Quantum Monte Carlo calculations of H₂ dissociation on Si(001)

الأصل · EN

We present quantum Monte Carlo calculations for various reaction pathways of H₂ with Si(001), using large model clusters of the surface. We obtain reaction energies and energy barriers noticeably higher than those from approximate exchange-correlation functionals. In improvement over previous studies, our adsorption barriers closely agree with experimental data. For desorption, the calculations give barriers for conventional pathways in excess of the presently accepted experimental value, and pinpoint the role of coverage effects and desorption from steps.