Abstract
Second-harmonic generation (SHG) is one of the outstanding properties for practical applications. However, the great majority of molecular ferroelectric materials have very low nonlinear optical coefficients, attenuating their attractive performance. Here we synthesized (4-amino-2-bromopyridinium)(4-amino-2-bromopyridine)tetrafluoroborate (1), whose second-order nonlinear optical coefficient reaches up to 2.56 pm V(-1), 2.67 times of that of KDP, and (4-amino-2-bromopyridinium)tetrafluoroborate (2), possessing a more incredible large second-order nonlinear optical coefficient as high as 10.24 pm V(-1), 10.67 times that of KDP. The compound 1 undergoes two reversible phase transitions at around T1 = 244.1 K and T2 = 154.6 K, caused by dramatic changes of the protonated cations and order-disorder of anions, which was disclosed by differential scanning calorimetry, heat capacity, dielectric anomalies, SHG, and single-crystal X-ray diffraction analysis. The pyroelectric measurements reveal that compound 1 is a Rochelle salt type ferroelectric, which has a large spontaneous polarization of about 3 μC/cm(2).
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