State Key Laboratory of Structural Chemistry , Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences , Fuzhou , Fujian 350002 , China.
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Key Laboratory of Nanomaterials , Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences , Fuzhou , Fujian 350002 , China.
J Am Chem Soc. 2018 Jun 6;140(22):6806-6809. doi: 10.1021/jacs.8b04014. Epub 2018 May 22.
Perovskite ferroelectrics with prominent nonlinear optical absorption have attracted great attention in the field of photonics. However, they are traditionally dominated by inorganic oxides and exhibit relatively small nonlinear optical absorption coefficients, which hinder their further applications. Herein, we report a new organic-inorganic hybrid bilayered perovskite ferroelectric, (CHNH)(NHCHNH)PbBr (1), showing an above-room-temperature Curie temperature (∼322 K) and notable spontaneous polarization (∼3.8 μC cm). Significantly, the unique quantum-well structure of 1 results in intriguing two-photon absorption properties with a giant nonlinear optical absorption coefficient as high as 5.76 × 10 cm GW, which is almost two-orders of magnitude larger than those of mostly traditional all-inorganic perovskite ferroelectrics. To our best knowledge, 1 is the first example of hybrid ferroelectrics with giant two-photon absorption coefficient. The mechanisms for ferroelectric and two-photon absorption are revealed. This work will shed light on the design of new ferroelectrics with two-photon absorption and promote their potentials in the photonic application.
具有显著非线性光学吸收的钙钛矿铁电体在光子学领域引起了极大的关注。然而，它们传统上由无机氧化物主导，表现出相对较小的非线性光学吸收系数，这阻碍了它们的进一步应用。在此，我们报告了一种新的有机-无机混合双层钙钛矿铁电体(CHNH)(NHCHNH)PbBr3(1)，其具有室温以上的居里温度（约 322 K）和显著的自发极化（约 3.8 μC cm）。值得注意的是，1 的独特量子阱结构导致了有趣的双光子吸收特性，具有高达 5.76×10cm GW 的巨大非线性光学吸收系数，几乎比大多数传统全无机钙钛矿铁电体大两个数量级。据我们所知，1 是具有巨大双光子吸收系数的混合铁电体的首例。揭示了铁电和双光子吸收的机制。这项工作将为具有双光子吸收的新型铁电体的设计提供启示，并促进它们在光子学应用中的潜力。
