Spin–spin interactions in defects in solids from mixed all-electron and pseudopotential first-principles calculations  

作　　者：Krishnendu Ghosh He Ma Mykyta Onizhuk Vikram Gavini Giulia Galli 

机构地区：[1]Department of Mechanical Engineering,University of Michigan,Ann Arbor,MI,USA [2]Pritzker School of Molecular Engineering,University of Chicago,Chicago,IL,USA [3]Department of Chemistry,University of Chicago,Chicago,IL,USA [4]Department of Materials Science and Engineering,University of Michigan,Ann Arbor,MI,USA [5]Materials Science Division,Argonne National Laboratory,Lemont,IL,USA

出　　处：《npj Computational Materials》2021年第1期1108-1115,共8页计算材料学（英文）

基　　金：K.G.and V.G.are grateful for the support of the Department of Energy,Office of Basic Energy Science,through grant number DE-SC0017380,under the auspices of which the computational framework for FE based AE DFT calculations was developed;M.O.and G.G.are grateful for the support from AFOSR FA9550-19-1-0358 under which applications to spin defects were developed;H.M.and G.G.are grateful for the support from MICCoM,under which code development was supported.MICCoM is part of the Computational Materials Sciences Program funded by the U.S.Department of Energy,Office of Science,Basic Energy Sciences,Materials Sciences and Engineering Division through Argonne National Laboratory,under contract number DE-AC02-06CH11357;This work used computational resources from the University of Michigan through the Greatlakes computing platform,resources from the Research Computing Center at the University of Chicago through UChicago MRSEC(NSF DMR-1420709);resources of the National Energy Research Scientific Computing Center(NERSC),a U.S.Department of Energy Office of Science User Facility operated under Contract No.DE-AC02-05CH11231.

摘　　要：Understanding the quantum dynamics of spin defects and their coherence properties requires an accurate modeling of spinspin interaction in solids and molecules,for example by using spin Hamiltonians with parameters obtained from first principles calculations.We present a real-space approach based on density functional theory for the calculation of spin-Hamiltonian parameters,where only selected atoms are treated at the all-electron level,while the rest of the system is described with the pseudopotential approximation.Our approach permits calculations for systems containing more than 1000 atoms,as demonstrated for defects in diamond and silicon carbide.We show that only a small number of atoms surrounding the defect needs to be treated at the all-electron level,in order to obtain an overall all-electron accuracy for hyperfine and zero-field splitting tensors.We also present results for coherence times,computed with the cluster correlation expansion method,highlighting the importance of accurate spin-Hamiltonian parameters for quantitative predictions of spin dynamics.

关 键 词：dynamics SOLIDS HAMILTONIAN 

分 类 号：O562[理学—原子与分子物理]