The influence of high-energy local orbitals and electron-phonon interactions on the band gaps and optical spectra of hexagonal boron nitride

Abstract

We report $ab$ $initio$ band diagram and optical absorption spectra of hexagonal boron nitride ($h$-BN), focusing on unravelling how the completeness of basis set for $GW$ calculations and how electron-phonon interactions (EPIs) impact on them. The completeness of basis set, an issue which was seldom discussed in previous optical spectra calculations of $h$-BN, is found crucial in providing converged quasiparticle band gaps. In the comparison among three different codes, we demonstrate that by including high-energy local orbitals in the all-electron linearized augmented plane waves based $GW$ calculations, the quasiparticle direct and fundamental indirect band gaps are widened by $\sim$0.2 eV, giving values of 6.81 eV and 6.25 eV respectively at the $G{W}_0$ level. EPIs, on the other hand, reduce them to 6.62 eV and 6.03 eV respectively at 0 K, and 6.60 eV and 5.98 eV respectively at 300 K. With clamped crystal structure, the first peak of the absorption spectrum is at 6.07 eV, originating from the direct exciton contributed by electron transitions around $K$ in the Brillouin zone. After including the EPIs-renormalized quasiparticles in the Bethe-Salpeter equation, the exciton-phonon coupling shifts the first peak to 5.83 eV at 300 K, lower than the experimental value of $\sim$6.00 eV. This accuracy is acceptable to an $ab$ $initio$ description of excited states with no fitting parameter.

References in corpus (27)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Van der Waals heterostructures
• Boron nitride substrates for high-quality graphene electronics
• Angle-resolved photoemission spectroscopy of the cuprate superconductors
• Electron-phonon interactions from first principles
• Hexagonal boron nitride is an indirect bandgap semiconductor
• Yambo: an \textit{ab initio} tool for excited state calculations
• Many-body perturbation theory calculations using the yambo code
• Huge excitonic effects in layered hexagonal boron nitride
• Two-dimensional Quasi-Freestanding Molecular Crystals for High-Performance Organic Field-Effect Transistors
• {\it Ab--initio} finite temperature excitons
• Observation of an intrinsic bandgap and Landau level renormalization in graphene/boron-nitride heterostructures
• The Band-Gap Problem in Semiconductors Revisited: Effects of Core States and Many-Body Self-Consistency
• Adequacy of Approximations in GW Theory
• Effect of Semicore Orbitals on the Electronic Band Gaps of Si, Ge, and GaAs within the GW Approximation
• Bright luminescence from indirect and strongly bound excitons in hBN
• Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure
• The temperature dependence of electronic eigenenergies in the adiabatic harmonic approximation
• Verification of first-principles codes: comparison of total energies, phonon frequencies, electron-phonon coupling and zero-point motion correction to the gap between ABINIT and QE/Yambo
• Accurate all-electron $G_0{W}_0$ quasiparticle energies employing the full-potential augmented planewave method
• Elimination of the linearization error in GW calculations based on the linearized augmented-plane-wave method
• Exciton-phonon coupling in the UV absorption and emission spectra of bulk hexagonal boron nitride
• Theory of phonon-assisted luminescence in solids: application to hexagonal boron nitride
• Exciton-phonon interaction in the strong coupling regime in hexagonal boron nitride
• Diffusion quantum Monte Carlo and GW study of the electronic properties of monolayer and bulk hexagonal boron nitride
• Electron-phonon scattering effects on electronic and optical properties of orthorhombic GeS
• Giant exciton-phonon coupling and zero-point renormalization in hexagonal monolayer boron nitride

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