Excited-state Forces within a First-principles Green's Function Formalism

Abstract

We present a new first-principles formalism for calculating forces for optically excited electronic states using the interacting Green's function approach with the GW-Bethe Salpeter Equation method. This advance allows for efficient computation of gradients of the excited-state Born-Oppenheimer energy, allowing for the study of relaxation, molecular dynamics, and photoluminescence of excited states. The approach is tested on photoexcited carbon dioxide and ammonia molecules, and the calculations accurately describe the excitation energies and photoinduced structural deformations.

2 figures and 2 tables

Cited by in corpus (26)

• Optical excitations in organic molecules, clusters and defects studied by first-principles Green's function methods
• The Bethe-Salpeter Equation Formalism: From Physics to Chemistry
• Quasi-Particle Self-Consistent $GW$ for Molecules
• Neutral and charged excitations in carbon fullerenes from first-principles many-body theories
• Tight binding analysis of Si and GaAs ultra thin bodies with subatomic resolution
• Excited-state relaxations and Franck-Condon shift in Si quantum dots
• Topological phonons in oxide perovskites controlled by light
• Ab Initio Calculations of Exciton Radiative Lifetimes in Bulk Crystals, Nanostructures and Molecules
• Transferable tight binding model for strained group IV and III-V materials and heterostructures
• Sub-picosecond photo-induced displacive phase transition in two-dimensional MoTe${}_2$
• Unified theory of electron-phonon renormalization and phonon-assisted optical absorption
• Excitonic polarons and self-trapped excitons from first-principles exciton-phonon couplings
• Exploring approximations to the GW self-energy ionic gradients
• Theory of excitonic polarons: From models to first-principles calculations
• Exciton self-trapping in bulk polyethylene
• Pros and Cons of the Bethe-Salpeter Formalism for Ground-State Energies
• The correlation energy functional within the GW-RPA approximation: exact forms, approximate forms and challenges
• Connections between many-body perturbation and coupled-cluster theories
• Self-Trapped Excitons in Metal-Halide Perovskites Investigated by Time-Dependent Density Functional Theory
• Conserving quasiparticle calculations for small metal clusters
• Strong exciton regulation of Raman scattering in monolayer dichalcogenides
• Optical response of small closed-shell sodium clusters
• A Guide to Molecular Properties from the Bethe-Salpeter Equation
• Fully Analytic Nuclear Gradients for the Bethe--Salpeter Equation
• Analytic $G_0{W}_0$ gradients based on a double-similarity transformation equation-of-motion coupled-cluster treatment
• Exploring the Influence of Dynamic Disorder on Transport Gap in Solid Pentacene