Evidence of large polarons in photoemission band mapping of the perovskite semiconductor CsPbBr${}_3$

Abstract

Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic structure of the inorganic LHP CsPbBr${}_3$ by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass $0.26\pm 0.02m_e$, 50% heavier than the bare mass $m_0=0.17m_e$ predicted by density functional theory. Calculations of electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fröhlich coupling parameter $\alpha =1.82$. A good agreement with our experimental data is obtained within the Feynmann polaron model, validating a viable theorical method to predict the carrier effective mass of LHPs ab-initio.

References in corpus (24)

• 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
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Optimized norm-conserving Vanderbilt pseudopotentials
• Maximally localized Wannier functions: Theory and applications
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Yambo: an \textit{ab initio} tool for excited state calculations
• Bright triplet excitons in lead halide perovskites
• Many-body perturbation theory calculations using the yambo code
• Probing the Low-Energy Electronic Structure of Complex Systems by ARPES
• Froehlich Polaron and Bipolaron: Recent Developments
• Fröhlich electron-phonon vertex from first principles
• Unfolding first-principles band structures
• Giant Rashba Splitting in CH3NH3PbBr3 Organic-Inorganic Perovskite
• Role of Polar Phonons in the Photo Excited State of Metal Halide Perovskites
• Tunable polaronic conduction in anatase TiO2
• The impact of the halide cage on the electronic properties of fully inorganic caesium lead halide perovskites
• Spontaneous Octahedral Tilting in the Cubic Inorganic Caesium Halide Perovskites CsSnX${}_3$ and CsPbX${}_3$ (X = F, Cl, Br, I)
• Tailoring the nature and strength of electron-phonon interactions in the SrTiO${}_3$(001) two-dimensional electron liquid
• Polarons from first principles, without supercells
• Carrier Lifetimes and Polaronic Mass Enhancement in the Hybrid Halide Perovskite CH${}_3$NH${}_3$PbI${}_3$ from Multiphonon Fröhlich Coupling
• Dynamic Symmetry Breaking and Spin Splitting in Metal Halide Perovskites
• Quantum Unfolding: A program for unfolding electronic energy bands of materials

Cited by in corpus (14)

• Electronic Defects in Metal Oxide Photocatalysts
• Nonlinear THz Control of the Lead Halide Perovskite Lattice
• Dynamic Rashba-Dresselhaus Effect
• Is there a polaron signature in angle-resolved photoemission of CsPbBr3?
• Topological polarons in halide perovskites
• Quantifying polaronic effects on charge-carrier scattering and mobility in lead--halide perovskites
• Dark states of electrons in a quantum system with two pairs of sublattices
• The effective mass problem for the Landau-Pekar equations
• Binding energy of polaronic trions and biexcitons in CsPbBr${}_3$ nanocrystals
• Determining Exciton Binding Energy and Reduced Effective Mass in Metal Tri-Halide Perovskites from Optical and Impedance Spectroscopy Measurements
• Strongly Anharmonic Organic Cation Vibrations in Hybrid Lead Halide Perovskite CH3NH3PbI3 on Electronic Ground State
• Quantifying Photoinduced Polaronic Distortions in Inorganic Lead Halide Perovskites Nanocrystals
• Excited-state band structure mapping
• Symmetry-protected topological polarons