The importance of anisotropic Coulomb interaction in LaMnO${}_3$

Abstract

In low-temperature anti-ferromagnetic LaMnO${}_3$, strong and localized electronic interactions among Mn 3d electrons prevent a satisfactory description from standard local density and generalized gradient approximations in density functional theory calculations. Here we show that the strong on-site electronic interactions are described well only by using direct and exchange corrections to the intra-orbital Coulomb potential. Only DFT+U calculations with explicit exchange corrections produce a balanced picture of electronic, magnetic and structural observables in agreement with experiment. To understand the reason, a rewriting of the functional form of the +U corrections is presented that leads to a more physical and transparent understanding of the effect of these correction terms. The approach highlights the importance of Hund's coupling (intra-orbital exchange) in providing anisotropy across the occupation and energy eigenvalues of the Mn d states. This intra-orbital exchange is the key to fully activating the Jahn-Teller distortion, reproducing the experimental band gap and stabilizing the correct magnetic ground state in LaMnO${}_3$. The best parameter values for LaMnO${}_3$ within the DFT (PBEsol) +U framework are determined to be U = 8 eV and J = 1.9 eV.

Figures 7 and 8 revised. Minor revisions throughout the Results Sections. Table IV revised, Table VI new

References in corpus (6)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Strong electronic correlations from Hund's coupling
• Screened hybrid functional applied to 3d^0-->3d^8 transition-metal perovskites LaMO3 (M=Sc-Cu): influence of the exchange mixing parameter on the structural, electronic and magnetic properties
• First-Principles Studies of the Atomic, Electronic, and Magnetic Structure of a-MnO2 (Cryptomelane)
• The importance of anisotropic Coulomb interactions and exchange to the band gap and antiferromagnetism of β-MnO2 from DFT+U

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