Journal
INORGANIC CHEMISTRY
Volume 60, Issue 13, Pages 10038-10046Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c01359
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Funding
- Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China [2021ZR118]
- National Natural Science Foundation of China [21771179, 21901246]
- Natural Science Foundation of Fujian Province [2019J01133]
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Three new non-centrosymmetric chalcogenides with strong second harmonic generation responses and high laser-induced damage thresholds have been successfully synthesized. Structural analysis and theoretical calculations reveal the relationship between NCS structures and NLO properties, providing effective solutions for overcoming technical challenges in IR-NLO materials.
Despite the fact that nonlinear optical (NLO) crystals such as AgGaS2 and AgGaSe2 have been widely used in the infrared (IR) range due to their large second harmonic generation (SHG) coefficients and wide range of IR transparency windows, the small laser-induced damage threshold (LIDT) remains a great issue hindering their high-power applications. Herein, three non-centrosymmetric (NCS) chalcogenides AZn(4)Ga(5)Se(12) (A = K, Rb, or Cs) are successfully obtained through an appropriate flux method after the extensive design and synthesis of the A/Zn/Ga/Q system. Single-crystal X-ray diffraction data demonstrate that they adopt trigonal space group R3 (No. 146) with three-dimensional diamond-like frameworks composed of [M9Se24] layers (M = Zn or Ga) stacking in the same direction and filled by charge-balancing A(+) cations. Noticeably, they all exhibit strong powder SHG responses (2.8-3.7 x AgGaS2) and amazing LIDTs (19.2-23.4 x AgGaS2). In addition, theoretical calculations are performed to further determine the relationship between NCS structures and NLO properties. This work provides effective solutions for overcoming the trade-off between strong SHG and high LIDT in IR-NLO materials.
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