Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory

Abstract

We present a formulation of spin-conserving and spin-flip, hybrid time-dependent density functional theory (TDDFT), including the calculation of analytical forces, which allows for efficient calculations of excited state properties of solid-state systems with hundreds to thousands of atoms. We discuss an implementation on both GPU and CPU based architectures, along with several acceleration techniques. We then apply our formulation to the study of several point defects in semiconductors and insulators, specifically the negatively charged nitrogen-vacancy and neutral silicon-vacancy centers in diamond, the neutral divacancy center in 4H silicon carbide, and the neutral oxygen-vacancy center in magnesium oxide. Our results highlight the importance of taking into account structural relaxations in excited states, in order to interpret and predict optical absorption and emission mechanisms in spin-defects.

References in corpus (26)

• Quantum ESPRESSO toward the exascale
• Self-consistent hybrid functional for condensed systems
• First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centre
• Quantum embedding theories
• Spin dynamics in the optical cycle of single nitrogen-vacancy centres in diamond
• The negatively charged nitrogen-vacancy centre in diamond: the electronic solution
• Optical properties of the nitrogen-vacancy singlet levels in diamond
• New infrared emission of the NV centre in diamond: Zeeman and uniaxial stress studies
• Phonon-Induced Population Dynamics and Intersystem Crossing in Nitrogen-Vacancy Centers
• Quantum simulations of materials on near-term quantum computers
• State-selective intersystem crossing in nitrogen-vacancy centers
• Optical charge state control of spin defects in 4H-SiC
• Photoluminescence and photochemistry of the $V_B^{-}$ defect in hexagonal boron nitride
• Room temperature coherent manipulation of single-spin qubits in silicon carbide with a high readout contrast
• Photoluminescence spectra of point defects in semiconductors: validation of first principles calculations
• Green's function formulation of quantum defect embedding theory
• Vibrational and vibronic structure of isolated point defects: the nitrogen-vacancy center in diamond
• Accurate optical spectra through time-dependent density functional theory based on screening-dependent hybrid functionals
• Designing defect-based qubit candidates in wide-gap binary semiconductors for solid-state quantum technologies
• Optically detected magnetic resonance in neutral silicon vacancy centers in diamond via bound exciton states
• A finite field approach to solving the Bethe Salpeter equation
• Simulating the electronic structure of spin defects on quantum computers
• Non-collinear density functional theory
• First-principles Studies of Strongly Correlated States in Defect Spin Qubits in Diamond
• Quantum simulations of Fermionic Hamiltonians with efficient encoding and ansatz schemes
• Computational protocol to evaluate electron-phonon interactions within density matrix perturbation theory

Cited by in corpus (21)

• Self-Trapped Excitons in Metal-Halide Perovskites Investigated by Time-Dependent Density Functional Theory
• Advances in Quantum Defect Embedding Theory
• Accurate Excitation Energies of Point Defects from Fast Particle-Particle Random Approximation Calculations
• First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
• Quantum Vibronic Effects on the Excitation Energies of the Nitrogen-Vacancy Center in Diamond
• Accurate and Efficient Prediction of Double Excitation Energies Using the Particle-Particle Random Phase Approximation
• GPU-Accelerated Solution of the Bethe-Salpeter Equation for Large and Heterogeneous Systems
• Towards dislocation-driven quantum interconnects
• Energy-Specific Bethe-Salpeter Equation Implementation for Efficient Optical Spectrum Calculations
• Approximate Excited-State Potential Energy Surfaces for Defects in Solids
• First-Principle Investigation Of Near-Field Energy Transfer Between Localized Quantum Emitters in Solids
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective
• Encoded probabilistic imaginary-time evolution on a trapped-ion quantum computer for ground and excited states of spin qubits
• Simulating optically-active spin defects with a quantum computer
• Machine Learning Phonon Spectra for Fast and Accurate Optical Lineshapes of Defects
• Energy transfer between localized emitters in photonic cavities from first principles
• Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange
• Design for telecom-wavelength quantum emitters in silicon based on alkali-metal-saturated vacancy complexes
• Computation of the expectation value of the spin operator ${\hat{S}}^2$ for the Spin-Flip Bethe-Salpeter Equation
• Elucidating the Inter-system Crossing of the Nitrogen-Vacancy Center up to Megabar Pressures
• LibppRPA: An Open-Source Library for Particle-Particle Random Phase Approximation