Shayantan Chaudhuri, University of Warwick
Recent experiments have shown that electrodeposition can lead to the creation of stable small nanoclusters and even single gold adatoms on polycrystalline boron-doped diamond (BDD) surfaces. Here, we used hybrid quantum mechanics/molecular mechanics (QM/MM) to investigate the stability of single gold atoms on these BDD surfaces to aid material design. Py-ChemShell was crucial for the work, allowing us to develop embedded-cluster models that facilitated studies of the adsorption of single metal atoms on oxygen-terminated diamond (110) surfaces with expensive hybrid-DFT methods. We built models of surface oxygen vacancies and charged boron substitution defects, and compared different density-functional approximations to predict the adsorption structure, energy, and the barrier for diffusion on pristine and defective surfaces. The results show that thermally stable deposition of individual gold atoms on BDD requires the presence of surface vacancies or charged substitutional defects, which will be crucial knowledge in the further development of these materials.
S. Chaudhuri, A. J. Logsdail and R. J. Maurer (2023) “Stability of Single Gold Atoms on Defective and Doped Diamond Surfaces”, J. Phys. Chem. C, 127, 16187–16203. DOI: 10.1021/acs.jpcc.3c03900