proposal that spin-polarised photoelectrons from magnetite provided the initial chiral symmetry breaking necessary for the inception of homochirality in Nature, as well as suggests a new strategy for asymmetric synthesis using spin-polarised electrons.