Fully Anharmonic, Non-Perturbative Theory of Vibronically Renormalized Electronic Band Structures

Abstract

We develop a first-principles approach for the treatment of vibronic interactions in solids that overcomes the main limitations of state-of-the-art electron-phonon coupling formalisms. In particular, anharmonic effects in the nuclear dynamics are accounted to all orders via ab initio molecular dynamics simulations. This non-perturbative, self-consistent approach evaluates the response of the wave functions along the computed anharmonic trajectory; thus it fully considers the coupling between nuclear and electronic degrees of freedom. We validate and demonstrate the merits of the concept by calculating temperature-dependent, momentum-resolved spectral functions for silicon and the cubic perovskite SrTiO3, a strongly anharmonic material featuring soft modes. In the latter case, our approach reveals that anharmonicity and higher-order vibronic couplings contribute substantially to the electronic-structure at finite-temperatures, noticeably affecting band gaps and effective masses, and hence macroscopic properties such as transport coefficients.

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• Accurate and efficient band-gap predictions for metal halide perovskites at finite temperature
• Zero-point Renormalization of the Band Gap of Semiconductors and Insulators Using the PAW Method
• Mass enhancement in 3d and s-p perovskites from symmetry breaking
• A machine learning route between band mapping and band structure
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Dynamical renormalization of electron-phonon coupling in conventional superconductors
• Wannier Function Perturbation Theory: Localized Representation and Interpolation of Wavefunction Perturbation
• Quantum Confinement of Electron-Phonon Coupling in Graphene Quantum Dots
• Tight-binding description of inorganic lead halide perovskites in cubic phase
• Zero-point lattice expansion and band gap renormalization: Grüneisen approach versus free energy minimization
• Verification and Validation of zero-point electron-phonon renormalization of the bandgap, mass enhancement, and spectral functions
• Electronic structure and optical properties of quantum crystals from first principles calculations in the Born-Oppenheimer approximation
• Non-perturbative Green's function method to determine the electronic spectral function due to electron-phonon interactions: Application to a graphene model from weak to strong coupling
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• Coexistence of Superconductivity and Superionicity in Li${}_2$MgH${}_{16}$
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• Strain Effects on Auger-Meitner Recombination in Silicon
• Tuning Thermal Conductivity and Electron-Phonon Interactions in Carbon and Boron Nitride Moiré Diamanes via Twist Angle Manipulation