Approximate Excited-State Potential Energy Surfaces for Defects in Solids

Abstract

A description of electron-phonon coupling at a defect or impurity is essential to characterizing and harnessing its functionality for a particular application. Electron-phonon coupling limits the amount of useful light produced by a single-photon emitter and can destroy the efficiency of optoelectronic devices by enabling defects to act as recombination centers. Information on atomic relaxations in the excited state of the center is needed to assess electron-phonon coupling but may be inaccessible due to failed convergence or computational expense. Here we develop an approximation technique to quantify electron-phonon coupling using only the forces of the excited state evaluated in the equilibrium geometry of the ground state. The approximations are benchmarked on well-studied defect systems, namely C${}_{\mathrm{N}}$ in GaN, the nitrogen-vacancy center in diamond, and the carbon dimer in h-BN. We demonstrate that the zero-phonon line energy can be approximated with just a single mode, while the Huang-Rhys factor converges by including displacements up to the second nearest neighbors. This work also provides important insight into the success of the widely utilized one-dimensional accepting-mode approximation, specifically demonstrating that the accepting-mode Huang-Rhys factor is a strict upper bound on the full multidimensional Huang-Rhys factor.

References in corpus (23)

• First-principles theory of nonradiative carrier capture via multiphonon emission
• First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centre
• First-Principles Calculations of Luminescence Spectrum Line Shapes for Defects in Semiconductors: The Example of GaN and ZnO
• A Computational Framework for Automation of Point Defect Calculations
• Carbon dimer defect as a source of the 4.1 eV luminescence in hexagonal boron nitride
• Nonrad: Computing Nonradiative Capture Coefficients from First Principles
• \emph{Ab initio} calculation of spin-orbit coupling for NV center in diamond exhibiting dynamic Jahn-Teller effect
• A comparative study of ab initio nonradiative recombination rate calculations under different formalisms
• Rapid Recombination by Cadmium Vacancies in CdTe
• Understanding and calibrating Density-Functional-Theory calculations describing the energy and spectroscopy of defect sites in hexagonal boron nitride
• Vibrational and vibronic structure of isolated point defects: the nitrogen-vacancy center in diamond
• Quantum embedding methods for correlated excited states of point defects: Case studies and challenges
• Anharmonic Lattice Relaxation during Non-radiative Carrier Capture
• Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory
• Machine-learning structural reconstructions for accelerated point defect calculations
• A substitutional quantum defect in WS${}_2$ discovered by high-throughput computational screening and fabricated by site-selective STM manipulation
• Rational Design of Efficient Defect-Based Quantum Emitters
• Advances in Quantum Defect Embedding Theory
• First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation
• Temperature dependence of the AB-lines and Optical Properties of the Carbon-Antisite Vacancy Pair in 4H-SiC
• Characterization of Chromium Impurities in $\beta$-Ga${}_2$O${}_3$
• Identifying Split Vacancy Defects with Machine-Learned Foundation Models and Electrostatics
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective

Cited by in corpus (2)

• Machine Learning Phonon Spectra for Fast and Accurate Optical Lineshapes of Defects
• "One defect, one potential" strategy for accurate machine learning prediction of defect phonons