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Computing electron–defect (e–d) interactions from first principles has remained impractical due to computational cost. Here we develop an interpolation scheme based on maximally localized Wannier functions (WFs) to efficiently computee–d interaction matrix elements. The interpolated matrix elements can accurately reproduce those computed directly without interpolation and the approach can significantly speed up calculations ofe–d relaxation times and defect-limited charge transport. We show example calculations of neutral vacancy defects in silicon and copper, for which we compute thee–d relaxation times on fine uniform and random Brillouin zone grids (and for copper, directly on the Fermi surface), as well as the defect-limited resistivity at low temperature. Our interpolation approach opens doors for atomistic calculations of charge carrier dynamics in the presence of defects.

 

Exact simulations of quantum circuits (QCs) are currently limited to ~50 qubits because the memory and computational cost required to store the QC wave function scale exponentially with qubit number. Therefore, developing efficient schemes for approximate QC simulations is a current research focus. Here we show simulations of QCs with a method inspired by density functional theory (DFT), a widely used approach to study many-electron systems. Our calculations can predict marginal single-qubit probabilities (SQPs) with over 90% accuracy in several classes of QCs with universal gate sets, using memory and computational resources linear in qubit number despite the formal exponential cost of the SQPs. This is achieved by developing a mean-field description of QCs and formulating optimal single- and two-qubit gate functionals – analogs of exchange-correlation functionals in DFT – to evolve the SQPs without computing the QC wave function. Current limitations and future extensions of this formalism are discussed. 

Abstract Charge transport in organic molecular crystals (OMCs) is conventionally categorized into two limiting regimes − band transport, characterized by weak electron-phonon (e-ph) interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles approach that can accurately predict the carrier mobility in this intermediate regime and shed light on its microscopic origin. Our approach combines a finite-temperature cumulant method to describe strong e-ph interactions with Green-Kubo transport calculations. We apply this parameter-free framework to naphthalene crystal, demonstrating electron mobility predictions within a factor of 1.5−2 of experiment between 100 and 300 K. Our analysis reveals the formation of a broad polaron satellite peak in the electron spectral function and the failure of the Boltzmann equation in the intermediate regime.