Many-body renormalisation of forces in f-electron materials

Abstract

We present the implementation of Dynamical Mean-Field Theory (DMFT) in the CASTEP \emph{ab-initio} code. We explain in detail the theoretical framework for DFT+DMFT and we demonstrate our implementation for three strongly-correlated systems with $f$-shell electrons: $\gamma$-cerium, cerium sesquioxide Ce${}_2$O${}_3$ and samarium telluride SmTe by using a Hubbard I solver. We find very good agreement with previous benchmark DFT+DMFT calculations of cerium compounds, while for SmTe, which was never studied within DFT+DMFT before to the best of our knowledge, we show the improved agreement with the experimental structural parameters as compared with LDA. Our implementation works equally well for both norm-conserving and ultra-soft pseudopotentials, and we apply it to the calculation of total energy, bulk modulus, equilibrium volumes and internal forces in the two cerium compounds. In Ce${}_2$O${}_3$ we report a dramatic reduction of the internal forces acting on coordinates not constrained by unit cell symmetries. This reduction is induced by the many-body effects, which can only be captured at the DMFT level. In addition, we derive an alternative form for treating the high-frequency tails of the Green function in Matsubara frequency summations. Our treatment allows a reduction in the bias when calculating the correlation energies and occupation matrices to high precision.

11 pages, 7 figures, CASTEP DMFT reference paper

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Cited by in corpus (14)

• Cerium Oxides without $U$: The Role of Many-Electron Correlation
• The Wannier Function Software Ecosystem for Materials Simulations
• Charge self-consistent electronic structure calculations with dynamical mean-field theory using Quantum ESPRESSO, Wannier90 and TRIQS
• Calculating DMFT forces in ab-initio ultrasoft pseudopotential formalism
• Compound-tunable embedding potential method and its application to fersmite crystal
• Isoelectronic tuning of heavy fermion systems: Proposal to synthesize Ce3Sb4Pd3
• A novel continuous time quantum Monte Carlo solver for dynamical mean field theory in the compact Legendre representation
• Dynamical Mean-Field Theory for spin-dependent electron transport in spin-valve devices
• Impact of electronic correlations on the superconductivity of high-pressure CeH${}_9$
• Pressure induced electronic transitions in Samarium monochalcogenides
• Exploring the exotic f states of prototype compounds CeSb and USb
• Phase transitions of correlated systems from graph neural networks with quantum embedding techniques
• Correlation-driven phonon renormalisation and the equation of state of $\gamma$-cerium
• Correlation-driven origin of shallow electron pocket in Co${}_{1/3}$TaS${}_2$ revealed by ARPES and cluster perturbation theory