Self-consistent Hubbard parameters or hybrid functionals are needed to predict the correct ground state of LiMnO2; standard DFT+U fails, and the failure is traced to Jahn-Teller ordering and electron localization.
HP -- A code for the calculation of Hubbard parameters using density-functional perturbation theory
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abstract
We introduce HP, an implementation of density-functional perturbation theory, designed to compute Hubbard parameters (on-site $U$ and inter-site $V$) in the framework of DFT+$U$ and DFT+$U$+$V$. The code does not require the use of computationally expensive supercells of the traditional linear-response approach; instead, unit cells are used with monochromatic perturbations that significantly reduce the computational cost of determining Hubbard parameters. HP is an open-source software distributed under the terms of the GPL as a component of Quantum ESPRESSO. As with other components, HP is optimized to run on a variety of different platforms, from laptops to massively parallel architectures, using native mathematical libraries (LAPACK and FFTW) and a hierarchy of custom parallelization layers built on top of MPI. The effectiveness of the code is showcased by computing Hubbard parameters self-consistently for the phospho-olivine Li$_x$Mn$_{1/2}$Fe$_{1/2}$PO$_4$ ($x=0, 1/2, 1$) and by highlighting the accuracy of predictions of the geometry and Li intercalation voltages.
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cond-mat.mtrl-sci 1years
2024 1verdicts
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The Interplay Between Electron Localization, Magnetic Order, and Jahn-Teller Distortion that Dictates LiMnO$_2$ Phase Stability
Self-consistent Hubbard parameters or hybrid functionals are needed to predict the correct ground state of LiMnO2; standard DFT+U fails, and the failure is traced to Jahn-Teller ordering and electron localization.