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

F. O. Saouma, C. C. Stoumpos, J. Wong, M. G. Kanatzidis and J. I. Jang ()
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F. O. Saouma: State University of New York (SUNY) at Binghamton
C. C. Stoumpos: Northwestern University
J. Wong: State University of New York (SUNY) at Binghamton
M. G. Kanatzidis: Northwestern University
J. I. Jang: State University of New York (SUNY) at Binghamton

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: 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, $${n_2} \propto E_{\rm{g}}^{ - 4}$$ n 2 ∝ E g - 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.

Date: 2017
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DOI: 10.1038/s41467-017-00788-x

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