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Antiferromagnetic band structure of La_2CuO_4: Becke-3–Lee-Yang-Parr calculations

Perry, Jason K. and Tahir-Kheli, Jamil and Goddard, William A., III (2001) Antiferromagnetic band structure of La_2CuO_4: Becke-3–Lee-Yang-Parr calculations. Physical Review B, 63 (14). Art. No. 144510. ISSN 0163-1829. doi:10.1103/physrevb.63.144510.

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Using the Becke-3–Lee-Yang-Parr (B3LYP) functional, we have performed band-structure calculations on the high-temperature superconductor parent compound, La_2CuO_4. Under the restricted spin formalism (ρ_↑ = ρ_↓), B3LYP band structure agrees well with the standard local-density approximation (LDA) band structure. It is metallic with a single Cu_(x^2 − y^2)/Op_σ band crossing the Fermi level. Under the unrestricted spin formalism (ρ_↑ ≠ ρ_↓), the B3LYP band structure has a spin-polarized antiferromagnetic solution with a band gap of 2.0 eV, agreeing well with experiment. This state is 0.52 eV (per formula unit) lower than that calculated under the restricted spin formalism. The apparent high energy of the spin-restricted state is attributed to an overestimate of on-site Coulomb repulsion, which is corrected in the unrestricted spin calculations. The stabilization of the total energy with spin polarization arises primarily from the stabilization of the x^2 − y^2 band, such that the character of the eigenstates at the top of the valence band in the antiferromagnetic state becomes a strong mixture of Cu_(x^2 − y^2)/Op_σ and Cu_(z^2)/O′p_z. Since the Hohenberg-Kohn theorem requires the spin-restricted and spin-unrestricted calculations to give identical ground-state energies and total spatial densities for the exact functionals, this large disparity in energy reflects the inadequacy of current functionals for describing the cuprates. This calls into question the use of band structures based on current restricted spin-density functionals (including LDA) as a basis for single-band theories of superconductivity in these materials.

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Goddard, William A., III0000-0003-0097-5716
Alternate Title:Antiferromagnetic band structure of La2CuO4: Becke-3–Lee-Yang-Parr calculations, The Antiferromagnetic Band Structure of La2CuO4 Revisited
Additional Information:© 2001 American Physical Society. (Received 7 July 2000; revised manuscript received 12 December 2000; published 19 March 2001) We wish to acknowledge helpful discussions with Dr. Francesco Faglioni and Dr. Eugene Heifets. This work was partially supported by the Materials and Process Simulation Center (MSC) at Caltech, which is supported by grants from DOE-ASCI, ARO/DURIP, ARO/MURI, 3M, Beckman Institute, Seiko-Epson, Dow, Avery-Dennison, Kellogg, and Asahi Chemical.
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Department of Energy (DOE)UNSPECIFIED
Army Research Office (ARO)UNSPECIFIED
Caltech Beckman InstituteUNSPECIFIED
Dow Chemical CompanyUNSPECIFIED
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Issue or Number:14
Classification Code:PACS number(s): 74.25.Jb, 71.15.Mb
Record Number:CaltechAUTHORS:20190626-121728673
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:96740
Deposited By: George Porter
Deposited On:26 Jun 2019 20:51
Last Modified:16 Nov 2021 17:23

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