<p>Epitaxial growth on lattice-(mis)matched substrates has advanced the understanding of semiconductors and enabled high-end technologies such as III-V-based light-emitting diodes. However, for metal halide perovskites, there is a knowledge gap in thin film heteroepitaxial growth, hindering progress towards new applications. Here we demonstrate the epitaxial growth of cubic (α)-CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> films on lattice-matched KCl substrates by pulsed laser deposition at room temperature. Epitaxial stabilization of α-CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> is confirmed via reciprocal space mapping, X-ray diffraction pole figures, electron backscatter diffraction and photoluminescence. A bandgap of 1.66 eV stable for over 300 days and Urbach energies of 12.3 meV for 15-nm-thick films are demonstrated. The impact of strain on α-phase stabilization is corroborated by first-principles density functional theory calculations, which also predict substantial bandgap tunability. This work demonstrates the potential of pulsed laser deposition for vapour-phase heteroepitaxial growth of metal halide perovskites, inspiring studies to unlock novel functionalities.</p><p></p>

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Room-temperature epitaxy of α-CH3NH3PbI3 halide perovskite by pulsed laser deposition

  • Junia S. Solomon,
  • Tatiana Soto-Montero,
  • Yorick A. Birkhölzer,
  • Daniel M. Cunha,
  • Wiria Soltanpoor,
  • Martin Ledinský,
  • Nikolai Orlov,
  • Erik C. Garnett,
  • Nicolás Forero-Correa,
  • Sebastian E. Reyes-Lillo,
  • Thomas B. Haward,
  • Joshua R. S. Lilly,
  • Laura M. Herz,
  • Gertjan Koster,
  • Guus Rijnders,
  • Linn Leppert,
  • Monica Morales-Masis

摘要

Epitaxial growth on lattice-(mis)matched substrates has advanced the understanding of semiconductors and enabled high-end technologies such as III-V-based light-emitting diodes. However, for metal halide perovskites, there is a knowledge gap in thin film heteroepitaxial growth, hindering progress towards new applications. Here we demonstrate the epitaxial growth of cubic (α)-CH3NH3PbI3 films on lattice-matched KCl substrates by pulsed laser deposition at room temperature. Epitaxial stabilization of α-CH3NH3PbI3 is confirmed via reciprocal space mapping, X-ray diffraction pole figures, electron backscatter diffraction and photoluminescence. A bandgap of 1.66 eV stable for over 300 days and Urbach energies of 12.3 meV for 15-nm-thick films are demonstrated. The impact of strain on α-phase stabilization is corroborated by first-principles density functional theory calculations, which also predict substantial bandgap tunability. This work demonstrates the potential of pulsed laser deposition for vapour-phase heteroepitaxial growth of metal halide perovskites, inspiring studies to unlock novel functionalities.