Department of Physics, City College of the City University of New York, New York, New York 10031, USA.
J Chem Phys. 2013 Sep 21;139(11):114111. doi: 10.1063/1.4820907.
Recent observations of considerable spin polarization in photoemission from metal surfaces through monolayers of chiral molecules were followed by several efforts to rationalize the results as the effect of spin-orbit interaction that accompanies electronic motion on helical, or more generally strongly curved, potential surfaces. In this paper we (a) argue, using simple models, that motion in curved force-fields with the typical energies used and the characteristic geometry of DNA cannot account for such observations; (b) introduce the concept of induced spin filtering, whereupon selectivity in the transmission of the electron orbital angular momentum can induce spin selectivity in the transmission process provided there is strong spin-orbit coupling in the substrate; and (c) show that the spin polarization in the tunneling current as well as the photoemission current from gold covered by helical adsorbates can be of the observed order of magnitude. Our results can account for most of the published observations that involved gold and silver substrates; however, recent results obtained with an aluminum substrate can be rationalized within the present model only if strong spin-orbit coupling is caused by the built-in electric field at the molecule-metal interface.
最近的观察表明,通过手性分子单层,金属表面光电子发射具有相当大的自旋极化。随后,人们做出了几种努力,试图将结果解释为伴随电子运动的自旋轨道相互作用的影响,这种相互作用发生在螺旋的,或者更一般地说,强烈弯曲的势面上。在本文中,我们(a)使用简单的模型论证,在典型能量和 DNA 的典型几何形状下,在弯曲力场中的运动并不能解释这些观察结果;(b)引入诱导自旋过滤的概念,即电子轨道角动量的传输选择性可以在存在强自旋轨道耦合的情况下诱导传输过程中的自旋选择性;(c)表明,在金覆盖的螺旋吸附物中,隧穿电流和光电子发射电流的自旋极化可以达到观察到的量级。我们的结果可以解释大多数涉及金和银基底的已发表观察结果;然而,只有当分子-金属界面处的内置电场引起强自旋轨道耦合时,目前的模型才能合理地解释最近用铝基底获得的结果。