Controlling the preferential motion of chiral molecular walkers on a surface

Chemical Science
David Abbasi-PérezLev Kantorovich

Abstract

Molecular walkers standing on two or more "feet" on an anisotropic periodic potential of a crystal surface may perform a one-dimensional Brownian motion at the surface-vacuum interface along a particular direction in which their mobility is the largest. In thermal equilibrium the molecules move with equal probabilities both ways along this direction, as expected from the detailed balance principle, well-known in chemical reactivity and in the theory of molecular motors. For molecules that possess an asymmetric potential energy surface (PES), we propose a generic method based on the application of a time-periodic external stimulus that would enable the molecules to move preferentially in a single direction thereby acting as Brownian ratchets. To illustrate this method, we consider a prototypical synthetic chiral molecular walker, 1,3-bis(imidazol-1-ylmethyl)-5(1-phenylethyl)benzene, diffusing on the anisotropic Cu(110) surface along the Cu rows. As unveiled by our kinetic Monte Carlo simulations based on the rates calculated using ab initio density functional theory, this molecule moves to the nearest equivalent lattice site via the so-called inchworm mechanism in which it steps first with the rear foot and then with the front f...Continue Reading

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Citations

Sep 12, 2019·Physical Chemistry Chemical Physics : PCCP·Hongqian SangLev Kantorovich
Dec 8, 2020·Beilstein Journal of Organic Chemistry·Amit Ghosh, Michael Schmittel
Jan 20, 2021·Chemical Reviews·Thomas BuhseJean-Claude Micheau
Oct 13, 2021·Nature Chemistry·Mario SamperiDavid B Amabilino

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