Selective enhancement of optical nonlinearity in two-dimensional organic-inorganic lead iodide perovskites

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

Research output: Contribution to journalArticle

31 Citations (Scopus)

Abstract

Reducing the dimensionality of three-dimensional hybrid metal halide perovskites can improve their optoelectronic properties. Here, we show that the third-order optical nonlinearity, n 2, of hybrid lead iodide perovskites is enhanced in the two-dimensional Ruddlesden-Popper series, (CH3(CH2)3NH3)2(CH3NH3) n-1Pb n I3n+1 (n = 1-4), where the layer number (n) is engineered for bandgap tuning from E g = 1.60 eV (n = ∞; bulk) to 2.40 eV (n = 1). Despite the unfavorable relation, n2 ∝ Eg -4, strong quantum confinement causes these two-dimensional perovskites to exhibit four times stronger third harmonic generation at mid-infrared when compared with the three-dimensional counterpart, (CH3NH3)PbI3. Surprisingly, however, the impact of dimensional reduction on two-photon absorption, which is the Kramers-Kronig conjugate of n 2, is rather insignificant as demonstrated by broadband two-photon spectroscopy. The concomitant increase of bandgap and optical nonlinearity is truly remarkable in these novel perovskites, where the former increases the laser-induced damage threshold for high-power nonlinear optical applications.

Original languageEnglish
Article number742
JournalNature Communications
Volume8
Issue number1
DOIs
Publication statusPublished - Dec 1 2017

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Iodides
perovskites
Photons
iodides
Energy gap
nonlinearity
Metal halides
Laser damage
Quantum confinement
augmentation
Harmonic generation
Optoelectronic devices
Spectrum Analysis
Lasers
Tuning
Metals
Spectroscopy
Infrared radiation
metal halides
photons

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Selective enhancement of optical nonlinearity in two-dimensional organic-inorganic lead iodide perovskites. / Saouma, F. O.; Stoumpos, C. C.; Wong, J.; Kanatzidis, Mercouri G; Jang, J. I.

In: Nature Communications, Vol. 8, No. 1, 742, 01.12.2017.

Research output: Contribution to journalArticle

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