Charge Transfer and Chemisorption of Fullerene Molecules on Metal Surfaces: Application to Dynamics of Nanocars

Abstract

It is widely believed that the dynamics of surface-bound fullerene molecules is not fully understood because current theoretical analyses do not include chargetransfer phenomena. A new theoretical approach to describe charge transfer and chemisorption processes for fullerenes on gold surfaces has been developed. The method is based on extensive semiempirical calculations that provide a consistent description of charge transfer and adsorption phenomena. Our theoretical approach is applied for analyzing complex dynamics of fullerene-based molecular machines, known as nanocars. It is found that the charge transfer makes the rolling of nanocars' wheels a preferable mode for translational motion because of the complex interactions with the metal surfaces. The physicalchemical aspects of the rolling mechanism are discussed.

Charge transfer dynamics at the boron subphthalocyanine chloride/C60 interface: non-adiabatic dynamics study with Libra-X

“…The UFF has been used to investigate several molecules, including C 60 and other systems. [116][117][118][119][120][121][122][123][124] Although the UFF is often considered a generic but lowaccuracy force field, 125,126 it is useful for our purposes, because it can help to highlight the qualitative changes in electronic dynamics that are induced by changes in the internuclear interaction potentials.…”

Unidirectional Rolling Motion of Nanocars Induced by Electric Field

“…Instead, our charge transfer/chemisorption model uses the method of image charges as described in details in our earlier work. 39 The polarized C 60 group is then able to interact with the field according to classical electrostatics laws.…”

“…Recently, we proposed a new theoretical method for taking into account the charge transfer processes on the interface between C 60 /nanocar molecules and gold metal. 39 The model predicts the dynamical charge redistribution on atoms in the C 60 wheels of the nanocar, which depends on their orientation with respect to the metal surface. As a consequence, the dipole moment of the system is not zero.…”

Libra: An open-Source “methodology discovery” library for quantum and classical dynamics simulations

“…The presently implemented force fields include UFF, [59] DREIDING, [60] GAFF, [61] TRIPOS, [62] MMFF94, [63,64] as well as few other diverse setups. [65][66][67][68] The partial charges can be set manually, computed by the quantum-mechanical methods, including those already implemented in Libra (interface would need to be specified), or can be computed using the charge equilibration (QEq) scheme of Rappe and Goddard. [29] The electrostatic interactions in periodic systems are computed using the 3D Ewald summation scheme implemented according to Karasawa and Goddard.…”