Heisenberg exchange enhancement by orbital relaxation in cuprate compounds

Physics – Condensed Matter – Strongly Correlated Electrons

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We calculate the Heisenberg exchange J in the quasi-2D antiferromagnetic cuprates La2CuO4, YBa2Cu3O6, Nd2CuO4 and Sr2CuO2Cl2. We apply all-electron (MC)SCF and non-orthogonal CI calculations to [Cu2O11]18-, [Cu2O9]14-, [Cu2O7]10- and [Cu2O7Cl4]14- clusters in a model charge embedding. The (MC)SCF triplet and singlet ground states are well characterized by Cu2+ (dx2-y2) and O2-. The antiferromagnetic exchange is strongly enhanced by admixing relaxed (MC)SCF triplet and singlet excited states, in which a single electron is transferred from the central O ion to Cu. We ascribe this effect to orbital relaxation in the charge transfer component of the wave function. Close agreement with experiment is obtained.

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