Dynamic Optical Properties of CH3NH3PbI3 Single Crystals As Revealed by One- and Two-Photon Excited Photoluminescence Measurements

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Abstract
The dynamic optical properties of perovskite CH3NH3PbI3 single crystals were studied by means of time-resolved photoluminescence (PL) spectroscopy at room temperature. The PL peak under one-photon excitation exhibits a red-shift with elapsing time, while two-photon PL is time-independent and appears at lower energy levels. The low-energy two-photon PL can be attributed to emissions from the localized states because of strong band-to-band absorption and photon re-absorption of the emitted light in the interior region. We revealed that the PL behaviors can be explained by the diffusion of photocarriers generated in the near-surface region to the interior region. The excitation fluence dependence of the one-photon PL dynamics is also discussed in terms of the electron–hole radiative recombination and carrier diffusion effects.
Funding Information
  • Sumitomo Electric Industries, Ltd.
  • Core Research for Evolutional Science and Technology, Japan Science and Technology Agency
  • Japan Science and Technology Agency

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