The original version of this Article contained an error in Fig.2,in which the colour coding of the legend,depicting the data for‘PWPAW’and‘FE-AE’,is interchanged.This has been corrected in both the PDF and HTML ve...The original version of this Article contained an error in Fig.2,in which the colour coding of the legend,depicting the data for‘PWPAW’and‘FE-AE’,is interchanged.This has been corrected in both the PDF and HTML versions of the Article.展开更多
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 ob...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.展开更多
文摘The original version of this Article contained an error in Fig.2,in which the colour coding of the legend,depicting the data for‘PWPAW’and‘FE-AE’,is interchanged.This has been corrected in both the PDF and HTML versions of the Article.
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 developedM.O.and G.G.are grateful for the support from AFOSR FA9550-19-1-0358 under which applications to spin defects were developed+2 种基金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-AC02-06CH11357This 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.
文摘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.
