Third-Order Optical Nonlinearities in Organometallic Methylammonium Lead Iodide Perovskite Thin Films

Basanth S. Kalanoor, Laxman Gouda, Ronen Gottesman, Shay Tirosh, Eynav Haltzi, Arie Zaban, Yaakov R. Tischler*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

138 Scopus citations

Abstract

With solar conversion efficiencies surpassing 20%, organometallic perovskites show tremendous promise for solar cell technology. Their high brightness has also led to demonstrations of lasing and power-efficient electroluminescence. Here we show that thin films of methylammonium lead iodide, prepared by solution processing at temperatures not exceeding 100°C, exhibit a highly nonlinear intensity-dependent refractive index due to changes in the free-carrier concentration and for femtosecond excitation at higher intensities undergo saturation that can be attributed to the Pauli blocking effect. Nonlinear refractive index and nonlinear absorption coefficients were obtained by the Z-scan technique, performed simultaneously in open- A nd closed-aperture configurations. Both nanosecond- A nd femtosecond-pulsed lasers at multiple wavelengths were used in order to distinguish between the mechanisms inducing the nonlinearities. The magnitude and sign of the nonlinear refractive index n2 were determined. For resonant excitation, free carrier generation is the dominant contribution to the nonlinear refractive index, with a large nonlinear refractive index of n2 = 69 × 10-12 cm2/W being observed for resonant femtosecond pumping and n2 = 34.4 × 10-9 cm2/W for resonant nanosecond pumping. For nonresonant femtosecond excitation, bound-charge-induced nonlinearity leads to n2 = 36 × 10-12 cm2/W. These values are equivalent to the best reported metrics for conventional semiconductors, suggesting that organometallic perovskites are promising materials for optical switching and bistability applications.

Original languageAmerican English
Pages (from-to)361-370
Number of pages10
JournalACS Photonics
Volume3
Issue number3
DOIs
StatePublished - 16 Mar 2016
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2016 American Chemical Society.

Keywords

  • Kerr effect
  • Z-scan
  • methyl ammonium lead iodide
  • nonlinear optics
  • nonlinear refraction
  • organometallic perovskite

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