Abstract

Crystallographic dislocation has been well-known to be one of the major causes responsible for the unfavorable carrier dynamics in conventional semiconductor devices. Halide perovskite has exhibited promising applications in optoelectronic devices. However, how dislocation impacts its carrier dynamics in the ‘defects-tolerant’ halide perovskite is largely unknown. Here, via a remote epitaxy approach using polar substrates coated with graphene, we synthesize epitaxial halide perovskite with controlled dislocation density. First-principle calculations and molecular-dynamics simulations reveal weak film-substrate interaction and low density dislocation mechanism in remote epitaxy, respectively. High-resolution transmission electron microscopy, high-resolution atomic force microscopy and Cs-corrected scanning transmission electron microscopy unveil the lattice/atomic and dislocation structure of the remote epitaxial film. The controlling of dislocation density enables the unveiling of the dislocation-carrier dynamic relation in halide perovskite. The study provides an avenue to develop free-standing halide perovskite film with low dislocation density and improved carried dynamics.

Highlights

  • Density functional theory (DFT) simulations and experimental implementation show that the modified electrostatic potential of polar substrates coated with graphene enables tunable film-substrate interaction strength leading to controlled dislocation density in epilayer

  • The epitaxial relationships have been revealed by high resolution Xray diffraction (XRD) reciprocal space mapping (RSM) and pole figures, which are out-of-plane CsPbBr3(001)‖Gr/NaCl(001)

  • The ferroelastic phase transition kinetics can be controlled by filmsubstrate coupling and remote epitaxy yields large spatial periodicity of the ferroelastic domains in CsPbBr3

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Summary

Introduction

The surface morphology and height profiles of both ionic and remote epitaxial films are shown in Supplementary Fig. 6c, g and d, h, respectively. The as-grown CsPbBr3 flakes in remote epitaxy and the status of graphene after growth are characterized by Raman spectrum and mapping, as shown in Supplementary Fig. 7b and c–f, respectively.

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