Electronic properties of transition metal atoms on Cu${}_2$N/Cu(100)

Abstract

We study the nature of spin excitations of individual transition metal atoms (Ti, V, Cr, Mn, Fe, Co and Ni) deposited on a Cu${}_2$N/Cu(100) surface using both spin-polarized density functional theory (DFT) and exact diagonalization of an Anderson model derived from DFT. We use DFT to compare the structural, electronic and magnetic properties of different transition metal adatoms on the surface. We find that the average occupation of the transition metal d shell, main contributor to the magnetic moment, is not quantized, in contrast with the quantized spin in the model Hamiltonians that successfully describe spin excitations in this system. In order to reconcile these two pictures, we build a multi-orbital Anderson Hamiltonian for the d shell of the transition metal hybridized with the p orbitals of the adjacent Nitrogen atoms, by means of maximally localized Wannier function representation of the DFT Hamiltonian. The exact solutions of this model have quantized total spin, without quantized charge at the d shell. We propose that the quantized spin of the models actually belongs to many-body states with two different charge configurations in the d shell, hybridized with the p orbital of the adjacent Nitrogen atoms. This scenario implies that the measured spin excitations are not fully localized at the transition metal.

12 pages, 14 figures, regular article

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Cited by in corpus (13)

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• Renormalization of single-ion magnetic anisotropy in the absence of Kondo effect
• Efficient Ab-initio Multiplet Calculations for Magnetic Adatoms on MgO
• Complete reversal of the atomic unquenched orbital moment by a single electron
• Competition between quantum spin tunneling and Kondo effect
• Electronic and Magnetic Properties of single Fe atoms on a CuN Surface; Effects of Electron Correlations
• Large effect of the metal substrate on the magnetic anisotropy of Co on hexagonal Boron Nitride
• Magnetic properties of the finite-length biatomic chains in the framework of the single domain-wall approximation
• Microscopic theory of spin-relaxation of a single Fe adatom coupled to substrate vibrations
• Optimizing tip-surface interactions in ESR-STM experiments
• First-principles study of electronic and magnetic properties of Fe atoms on Cu2N/Cu(100)