Unified theory of electron-phonon renormalization and phonon-assisted optical absorption

Abstract

We present a theory of electronic excitation energies and optical absorption spectra which incorporates energy-level renormalization and phonon-assisted optical absorption within a unified framework. Using time-independent perturbation theory we show how the standard approaches for studying vibronic effects in molecules and those for addressing electron-phonon interactions in solids correspond to slightly different choices for the non-interacting Hamiltonian. Our present approach naturally leads to the Allen-Heine theory of temperature-dependent energy levels, the Franck-Condon principle, the Herzberg-Teller effect and to phonon-assisted optical absorption in indirect band gap materials. In addition, our theory predicts sub-gap phonon-assisted optical absorption in direct gap materials, as well as an exponential edge which we tentatively assign to the Urbach tail. We also consider a semiclassical approach to the calculation of optical absorption spectra which simultaneously captures energy-level renormalization and phonon-assisted transitions and is especially suited to first-principles electronic structure calculations. We demonstrate this approach by calculating the phonon-assisted optical absorption spectrum of bulk silicon.

arXiv commentThis is an author-created, un-copyedited version of an article published in J. Phys.: Condens. Matter. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at http://dx.doi.org/10.1088/0953-8984/26/36/365503

References in corpus (12)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Phonons and related properties of extended systems from density-functional perturbation theory
• Ab initio pseudopotentials for electronic structure calculations of poly-atomic systems using density-functional theory
• Phonon-assisted optical absorption in silicon from first principles
• {\it Ab--initio} finite temperature excitons
• Anharmonic vibrational properties in periodic systems: energy, electron-phonon coupling, and stress
• Temperature Dependence of the Band Gap of Semiconducting Carbon Nanotubes
• Effect of the quantistic zero-point atomic motion on the opto-electronic properties of diamond and trans-polyacetylene
• Excited-state Forces within a First-principles Green's Function Formalism
• Comparing electron-phonon coupling strength in diamond, silicon and silicon carbide: First-principles study
• A path-integral molecular dynamics simulation of diamond
• Theory of temperature dependent phonon-renormalized properties

Cited by in corpus (35)

• Electron-phonon interactions from first principles
• One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization
• Theory of the special displacement method for electronic structure calculations at finite temperature
• Stochastic approach to phonon-assisted optical absorption
• First-principles calculations of indirect Auger recombination in nitride semiconductors
• Anharmonic stabilization and band gap renormalization in the perovskite CsSnI${}_3$
• Correlation effects on electron-phonon coupling in semiconductors: many-body theory along thermal lines
• Exciton-phonon coupling in the UV absorption and emission spectra of bulk hexagonal boron nitride
• Vibrational averages along thermal lines
• First-Principles Electron Transport with Phonon Coupling: Large-Scale at Low Cost
• Giant electron-phonon interactions in molecular crystals and the importance of non-quadratic coupling
• Energy gap closure of crystalline molecular hydrogen with pressure
• Phonon-assisted optical absorption in BaSnO${}_3$ from first principles
• Theory of temperature dependent phonon-renormalized properties
• Phonon-induced localization of excitons in molecular crystals from first principles
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Vibrational renormalisation of the electronic band gap in hexagonal and cubic ice
• Finite temperature optoelectronic properties of BAs from first principles
• Wannier Function Perturbation Theory: Localized Representation and Interpolation of Wavefunction Perturbation
• Phonon limited thermoelectric transport in Pb
• Quantum Confinement of Electron-Phonon Coupling in Graphene Quantum Dots
• Boron phosphide as a \emph{p}-type transparent conductor: optical absorption and transport through electron-phonon coupling
• Temperature dependence of the optical properties of silicon nanocrystals
• Ab initio investigation on the experimental observation of metallic hydrogen
• Self-consistent electron lifetimes for electron-phonon scattering
• Phonon-assisted damping of plasmons in three- and two-dimensional metals
• Ab initio calculation of the magnetic Gibbs free energy of materials using magnetically constrained supercells
• Electronic structure and optical properties of quantum crystals from first principles calculations in the Born-Oppenheimer approximation
• Internal Geometric Friction in a Kitaev Chain Heat Engine
• Indirect light absorption model for highly strained silicon infrared sensors
• Electron-phonon interaction contribution to the total energy of group IV semiconductor polymorphs: evaluation and implications
• Topological and Finite Size Effects in a Kitaev Chain Heat Engine
• Coupled Oscillators and Dielectric Function
• Stochastic sampling of quadrature grids for the evaluation of vibrational expectation values
• Phonon-assisted photoluminescence of bilayer MoS${}_2$ from first principles