Local structural disorder in crystalline materials

Abstract

Local positional disorder in soft, anharmonic materials has emerged as a central factor in shaping their electronic, vibrational, optical, and transport properties. Viewed mainly as a source of performance degradation, recent theoretical insights reveal that local disorder profoundly influences the electronic structure and phonon dynamics, without inducing deep electronic traps or non-radiative recombination pathways. In this work, we highlight advances in modeling local disorder using polymorphous and anharmonic frameworks, showing how these methods explain experimental observations and predict new trends. We emphasize the role of disorder in the breakdown of the phonon quasiparticle picture and in modulating electron-phonon and phonon-phonon interactions, particularly in soft, anharmonic phases of matter, with significant effects on electrical and thermal transport. We outline opportunities for integrating these insights into predictive modeling for energy materials and propose combining advanced first-principles methods with machine learning.

References in corpus (26)

• Electron-phonon interactions from first principles
• Lattice dynamics of anharmonic solids from first principles
• Local polar fluctuations in lead halide perovskite crystals
• Self-consistent phonon calculations of lattice dynamical properties in cubic SrTiO${}_3$ with first-principles anharmonic force constants
• Direct Observation of Dynamic Symmetry Breaking above Room Temperature in Methylammonium Lead Iodide Perovskite
• Perturbo: a software package for ab initio electron-phonon interactions, charge transport and ultrafast dynamics
• Origin of band gaps in 3d perovskite oxides
• The Stochastic Self-Consistent Harmonic Approximation: Calculating Vibrational Properties of Materials with Full Quantum and Anharmonic Effects
• The polymorphous nature of cubic halide perovskites
• Second order structural phase transitions, free energy curvature, and temperature-dependent anharmonic phonons in the self-consistent harmonic approximation: theory and stochastic implementation
• Anharmonicity and Ultra-Low Thermal Conductivity in Lead-Free Halide Double Perovskites
• A polymorphous band structure model of gapping in the anti-ferromagnetic and paramagnetic phases of the Mott insulators MnO, FeO, CoO, and NiO
• Theory of the special displacement method for electronic structure calculations at finite temperature
• Direct evidence of weakly dispersed and strongly anharmonic optical phonons in hybrid perovskites
• Anharmonic electron-phonon coupling in ultrasoft and locally disordered perovskites
• The effects of intrinsic local distortions vs. dynamic thermal motions on the stability and band gaps of cubic oxide and halide perovskites
• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• Predicting charge transport in the presence of polarons: The beyond-quasiparticle regime in SrTiO${}_3$
• Anharmonic lattice dynamics via the special displacement method
• Anharmonic lattice dynamics in large thermodynamic ensembles with machine-learning force fields: CsPbBr${}_3$ a phonon-liquid with Cs rattlers
• Aziridinium lead iodide: a stable, low bandgap hybrid halide perovskite for photovoltaics
• Dynamic Nanodomains Dictate Macroscopic Properties in Lead Halide Perovskites
• Ultrafast lattice disordering can be accelerated by electronic collisional forces
• Multiple lattice instabilities and complex ground state in Cs${}_2$AgBiBr${}_6$
• Energy-lowering symmetry breaking creates a flat-band insulator in paramagnetic Nb3Cl8
• Efficient First-Principles Framework for Overdamped Phonon Dynamics and Anharmonic Electron-Phonon Coupling in Superionic Materials