How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

Abstract

Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics. When combined with first-principles calculations and applied to the prototypical MAPbI${}_3$ system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Our findings demonstrate that orbital overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.

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Cited by in corpus (29)

• Ultrafast imaging of polariton propagation and interactions
• Dynamic Shortening of Disorder Potentials in Anharmonic Halide Perovskites
• Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors
• Fast and anomalous exciton diffusion in two-dimensional hybrid perovskites
• Vibrational relaxation dynamics in layered perovskite quantum wells
• Photoinduced phase separation in the lead halides is a polaronic effect
• A unification of the Holstein polaron and dynamic disorder pictures of charge transport in organic semiconductors
• The tetragonal phase of CH${}_3$NH${}_3$PbI${}_3$ is strongly anharmonic
• Excitonic polarons and self-trapped excitons from first-principles exciton-phonon couplings
• High Open-Circuit Voltages in Lead-Halide Perovskite Solar Cells - Experiment, Theory and Open Questions
• Dynamic Nanodomains Dictate Macroscopic Properties in Lead Halide Perovskites
• Bond-Peierls polaron: Moderate mass enhancement and current-carrying ground state
• The Disorder Origin of Raman Scattering In Perovskites Single Crystals
• Size-dependent lattice symmetry breaking determines the exciton fine structure of perovskite nanocrystals
• Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite
• Simulations of Trions and Biexcitons in Layered Hybrid Organic-Inorganic Lead Halide Perovskites
• Quantifying polaronic effects on charge-carrier scattering and mobility in lead--halide perovskites
• Tight-binding description of inorganic lead halide perovskites in cubic phase
• A Reciprocal-Space Formulation of Mixed Quantum-Classical Dynamics
• Frenkel/charge transfer Holstein Hamiltonian applied to energy transfer in 2D layered metal-organic frameworks
• Charge transport limited by nonlocal electron-phonon interaction. II. Numerically exact quantum dynamics in the slow-phonon regime
• Conductivity of an electron coupled to anharmonic phonons
• Halide perovskites under polarized light: Vibrational symmetry analysis using polarized Raman
• Towards understanding the electronic structure of the simpler members of two-dimensional halide-perovskites
• Thermal fluctuations and carrier localization induced by dynamic disorder in MAPbI3 described by a first-principles based tight-binding model
• Description of Excitonic Absorption Using the Sommerfeld Enhancement Factor and Band-Fluctuations
• Domain-Wall Ferroelectric Polarons in a two-dimensional Rotor Lattice Model
• Quantum-classical study of charge transport in organic semiconductors with multiple low-frequency vibrational modes
• Renormalization of excitonic properties by polar phonons