We present an overview of the ONETEP program for linear-scaling density functional theory (DFT) calculations with large basis set (planewave) accuracy on parallel computers. The DFT energy is computed from the density matrix, which is constructed from spatially localized orbitals we call Non-orthogonal Generalized Wannier Functions (NGWFs), expressed in terms of periodic sinc (psinc) functions. During the calculation, both the density matrix and the NGWFs are optimized with localization constraints. By taking advantage of localization, ONETEP is able to perform calculations including thousands of atoms with computational effort, which scales linearly with the number or atoms. The code has a large and diverse range of capabilities, explored in this paper, including different boundary conditions, various exchangecorrelation functionals (with and without exact exchange), finite electronic temperature methods for metallic systems, methods for strongly correlated systems, molecular dynamics, vibrational calculations, time-dependent DFT, electronic transport, core loss spectroscopy, implicit solvation, quantum mechanical (QM)/molecular mechanical and QM-in-QM embedding, density of states calculations, distributed multipole analysis, and methods for partitioning charges and interactions between fragments. Calculations with ONETEP provide unique insights into large and complex systems that require an accurate atomic-level description, ranging from biomolecular to chemical, to materials, and to physical problems, as we show with a small selection of illustrative examples. ONETEP has always aimed to be at the cutting edge of method and software developments, and it serves as a platform for developing new methods of electronic structure simulation. We therefore conclude by describing some of the challenges and directions for its future developments and applications.

Strain is a powerful experimental tool to explore new electronic states and understand unconventional superconductivity. Here, we investigate the effect of uniaxial strain on the nematic and superconducting phase of single crystal FeSe using magnetotransport measurements. We find that the resistivity response to the strain is strongly temperature dependent and it correlates with the sign change in the Hall coefficient being driven by scattering, coupling with the lattice and multiband phenomena. Band-structure calculations suggest that under strain the electron pockets develop a large in-plane anisotropy as compared with the hole pocket. Magnetotransport studies at low temperatures indicate that the mobility of the dominant carriers increases with tensile strain. Close to the critical temperature, all resistivity curves at constant strain cross in a single point, indicating a universal critical exponent linked to a strain-induced phase transition. Our results indicate that the superconducting state is enhanced under compressive strain and suppressed under tensile strain, in agreement with the trends observed in FeSe thin films and overdoped pnictides, whereas the nematic phase seems to be affected in the opposite way by the uniaxial strain. By comparing the enhanced superconductivity under strain of different systems, our results suggest that strain on its own cannot account for the enhanced high T c superconductivity of FeSe systems.

We demonstrate the capability of embedded mean eld theory (EMFT) within the linear-scaling density-functional theory code onetep, which enables DFT-in-DFT quantum embedding calculations on systems containing thousands of atoms at a fraction of the cost of a full calculation. We perform simulations on a wide range of systems from molecules to complex nanostructures to demonstrate the performance of our implementation with respect to accuracy and eciency. This work paves the way for the application of this class of quantum embedding method to large-scale systems that are beyond the reach of existing implementations.Another option is to enforce orthogonality manually to avoid the non-additive term ever appearing: this can be done either by construction, 37 or by projecting out the environment orbitals.3840 Each of these options has its own strengths and weaknesses, and some are more suitable than others for a given situation.Recently, another quantum embedding method that avoids these issues has been pro-