Title:Competition between Spin Excitation and Kondo Correlation in Magnetic
Molecular Junctions: Theoretical Insight from First-principles-based Simulations
Volume: 2
Issue: 4
Author(s): Qingfeng Zhuang, Lyuzhou Ye and Xiao Zheng*
Affiliation:
- Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics and Synergetic
Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China,
Hefei, Anhui 230026, China
Keywords:
Magnetic molecular systems, spin excitation, kondo effect, density functional theory, complete active space selfconsistent field method, hierarchical equations of motion, scanning tunneling microscope.
Abstract: In magnetic molecular junctions, the interactions between the local spin state at the transition-
metal center and the conduction electrons from the electrodes or substrates can bring about
many interesting strong correlation effects. Spin excitation and the Kondo effect are two representative
phenomena, where the spin-unpaired d or f electrons plays the key role in forming these manybody
states. This paper reviews the recent developments and applications of several first-principles
methods in conjunction with the hierarchical equations of motion (HEOM) approach for the accurate
simulation of magnetic molecular systems. The large-scale electrodes and substrates are treated
by the density functional theory (DFT), while the properties of the magnetic center are studied by
using the high-level complete active space self-consistent field method. The competition between
the spin excitation and the Kondo effect are scrutinized by the HEOM approach. This combined
DFT+HEOM method has proven to be useful for the accurate characterization of strongly-correlated
magnetic molecular systems.
