Wannier90 as a community code: new features and applications

Wannier90 is an open-source computer program for calculating maximally-localised Wannier functions (MLWFs) from a set of Bloch states. It is interfaced to many widely used electronic-structure codes thanks to its independence from the basis sets representing these Bloch states. In the past few years the development of Wannier90 has transitioned to a community-driven model; this has resulted in a number of new developments that have been recently released in Wannier90 v3.0. In this article we describe these new functionalities, that include the implementation of new features for wannierisation and disentanglement (symmetry-adapted Wannier functions, selectively-localised Wannier functions, selected columns of the density matrix) and the ability to calculate new properties (shift currents and Berry-curvature dipole, and a new interface to many-body perturbation theory); performance improvements, including parallelisation of the core code; enhancements in functionality (support for spinor-valued Wannier functions, more accurate methods to interpolate quantities in the Brillouin zone); improved usability (improved plotting routines, integration with high-throughput automation frameworks), as well as the implementation of modern software engineering practices (unit testing, continuous integration, and automatic source-code documentation). These new features, capabilities, and code development model aim to further sustain and expand the community uptake and range of applicability, that nowadays spans complex and accurate dielectric, electronic, magnetic, optical, topological and transport properties of materials.

Spectral properties of extended systems from Koopmans-compliant functionals

Riccardo De Gennaro

Electronic-structure simulations have been impacting the study of materials properties thanks to the simplicity of density-functional theory, a method that gives access to the ground state of the system. Although very important, ground-state properties represent just part of the information, and often technological applications rely more on excited-state properties. In the context of density-functional theory, the latter are difficult to extract and one usually has to resort to more sophisticated approaches. In the last years, Koopmans spectral functionals have emerged as an effective method which combines the feasibility of density-functional theory with the accuracy of more complex methods, such as many-body perturbation theory. While retaining its simplicity, Koopmans functionals extend the domain of density-functional theory providing direct access to charged excitations, and ultimately to the photoemission spectra of materials. This approach has been extensively employed in finite systems, displaying an accuracy which is comparable to that of state-of-the-art many-body perturbation theory methods. In extended systems, calculations were bound to the supercell (Gamma-only) method, preventing the access to the full band structure of the system. In this work we overcome this limitation, proving that a band structure description of the energy spectrum is possible, and providing a scheme to carry out calculations in crystalline materials. The first result of this work consists in proving the compliance of Koopmans functionals with the translation symmetry of the system. The validity of Bloch's theorem, thus the possibility of describing the spectrum via a band structure picture, depends on this condition. Because of the orbital-density-dependent nature of the functional, the invariance of the total energy with respect to unitary transformations of the one-electron orbitals is broken. The energy is then minimized by a particular set of orbitals, called ``variational'', which are strongly localized in space. In extended periodic systems, the localized, thus non-periodic, character of the variational orbitals is inherited by the effective orbital-density-dependent Hamiltonians, which apparently break the translation symmetry of the system. Here we show that, by requiring the variational orbitals to be Wannier functions, the translation symmetry is preserved and Bloch's theorem holds. In the second part, we devise a scheme to unfold the band structure from supercell (Gamma-only) calculations, and reconstruct the k-dependence of the quasiparticle energies. This method is then used to compute the band structures of a set of benchmark semiconductors and insulators. Finally, we describe a novel formulation of Koopmans functionals for extended periodic systems, which exploits from the beginning the translation properties of Wannier functions to realize a primitive cell-based implementation of Koopmans functionals. Results obtained from this second approach are also discussed. In the last part, we present the preliminary study of impurity states arising in crystalline materials in the presence of point defects.

EPFL2022

Spectral properties of extended systems from Koopmans-compliant functionals

Riccardo De Gennaro

EPFL2022