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 electronicstructure 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, selectivelylocalised 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 arXiv:1907.09788v1 [cond-mat.mtrl-sci]

Hot carriers (HC) generated by surface plasmon polaritons (SPPs) in noble metals are promising for application in optoelectronics, plasmonics and renewable energy. However, existing models fail to explain key quantitative details of SPP-to-HC conversion experiments. Here we develop a quantum mechanical framework and apply first-principles calculations to study the energy distribution and scattering processes of HCs generated by SPPs in Au and Ag. We find that the relative positions of the s and d bands of noble metals regulate the energy distribution and mean free path of the HCs, and that the electron–phonon interaction controls HC energy loss and transport. Our results prescribe optimal conditions for HC generation and extraction, and invalidate previously employed free-electron-like models. Our work combines density functional theory, GW and electron–phonon calculations to provide microscopic insight into HC generation and ultrafast dynamics in noble metals.

Relaxation times employed to study electron transport in metals are typically taken to be constants and obtained empirically. Here, we use fully ab initio calculations to compute the electron-phonon relaxation times of Cu, Ag, and Au and find that they vary significantly on the Fermi surface, with values from ∼15 to 45 fs that are correlated with the Fermi surface topology. We compute room-temperature resistivities in excellent agreement with experiment by combining GW quasiparticle band structures, Wannier-interpolated band velocities, and ab initio relaxation times. We introduce an importance sampling scheme to speed up the convergence of resistivity and transport calculations. DOI: 10.1103/PhysRevB.94.155105 Copper, silver, and gold are noble metals with broad application in electronics, power generation, catalysis, and plasmonics. They have attracted interest since the early days of solid state theory, as their electronic structure deviates from the free-electron model that applies to the alkali metals. The Fermi surface (FS) of noble metals is not spherical as in free-electron theory but is deformed due to the proximity of the d bands to the free-electron-like sp band [1][2][3][4]. Electron scattering processes at the FS are of particular relevance for noble metal applications, as they regulate charge and heat transport [5,6]. At room temperature in relatively pure metals, scattering with phonons [7,8] is dominant, while scattering with defects and impurities is important at low temperatures and in alloys or samples of low purity.Transport in metals can be understood heuristically with the Drude theory [9], which assumes free electrons with a constant (that is, band-and k-independent) relaxation time (RT). Even in noble metals, where important deviations are expected from the Drude theory, resistive losses and optical experiments are routinely interpreted using constant relaxation times [9][10][11]. More advanced models, such as state-of-theart ab initio calculations of resistivity and other transport properties [12,13], typically employ density functional theory (DFT) band structures combined with constant RTs inferred from experiment or estimated heuristically.However, the RT of an electron in a Bloch state depends, in general, on the band and crystal momentum k, a point that has so far been often neglected. Accurate calculations of electron RTs are computationally costly, as they require fine Brillouin zone (BZ) sampling [14][15][16], prompting adoption of simplified schemes that employ either a constant RT [17] or an average scattering strength [18]. An exception are recent transport calculations in Al [19] and two-dimensional materials [19][20][21] that included the band and k dependence of the RTs.As striking new experimental findings on noble metals emerge [22][23][24], predictive theories are needed to study electron scattering in these materials. For example, recent * sglouie@berkeley.edu experiments by Kim et al. [22] show a remarkable resistivity drop when a single crystal of Ag is doped wit...