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Anti-Stokes photoluminescence from CsPbBr3 nanostructures embedded in a Cs4PbBr6 crystal

Yuto Kajino1, Shuji Otake1, Takumi Yamada2, Kazunobu Kojima3,*, Tomoya Nakamura2, Atsushi Wakamiya2, Yoshihiko Kanemitsu2, and Yasuhiro Yamada1,†

  • 1Graduate School of Science, Chiba University, Inage, Chiba 263-8522, Japan
  • 2Institute for Chemical Research, Kyoto University, Gokasho, Uji 611-0011, Japan
  • 3Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Aoba, Sendai 980-8577, Japan

  • *Present address: Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, 565-0871, Japan.
  • †yasuyamada@chiba-u.jp

Phys. Rev. Materials 6, L043001 – Published 14 April, 2022

DOI: https://doi.org/10.1103/PhysRevMaterials.6.L043001

Abstract

Lead halide perovskites possess high photoluminescence (PL) efficiency and strong electron-phonon interactions, and therefore optical cooling using up-conversion PL has been expected. We investigate anti-Stokes PL from green-luminescent Cs4PbBr6, whose origin is attributable to CsPbBr3 nanostructures embedded in a Cs4PbBr6 crystal. Because of the high transparency, low refractive index, and high stability of Cs4PbBr6, the green PL displays high external quantum efficiency without photodegradation. Time-resolved PL spectroscopy reveals the excitonic behaviors in the recombination process. The shape of the PL spectrum is almost independent of excitation photon energy, which means that the spectral width is determined by homogeneous broadening. We demonstrate that the phonon-assisted process dominates the Urbach tail of optical absorption and anti-Stokes PL at room temperature. Anti-Stokes PL is observed down to 70 K. We determine the temperature dependence of the Urbach energy and estimate the strength of the electron-phonon coupling. Our spectroscopic data show that CsPbBr3 nanostructures have potentially useful features for optical cooling.

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