Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials

Abstract

We present in full detail a newly developed formalism enabling density functional perturbation theory (DFPT) calculations from a DFT+$U$ ground state. The implementation includes ultrasoft pseudopotentials and is valid for both insulating and metallic systems. It aims at fully exploiting the versatility of DFPT combined with the low-cost DFT+$U$ functional. This allows to avoid computationally intensive frozen-phonon calculations when DFT+$U$ is used to eliminate the residual electronic self-interaction from approximate functionals and to capture the localization of valence electrons e.g. on $d$ or $f$ states. In this way, the effects of electronic localization (possibly due to correlations) are consistently taken into account in the calculation of specific phonon modes, Born effective charges, dielectric tensors and in quantities requiring well converged sums over many phonon frequencies, as phonon density of states and free energies. The new computational tool is applied to two representative systems, namely CoO, a prototypical transition metal monoxide and LiCoO${}_2$, a material employed for the cathode of Li-ion batteries. The results show the effectiveness of our formalism to capture in a quantitatively reliable way the vibrational properties of systems with localized valence electrons.

arXiv comment18 pages, 3 figures (Supplemental Material: 4 pages, 6 figures)

References in corpus (23)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• Pseudopotentials for high-throughput DFT calculations
• Thermal Contraction and Disordering of the Al(110) Surface
• Precision and efficiency in solid-state pseudopotential calculations
• Hubbard-corrected DFT energy functionals: the LDA+U description of correlated systems
• Implementation of the Projector Augmented Wave LDA+U Method: Application to the Electronic Structure of NiO
• Correlated metals and the LDA+U method
• Hubbard parameters from density-functional perturbation theory
• Koopmans' condition for density-functional theory
• Born Effective Charges of Barium Titanate: band by band decomposition and sensitivity to structural features
• Spectral density and metal-insulator phase transition in Mott insulators within RDMFT
• Thermoelasticity of Fe2+-bearing bridgmanite
• Optical Spectroscopy in CoO: Phonons, Electric, and Magnetic Excitations
• The role of electronic correlations on the phonon modes of MnO and NiO
• Electric fields with ultrasoft pseudo-potentials: applications to benzene and anthracene
• Origin of magnetic interactions and their influence on the structural properties of Ni2MnGa and related compounds
• Spin crossover in (Mg,Fe${}^{3+}$)(Si,Fe${}^{3+}$)O${}_3$ bridgmanite: effects of disorder, iron concentration, and temperature
• Efficient DFT+U calculations of ballistic electron transport: Application to Au monatomic chains with a CO impurity

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