Abstract

Abstract Two-dimensional (2D) organic–inorganic perovskites have shown interesting optical properties due to the natural quantum-well structures. The repetition of soft organic and hard inorganic intercalations also renders 2D perovskites rich phonon dynamics. Here, we investigated the coherent acoustic phonons in (PEA)2PbI4 perovskite films by time-resolved Brillouin spectroscopy. The coherent acoustic phonons were launched indirectly in perovskite films by exciting Au nanoplates which were used as optoacoustic transducers. A longitudinal sound velocity ν = 1937 ± 31 m/s, and an elastic modulus E = 9.84 GPa along the cross-plane direction of perovskites were obtained from analysis of the Brillouin oscillation frequency. Following a bead-spring model, we calculated a spring constant k ≈ 1.709 N m−1 for PEA cations which is comparably small for perovskites. We also demonstrated that coherent acoustic phonons are sensitive to differentiate structural heterogeneity and monitor dynamic phase evolution in perovskite films. Domains of PbI2-rich and PbI2-poor phases were identified. Under light stimulus, PbI2-poor phases were gradually disappearing and PbI2-rich phases became crystallized. The observations of structural and elastic heterogeneity and dynamic phase evolution using coherent acoustic phonons provide a toolbox for submicroscale elastic characterization of perovskites.

Highlights

  • Hybrid organic–inorganic halide perovskites have attracted enormous attention in photovoltaics and optoelectronic applications, including solar cells, light-emitting diodes, and photodetectors [1,2,3], due to their large light absorption coefficients, high photoluminescence quantum yields, tunable wide spectral ranges, and low-cost solution manufacturing processes [4,5,6]

  • We demonstrated that coherent acoustic phonons are sensitive to differentiate structural heterogeneity and monitor dynamic phase evolution in perovskite films

  • We have demonstrated that coherent acoustic phonons can probe the structural inhomogeneity and ion migrations in phenethylammonium lead iodide ((PEA)2PbI4) perovskites which were used as a model to investigate structural response under environmental stresses

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Summary

Introduction

Hybrid organic–inorganic halide perovskites have attracted enormous attention in photovoltaics and optoelectronic applications, including solar cells, light-emitting diodes, and photodetectors [1,2,3], due to their large light absorption coefficients, high photoluminescence quantum yields, tunable wide spectral ranges, and low-cost solution manufacturing processes [4,5,6]. We have demonstrated that coherent acoustic phonons can probe the structural inhomogeneity and ion migrations in phenethylammonium lead iodide ((PEA)2PbI4) perovskites which were used as a model to investigate structural response under environmental stresses. The coherent acoustic phonons were launched in perovskites by exciting single Au nanoplates (NPLs) which were deposited on surface of the film and used as optoacoustic transducers. Propagation of coherent acoustic phonons in perovskites was detected in time-resolved Brillouin microscopy with probe wavelength of 530 nm that is close to the energy bandgap. Propagation of coherent acoustic phonons in perovskite film was detected with pump-probe spectroscopy.

PbI2-rich
Conclusions
Experimental methods
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