Jin Soo Park

First-principles calculations of e-ph interactions are becoming a pillar of electronic structure theory. However, the current approach is incomplete. The piezoelectric (PE) e-ph interaction, a long-range scattering mechanism due to acoustic phonons in noncentrosymmetric polar materials, is not accurately described at present. Current calculations include short-range e-ph interactions (obtained by interpolation) and the dipolelike Frölich long-range coupling in polar materials, but lack important

Lattice vibrations in materials induce perturbations on the electron dynamics in the form of long-range (dipole and quadrupole) and short-range (octopole and higher) potentials. The dipole Fr\"ohlich term can be included in current first-principles electron-phonon (e-ph) calculations and is present only in polar materials. The quadrupole e-ph interaction is present in both polar and nonpolar materials, but currently it cannot be computed from first principles. Here we show an approach to compute

Electron-phonon ($e\text{\ensuremath{-}}\mathrm{ph}$) interactions are pervasive in condensed matter, governing phenomena such as transport, superconductivity, charge-density waves, polarons, and metal-insulator transitions. First-principles approaches enable accurate calculations of $e\text{\ensuremath{-}}\mathrm{ph}$ interactions in a wide range of solids. However, they remain an open challenge in correlated electron systems (CES), where density functional theory often fails to describe the gr

Scattering of carriers with ionized impurities governs charge transport in doped semiconductors. However, electron interactions with ionized impurities cannot be fully described with quantitative first-principles calculations, so their understanding relies primarily on simplified models. Here we show an ab initio approach to compute the interactions between electrons and ionized impurities or other charged defects. It includes the short- and long-range electron-defect ($e$-d) interactions on equ

We present a first-principles approach for computing the phonon-limited ${T}_{1}$ spin relaxation time due to the Elliott-Yafet mechanism. Our scheme combines fully relativistic spin-flip electron-phonon interactions with an approach to compute the effective spin of band electrons in materials with inversion symmetry. We apply our method to silicon and diamond, for which we compute the temperature dependence of the spin relaxation times and analyze the contributions to spin relaxation from diffe

Electron dynamics in external electric fields governs the behavior of solid-state electronic devices. First-principles calculations enable precise predictions of charge transport in low electric fields. However, studies of high-field electron dynamics remain elusive due to a lack of accurate and broadly applicable methods. Here, we develop an efficient approach to solve the real-time Boltzmann transport equation with both the electric field term and ab initio electron-phonon collisions. These si

Developing a microscopic understanding of spin decoherence is essential to advancing quantum technologies. Electron spin decoherence due to atomic vibrations (phonons) plays a special role as it sets an intrinsic limit to the performance of spin-based quantum devices. Two main sources of phonon-induced spin decoherence-the Elliott-Yafet and Dyakonov-Perel mechanisms-have distinct physical origins and theoretical treatments. Here, we show calculations that unify their modeling and enable accurate

First-principles calculations of electron interactions in materials have seen rapid progress in recent years, with electron-phonon (<a:math xmlns:a="http://www.w3.org/1998/Math/MathML" display="inline"><a:mrow><a:mi>e</a:mi><a:mtext>−</a:mtext><a:mrow><a:mi>ph</a:mi></a:mrow></a:mrow></a:math>) interactions being a prime example. However, these techniques use large matrices encoding the interactions on dense momentum grids, which reduces computational efficiency and obscures interpretability. Fo

Optically active spin defects in solids are promising platforms for quantum technologies. Here, we present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle used to address spin defects. Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects in the calculation of many-body electronic states and their spin-o

Understanding electronic interactions in high-temperature superconductors is an outstanding challenge. In the widely studied cuprate materials, experimental evidence points to strong electron-phonon ( <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:mi>e</a:mi> </a:math> -ph) coupling and broad photoemission spectra. Yet, the microscopic origin of this behavior is not fully understood. Here, we study <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:mi>e</b:mi> </b:math> -ph inter

Electron spin decoherence from atomic vibrations (phonons) limits the performance of spin-based devices but is difficult to model quantitatively. Here, the authors present a new theory for addressing this challenge. Their approach unifies the theoretical treatment of two mechanisms -- spin scattering off phonons and spin precession altered by phonons -- and provides unprecedented microscopic insight into spin motion in materials. This work enables precise predictions for spin relaxation and deco

Metal halide octahedra form the fundamental functional building blocks of metal halide perovskites, dictating their structures, optical properties, electronic structures, and dynamics. In this study, we show that the connectivity of bismuth halide octahedra in Cs 3 Bi 2 Br 9 and Cs 3 Bi 2 I 9 quantum dots (QDs) changes with different halide elements. We use first-principles calculations to reveal the key role of the connectivity of bismuth halide octahedra on the wave function symmetry, Huang–Rh

Electron-phonon (e-ph) interactions are pervasive in condensed matter, governing phenomena such as transport, superconductivity, charge-density waves, polarons, and metal-insulator transitions. First-principles approaches enable accurate calculations of e-ph interactions in a wide range of solids. However, they remain an open challenge in correlated electron systems (CES), where density functional theory often fails to describe the ground state. Therefore reliable e-ph calculations remain out of