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Charge Carrier Localization in Doped Perovskite Nanocrystals Enhances Radiative Recombination

Sascha Feldmann, Mahesh K. Gangishetty, Ivona Bravić, Timo Neumann, Bo Peng, Thomas Winkler, Richard H. Friend, Bartomeu Monserrat, Daniel N. Congreve, Felix Deschler

2021Journal of the American Chemical Society94 citationsDOIOpen Access PDF

Abstract

Nanocrystals based on halide perovskites offer a promising material platform for highly efficient lighting. Using transient optical spectroscopy, we study excitation recombination dynamics in manganese-doped CsPb(Cl,Br)3 perovskite nanocrystals. We find an increase in the intrinsic excitonic radiative recombination rate upon doping, which is typically a challenging material property to tailor. Supported by ab initio calculations, we can attribute the enhanced emission rates to increased charge carrier localization through lattice periodicity breaking from Mn dopants, which increases the overlap of electron and hole wave functions locally and thus the oscillator strength of excitons in their vicinity. Our report of a fundamental strategy for improving luminescence efficiencies in perovskite nanocrystals will be valuable for maximizing efficiencies in light-emitting applications.

Topics & Concepts

Perovskite (structure)ChemistryExcitonDopingDopantNanocrystalLuminescenceHalideSpontaneous emissionChemical physicsCharge carrierAb initioOscillator strengthMolecular physicsOptoelectronicsCondensed matter physicsNanotechnologySpectral lineMaterials scienceInorganic chemistryPhysicsOpticsCrystallographyLaserQuantum mechanicsOrganic chemistryPerovskite Materials and ApplicationsQuantum Dots Synthesis And PropertiesChalcogenide Semiconductor Thin Films