A finite field approach to solving the Bethe Salpeter equation

Abstract

We present a method to compute optical spectra and exciton binding energies of molecules and solids based on the solution of the Bethe-Salpeter equation (BSE) and the calculation of the screened Coulomb interaction in finite field. The method does not require the explicit evaluation of dielectric matrices nor of virtual electronic states, and can be easily applied without resorting to the random phase approximation. In addition it utilizes localized orbitals obtained from Bloch states using bisection techniques, thus greatly reducing the complexity of the calculation and enabling the efficient use of hybrid functionals to obtain single particle wavefunctions. We report exciton binding energies of several molecules and absorption spectra of condensed systems of unprecedented size, including water and ice samples with hundreds of atoms.

References in corpus (15)

• Phonons and related properties of extended systems from density-functional perturbation theory
• Maximally localized Wannier functions: Theory and applications
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Yambo: an \textit{ab initio} tool for excited state calculations
• Ab initio calculation of excitonic effects in the optical spectra of semiconductors
• Self-consistent hybrid functional for condensed systems
• Turbo charging time-dependent density-functional theory with Lanczos chains
• A new and efficient approach to time-dependent density-functional perturbation theory for optical spectroscopy
• Charge-transfer excitations in molecular donor-acceptor complexes within the many-body Bethe-Salpeter approach
• Bound excitons in time-dependent density-functional-theory: optical and energy-loss spectra
• An assessment of the low-lying excitation energies and triplet instabilities of organic molecules with an ab initio Bethe-Salpeter equation approach
• Large scale GW-BSE calculations with N3 scaling: excitonic effects in dye sensitised solar cells
• Cubic-scaling iterative solution of the Bethe-Salpeter equation for finite systems
• A Finite-field Approach for $GW$ Calculations Beyond the Random Phase Approximation
• First-principles investigation of organic photovoltaic materials C${}_{60}$, C${}_{70}$, [C${}_{60}$]PCBM, and bis-[C${}_{60}$]PCBM using a many-body $G_0{W}_0$-Lanczos approach

Cited by in corpus (20)

• The Bethe-Salpeter Equation Formalism: From Physics to Chemistry
• Quantum simulations of materials on near-term quantum computers
• Reference Energies for Intramolecular Charge-Transfer Excitations
• Quantum Embedding Theory for Strongly-correlated States in Materials
• Photoluminescence spectra of point defects in semiconductors: validation of first principles calculations
• Roadmap on Electronic Structure Codes in the Exascale Era
• GPU Acceleration of Large-Scale Full-Frequency GW Calculations
• Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory
• Simulating the electronic structure of spin defects on quantum computers
• First-principles Studies of Strongly Correlated States in Defect Spin Qubits in Diamond
• Fast optical absorption spectra calculations for periodic solid state systems
• Bethe Salpeter Equation Spectra for Very Large Systems
• PyCDFT: A Python package for constrained density functional theory
• Computational protocol to evaluate electron-phonon interactions within density matrix perturbation theory
• A finite electric-field approach to evaluate the vertex correction for the screened Coulomb interaction in the quasiparticle self-consistent GW method
• GPU-Accelerated Solution of the Bethe-Salpeter Equation for Large and Heterogeneous Systems
• Optical absorption spectroscopy probes water wire and its ordering in a hydrogen-bond network
• Optical spectra of small silver clusters with the Bethe-Salpeter formalism: a Reassessment
• Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange
• First-principles predictions of out-of-plane group IV and V dimers as high-symmetry high-spin defects in hexagonal boron nitride