Perspective: Theory and simulation of hybrid halide perovskites

Abstract

Organic-inorganic halide perovskites present a number of challenges for first-principles atomistic materials modelling. These `plastic crystals' feature dynamic processes across multiple length-scales and time-scales, which include: (i) transport of slow ions and fast electrons; (ii) highly anharmonic lattice dynamics with short phonon lifetimes; (iii) local symmetry breaking of the average crystallographic space group; (iv) strong relativistic (spin-orbit coupling) effects on the electronic band structure; (v) thermodynamic metastability and rapid chemical breakdown. These issues, which affect the operation of solar cells, are outlined in this perspective. We also discuss general guidelines for performing quantitative and predictive simulations of these materials, which are relevant to metal-organic frameworks and other hybrid semiconducting, dielectric and ferroelectric compounds.

References in corpus (15)

• Electron-phonon interactions from first principles
• Distribution of phonon lifetime in Brillouin zone
• Identifying defect-tolerant semiconductors with high minority carrier lifetimes: Beyond hybrid lead halide perovskites
• Molecular ferroelectric contributions to anomalous hysteresis in hybrid perovskite solar cells
• Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites
• The Synthesis, Structure and Electronic Properties of a Lead-Free Hybrid Inorganic-Organic Double Perovskite (MA)2KBiCl6 (MA = methylammonium)
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• One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization
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• Tuning of the Thermoelectric Figure of Merit of CH${}_3$NH${}_3$MI${}_3$ (M=Pb,Sn) Photovoltaic Perovskites
• Phonon anharmonicity, lifetimes and thermal transport in CH${}_3$NH${}_3$PbI${}_3$ from many-body perturbation theory
• GW quasiparticle band gap of the hybrid organic-inorganic perovskite CH${}_3$NH${}_3$PbI${}_3$: Effect of spin-orbit interaction, semicore electrons, and self-consistency
• Temperature Dependence of the Energy Levels of Methylammonium Lead Iodide Perovskite from First Principles
• Chemical and Lattice Stability of the Tin Sulfides
• Ab initio thermodynamic model of Cu${}_2$ZnSnS${}_4$

Cited by in corpus (18)

• Perovskite-Inspired Materials for Photovoltaics -- From Design to Devices
• The polymorphous nature of cubic halide perovskites
• On the role of the electron-phonon interaction in the temperature dependence of the gap of lead halide perovskites
• Infrared Spectroscopic Study of Vibrational Modes across the Orthorhombic-Tetragonal Phase Transition in Methylammonium Lead Halide Single Crystals
• Photoinduced phase separation in the lead halides is a polaronic effect
• The tetragonal phase of CH${}_3$NH${}_3$PbI${}_3$ is strongly anharmonic
• Modelization of charge carriers mobilities in halide perovskites: Fröhlich scattering and quantum localization effects in a dynamic disorder regime
• Mixed Formamidinium-Methylammonium Lead Iodide perovskite from first-principles: Hydrogen-bonding impact on the electronic properties
• Structure and Binding in Halide Perovskites: Analysis of Static and Dynamic Effects from Dispersion-Corrected Density Functional Theory
• Modelling Grain Boundaries in Polycrystalline Halide Perovskite Solar Cells
• Enhanced Piezoelectric Response in Hybrid Lead Halide Perovskite Thin Films via Interfacing with Ferroelectric PbZr${}_{0.2}$Ti${}_{0.8}$O${}_3$
• First principles study of ferroelastic twins in halide perovskites
• Influence of Chloride Substitution on the Rotational Dynamics of Methylammonium in MAPbI${}_{3-x}$Cl${}_x$ Perovskites
• Assessing carrier mobility, dopability, and defect tolerance in the chalcogenide perovskite BaZrS${}_3$
• Multiple lattice instabilities and complex ground state in Cs${}_2$AgBiBr${}_6$
• On the question of dynamic domains and critical scattering in cubic methylammonium lead triiodide
• Stress effects on vibrational spectra of a cubic hybrid perovskite: A probe of local strain
• Bond polarizability as a probe of local crystal fields in hybrid lead-halide perovskites