Polarization-selective three-photon absorption and subsequent photoluminescence in CsPbBr3 single crystal at room temperature

D. J. Clark, C. C. Stoumpos, F. O. Saouma, Mercouri G Kanatzidis, J. I. Jang

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Abstract

We report on highly polarization-selective three-photon absorption (3PA) in a Bridgman-grown single crystal of CsPbBr3 oriented along the (112) direction, which is an inorganic counterpart to emerging organic-inorganic hybrid halide perovskites for solar-cell and optoelectronic applications. The crystal exhibits strong photoluminescence (PL) at room temperature as a direct consequence of 3PA of fundamental radiation. Interestingly, 3PA disappears when the input polarization is parallel to the (-110) direction. This 3PA effect is strongest when orthogonal to (-110) and the corresponding 3PA coefficient was measured to be γ=0.14±0.03cm3/GW2 under picosecond-pulse excitation at the fundamental wavelength of λ=1200 nm. The laser-induced damage threshold was also determined to be about 20 GW/cm2 at the same wavelength. Based on relative PL intensities upon λ tuning over the entire 3PA range (1100-1700 nm), we determined the nonlinear optical dispersion of the 3PA coefficient for CsPbBr3, which is consistent with a theoretical prediction. Experimentally observed significant polarization dependence of γ was explained by relevant selection rules. The perovskite is potentially important for nonlinear optical applications owing to its highly efficient 3PA-induced PL response with a sharp on/off ratio by active polarization control.

Original languageEnglish
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume93
Issue number19
DOIs
Publication statusPublished - May 5 2016

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ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

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