Recent experiments on electron scattering through molecular films have shown that chiral molecules can be efficient sources of polarized electrons even in the absence of heavy nuclei as source of a strong spin-orbit interaction. We show that self-assembled monolayers (SAMs) of chiral molecules are strong electron polarizers due to the high density effect of the monolayers and explicitly compute the scattering amplitude off a helical molecular model of carbon atoms. Longitudinal polarization is shown to be the signature of chiral scattering. For elastic scattering, we find that at least double scattering events must take place for longitudinal polarization to arise. We predict energy windows for strong polarization, determined by the energy dependences of spin-orbit strength and multiple scattering probability. An incoherent mechanism for polarization amplification is proposed, that increases the polarization linearly with the number of helix turns, consistent with recent experiments on DNA SAMs.
We analyze single scattering of unpolarized photoelectrons through a monolayer of chiral molecules modeled by a continuous hardcore helix and spin-orbit coupling. The molecular helix is represented by an optical contact potential containing a non-hermitian component describing inelastic events. Transmitted photoelectrons are transversely polarized at optimal angles, and separated into up and down spin with up to 20% efficiency. Such a process involves the interference of both spin-orbit and inelastic strengths, that are parameterized quantitatively to recent experiments in chiral self-assembled monolayers (SAMs). The structure factor of the model chiral molecule shows the energy dependence of the differential cross section which decays strongly as energy increases. Larger incident momenta reduce axial deviations from the forward direction and the spin-orbit interaction becomes less effective. Transverse electron polarization is then restricted to a characteristic energy window.
We carried out a molecular-dynamics (MD) study of the self-diffusion tensor of a Lennard-Jones-type fluid, confined in a slit pore with attractive walls. We developed Bayesian equations, which modify the virtual layer sampling method proposed by Liu, Harder, and Berne (LHB) [P. Liu, E. Harder, and B. J. Berne, J. Phys. Chem. B 108, 6595 (2004)]. Additionally, we obtained an analytical solution for the corresponding nonhomogeneous Langevin equation. The expressions found for the mean-squared displacement in the layers contain naturally a modification due to the mean force in the transverse component in terms of the anisotropic diffusion constants and mean exit time. Instead of running a time consuming dual MD-Langevin simulation dynamics, as proposed by LHB, our expression was used to fit the MD data in the entire survival time interval not only for the parallel but also for the perpendicular direction. The only fitting parameter was the diffusion constant in each layer.
We present an experimental and theoretical study of the kinetic energy dependence of spin filtering of electrons by organized layers of DNA adsorbed on a gold substrate. When Au 4f7/2,5/2 levels are ionized by circularly polarized X-rays, the emitted electrons will be spin polarized. The spin distribution depends on the particular sublevel and is opposite for right versus left circularly polarized light. If the DNA overlayer preferentially attenuates one spin over another, then there should be a circular dichroism (CD) in the X-ray photoelectron spectroscopy (XPS) spectra observed with the different polarizations. Using synchrotron radiation excitation, XPS CD measurements were made of electrons with kinetic energies in the range 30 to 760 eV. In all cases there was no evidence of any significant dichroism. These results are explained by a model in which the longitudinal polarization is strongly dependent on the k-vector, and hence the energy or the de Broglie wavelength, which are simply connected to the magnitude of this vector of the incoming electrons. For a helix with a fixed number of turns, this dependence is due to a coherent process associated with multiple scattering. This model predicts that there is a window of energies where changes in the polarization should be expected. Two competing effects determine this window: The energy has to be small enough to allow for at least double scattering, but large enough so that the de Broglie wavelength probes the chiral structure. Also at very low energies the spin–orbit interaction weakens and no polarization results.
We present an analytical model for the role of hydrogen bonding on the spin-orbit coupling of model DNA molecule. Here we analyze in detail the electric fields due to the polarization of the Hydrogen bond on the DNA base pairs and derive, within tight binding analytical band folding approach, an intrinsic Rashba coupling which should dictate the order of the spin active effects in the Chiral-Induced Spin Selectivity (CISS) effect. The coupling found is ten times larger than the intrinsic coupling estimated previously and points to the predominant role of hydrogen bonding in addition to chirality in the case of biological molecules. We expect similar dominant effects in oligopeptides, where the chiral structure is supported by hydrogen-bonding and bears on orbital carrying transport electrons.
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