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Issue 23, 2019
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Controlling the preferential motion of chiral molecular walkers on a surface

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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 foot. As a result, the molecule diffuses via a two-step mechanism, and due to its inherent asymmetry, the corresponding PES is also spatially asymmetric. Taking advantage of this fact, we show how the external stimulus can be tuned to separate molecules of different chirality, orientation and conformation. The consequences of these findings for molecular machines and the separation of enantiomers are also discussed.

Graphical abstract: Controlling the preferential motion of chiral molecular walkers on a surface

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Publication details

The article was received on 07 Mar 2019, accepted on 08 May 2019 and first published on 14 May 2019


Article type: Edge Article
DOI: 10.1039/C9SC01135H
Chem. Sci., 2019,10, 5864-5874
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    Controlling the preferential motion of chiral molecular walkers on a surface

    D. Abbasi-Pérez, H. Sang, L. Pérez-García, A. Floris, D. B. Amabilino, R. Raval, J. M. Recio and L. Kantorovich, Chem. Sci., 2019, 10, 5864
    DOI: 10.1039/C9SC01135H

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