论文标题

关于生命同Rirality的起源:用自旋极化电子诱导对映体过量

On the Origins of Life's Homochirality: Inducing Enantiomeric Excess with Spin-Polarized Electrons

论文作者

Ozturk, S. Furkan, Sasselov, Dimitar D.

论文摘要

我们所知道的这是同源性的,但生物同源性在早期地球上的起源仍然难以捉摸。浅闭合巴辛湖是地球早期的合理益生元环境,预计大多数将具有明显的沉积磁铁矿沉积物。我们假设磁铁矿沉积物的紫外线(200-300nm)可以产生足以诱导手性选择性益生元化学的水合的自旋偏振电子。这样的电子是有效的还原剂,可驱动自旋极化方向可以改变对映射反应动力学的反应。我们对这种手性偏置的估计是基于在手性诱导的自旋选择性(CISS)效应中观察到的强有有效的自旋轨道耦合,适用于不同异构体的还原反应中的能量差异。在最初的CISS实验中,在室温下观察到通过DSDNA分子的单层传播的自旋选择性电子传输 - 表明分子手性和电子自旋之间存在很强的耦合。我们提出,当应用于还原化学时,由于CISS效应而导致的手性对称性破坏可以诱导益生元地球上的对映选择性合成,从而促进生命构件的同源性组装。

Life as we know it is homochiral, but the origins of biological homochirality on early Earth remain elusive. Shallow closed-basin lakes are a plausible prebiotic environment on early Earth, and most are expected to have significant sedimentary magnetite deposits. We hypothesize that UV (200-300nm) irradiation of magnetite deposits could generate hydrated spin-polarized electrons sufficient to induce chirally selective prebiotic chemistry. Such electrons are potent reducing agents that drive reduction reactions where the spin polarization direction can alter enantioselectively the reaction kinetics. Our estimate of this chiral bias is based on the strong effective spin-orbit coupling observed in the chiral-induced spin selectivity (CISS) effect, as applied to energy differences in reduction reactions for different isomers. In the original CISS experiments, spin selective electron transmission through a monolayer of dsDNA molecules is observed at room temperature - indicating a strong coupling between molecular chirality and electron spin. We propose that the chiral symmetry breaking due to the CISS effect, when applied to reduction chemistry, can induce enantioselective synthesis on the prebiotic Earth and thus facilitate the homochiral assembly of life's building blocks.

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