Ab initio calculations of the electronic structure of cuprates using large scale cluster techniques

TL;DR

This paper uses large-scale ab initio cluster calculations to analyze the electronic structures of various cuprates, providing detailed insights into their magnetic, electric, and orbital properties, with results aligning well with experimental data.

Contribution

It introduces a comprehensive ab initio cluster approach for cuprates, enabling detailed analysis of electronic, magnetic, and orbital properties across multiple compounds.

Findings

Good agreement with experimental magnetic hyperfine fields

Detailed orbital occupation and electric field gradient data

Insights into doping effects on electronic structure

Abstract

The local electronic structures of La2CuO4, three members of the Yttrium-family (YBa2Cu3O6, YBa2Cu3O7, and YBa2Cu4O8), and to some extent of Nd2CuO4 have been determined using all-electron ab-initio cluster calculations for clusters comprising up to thirteen planar copper atoms associated with their nearest planar and apical oxygen atoms. Spin-polarized calculations in the framework of density functional theory have enabled an estimation of the superexchange couplings J. Electric field gradients at the planar copper sites are determined and their dependence on the occupation of the various atomic orbitals are investigated in detail. The changes of the electronic field gradient and of the occupation of orbitals upon doping are studied and discussed. Furthermore, magnetic hyperfine fields are evaluated and disentangled into on-site and transferred contributions, and the chemical shifts at the copper nucleus are calculated. In general the results are in good agreement with values deduced from experiments except for the value of the chemical shift with applied field perpendicular to the CuO2-plane.