Long-Range Nonequilibrium Coherent Tunneling Induced by Fractional Vibronic Resonances.

We study the influence of a linear energy bias on a nonequilibrium excitation on a chain of molecules coupled to local vibrations (a tilted Holstein model) using both a random-walk rate kernel theory and a nonperturbative, massively parallelized adaptive-basis algorithm. We uncover structured and discrete vibronic resonance behavior fundamentally different from both linear response theory and homogeneous polaron dynamics. Remarkably, resonance between the phonon energy ℏω and the bias δϵ occurs not only at integer but also fractional ratios δϵ/(ℏω) = m/n, which effect long-range n-bond m-phonon tunneling. These observations are reproduced in a model calculation of a recently demonstrated Cy3 system, and the effect of dipole-dipole-type non-nearest-neighbor coupling and vibrationally relaxed initial states is also considered. Potential applications range from molecular electronics to optical lattices and artificial light harvesting via vibronic engineering of coherent quantum transport.

Interface-Induced Conservation of Momentum Leads to Chiral-Induced Spin Selectivity.

We study the nonequilibrium dynamics of electron transmission from a straight waveguide to a helix with spin-orbit coupling. Transmission is found to be spin-selective and can lead to large spin polarizations of the itinerant electrons. The degree of spin selectivity depends on the width of the interface region, and no polarization is found for single-point couplings. We show that this is due to momentum conservation conditions arising from extended interfaces. We therefore identify interface structure and conservation of momentum as crucial ingredients for chiral-induced spin selectivity, and we confirm that this mechanism is robust against static disorder.