TY - JOUR
T1 - Selective enhancement of optical nonlinearity in two-dimensional organic-inorganic lead iodide perovskites
AU - Saouma, F. O.
AU - Stoumpos, C. C.
AU - Wong, J.
AU - Kanatzidis, M. G.
AU - Jang, J. I.
N1 - Funding Information:
This work was supported by Basic Science Research Program (2017R1D1A1B03035539) through the National Research Foundation of Korea (NRF), funded by the Korean government. C.C.S. and M.G.K. acknowledge the support under ONR Grant N00014-17-1-2231. We thank Gooch and Housego for generously supplying a high-quality AgGaSe2 crystal.
PY - 2017/12/1
Y1 - 2017/12/1
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-017-00788-x
DO - 10.1038/s41467-017-00788-x
M3 - Article
C2 - 28963449
AN - SCOPUS:85030311356
VL - 8
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 742
ER -