The Stability, Energetics, and Magnetic States of Cobalt Adatoms on Graphene

Abstract

We investigate the stability and electronic properties of single Co atoms on graphene with near-exact many-body calculations. A frozen-orbital embedding scheme was combined with auxiliary-field quantum Monte Carlo to increase the reach in system sizes. Several energy minima are found as a function of the distance $h$ between Co and graphene. Energetics only permit the Co atom to occupy the top site at $h=2.2$ Å in a high-spin $3d^{8}4s^1$ state, and the van der Waals region at $h=3.3$ Å in a high-spin $3d^{7}4s^2$ state. The findings provide an explanation for recent experimental results with Co on free-standing graphene.

5 pages, 3 figures

References in corpus (13)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• The electronic properties of graphene
• Emergence of magnetism in graphene materials and nanostructures
• Adatoms and clusters of 3d transition metals on graphene: Electronic and magnetic configurations
• van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions
• Auxiliary-field quantum Monte Carlo calculations of molecular systems with a Gaussian basis
• Orbital selective and tunable Kondo effect of magnetic adatoms on graphene: Correlated electronic structure calculations
• Adsorption of cobalt on graphene: Electron correlation effects from a quantum chemical perspective
• Bond breaking with auxiliary-field quantum Monte Carlo
• Eliminating spin contamination in auxiliary-field quantum Monte Carlo: realistic potential energy curve of F2
• Ab Initio Many-body Study of Cobalt Adatoms Adsorbed on Graphene
• Single 3$d$ transition metal atoms on multi-layer graphene systems: electronic configurations, bonding mechanisms and role of the substrate
• Auxiliary-field quantum Monte Carlo study of first- and second-row post-d elements

Cited by in corpus (11)

• On Achieving High Accuracy in Quantum Chemical Calculations of 3d Transition Metal Systems: A Comparison of Auxiliary-Field Quantum Monte Carlo with Coupled Cluster, Density Functional Theory, and Experiment for Diatomic Molecules
• Some Recent Developments in Auxiliary-Field Quantum Monte Carlo for Real Materials
• Quantum embedding methods for correlated excited states of point defects: Case studies and challenges
• An Auxiliary-Field Quantum Monte Carlo Study of the Chromium Dimer
• Computation of ground-state properties in molecular systems: back-propagation with auxiliary-field quantum Monte Carlo
• Electronic structure and magnetism of samarium and neodymium adatoms on free-standing graphene
• Local embedding and effective downfolding in the auxiliary-field quantum Monte Carlo method
• Error Cancellation in Diffusion Monte Carlo Calculations of Surface Chemistry
• Current-induced one-dimensional diffusion of Co ad-atoms on graphene nanoribbons
• Phase diagram of a pseudogap Anderson model with application to graphene
• Fundamental properties of transition-metals-adsorbed graphene