Modulation of the thermodynamic, kinetic and magnetic properties of the hydrogen monomer on graphene by charge doping

TL;DR

This study uses ab initio simulations to explore how charge doping affects the thermodynamic, kinetic, and magnetic properties of hydrogen monomers on graphene, revealing mechanisms and potential for device design.

Contribution

It provides detailed insights into how electron and hole doping modify hydrogen behavior on graphene, including diffusion barriers and magnetic properties, advancing understanding of hydrogen-graphene interactions.

Findings

Electron doping increases diffusion potential barrier.

Hole doping lowers diffusion potential barrier.

Both dopings increase desorption potential barrier.

Abstract

The thermodynamic, kinetic and magnetic properties of the hydrogen monomer on doped graphene layers were studied by ab initio simulations. Electron doping was found to heighten the diffusion potential barrier, while hole doping lowers it. However, both kinds of dopings heighten the desorption potential barrier. The underlying mechanism was revealed by investigating the effect of doping on the bond strength of graphene and on the electron transfer and the coulomb interaction between the hydrogen monomer and graphene. The kinetic properties of H and D monomers on doped graphene layers during both the annealing process (annealing time $t_0 =$300 s) and the constant-rate heating process (heating rate $\alpha =$1.0 K/s) were simulated. Both electron and hole dopings were found to generally increase the desorption temperatures of hydrogen monomers. Electron doping was found to prevent the diffusion of hydrogen monomers, while the hole doping enhances their diffusion. Macroscopic diffusion of hydrogen monomers on graphene can be achieved when the doping-hole density reaches $5.0\times10^{13}$ cm$^{-2}$. The magnetic moment and exchange splitting were found to be reduced by both electron and hole dopings, which was explained by a simple exchange model. The study in this report can further enhance the understanding of the interaction between hydrogen and graphene and is expected to be helpful in the design of hydrogenated-graphene-based devices.