Automated all-functionals infrared and Raman spectra

Abstract

Infrared and Raman spectroscopies are ubiquitous techniques employed in many experimental laboratories, thanks to their fast and non-destructive nature able to capture materials' features as spectroscopic fingerprints. Nevertheless, these measurements frequently need theoretical support in order to unambiguously decipher and assign complex spectra. Linear-response theory provides an effective way to obtain the higher-order derivatives needed, but its applicability to modern exchange-correlation functionals remains limited. Here, we devise an automated, open-source, user-friendly approach based on ground-state density-functional theory and the electric enthalpy functional to allow seamless calculations of first-principles infrared and Raman spectra. By employing a finite-displacement and finite-field approach, we allow for the use of any functional, as well as an efficient treatment of large low-symmetry structures. Additionally, we propose a simple scheme for efficiently sampling the Brillouin zone with different electric fields. To demonstrate the capabilities of our approach, we provide illustrations using the ferroelectric LiNbO${}_3$ crystal as a paradigmatic example. We predict infrared and Raman spectra using various (semi)local, Hubbard corrected, and hybrid functionals. Our results also show how PBE0 and extended Hubbard functionals yield in this case the best match in term of peak positions and intensities, respectively.

References in corpus (32)

• 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
• Maximally-localized generalized Wannier functions for composite energy bands
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Quantum ESPRESSO toward the exascale
• Pseudopotentials for high-throughput DFT calculations
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Precision and efficiency in solid-state pseudopotential calculations
• Hubbard-corrected DFT energy functionals: the LDA+U description of correlated systems
• A First-Principles Approach to Insulators in Finite Electric Fields
• Ensemble density-functional theory for ab-initio molecular dynamics of metals and finite-temperature insulators
• Hubbard parameters from density-functional perturbation theory
• First principles calculation of vibrational Raman spectra in large systems: signature of small rings in crystalline SiO2
• AiiDA 1.0, a scalable computational infrastructure for automated reproducible workflows and data provenance
• Berry-phase treatment of the homogeneous electric field perturbation in insulators
• Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations
• Workflows in AiiDA: Engineering a high-throughput, event-based engine for robust and modular computational workflows
• Adaptively Compressed Exchange Operator
• Breakdown of optical phonons' splitting in two-dimensional materials
• First principles study of electronic and structural properties of CuO
• Norm-conserving pseudopotentials with chemical accuracy compared to all-electron calculations
• Dynamics of Berry-phase polarization in time-dependent electric fields
• Pressure and stress tensor of complex anharmonic crystals within the stochastic self-consistent harmonic approximation
• Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials
• Energetics and cathode voltages of LiMPO${}_4$ olivines (M = Fe, Mn) from extended Hubbard functionals
• Time-Dependent Self Consistent Harmonic Approximation: Anharmonic nuclear quantum dynamics and time correlation functions
• Pulay forces in density-functional theory with extended Hubbard functionals: From nonorthogonalized to orthogonalized manifolds
• Raman spectra of fine-grained materials from first principles
• Automated all-functionals infrared and Raman spectra
• Dielectric Response of Periodic Systems from Quantum Monte Carlo Calculations
• Using high multipolar orders to reconstruct the sound velocity in piezoelectrics from lattice dynamics
• Wigner Gaussian dynamics: simulating the anharmonic and quantum ionic motion

Cited by in corpus (8)

• Automated all-functionals infrared and Raman spectra
• BaZrS${}_{\text{3}}$ Lights Up: The Interplay of Electrons, Photons, and Phonons in Strongly Luminescent Single Crystals
• First-principles Hubbard parameters with automated and reproducible workflows
• Automated computational workflows for muon spin spectroscopy
• Algorithmic differentiation for plane-wave DFT: materials design, error control and learning model parameters
• Ab initio functional-independent calculations of the clamped Pockels tensor of tetragonal barium titanate
• Making atomistic materials calculations accessible with the AiiDAlab Quantum ESPRESSO app
• Elastic Constants and Bending Rigidities from Long-Wavelength Perturbation Expansions