4.7 Article

Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation

Journal

INORGANIC CHEMISTRY
Volume 61, Issue 3, Pages 1797-1804

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c03820

Keywords

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Funding

  1. National Natural Science Foundation of China [21771179, 22175175, 21901246]
  2. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China [2021ZR118]
  3. Natural Science Foundation of Fujian Province [2019J01133]

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In this study, three quaternary rare-earth sulfides were synthesized and one of them exhibited high second-harmonic-generation intensity and laser-induced damage threshold, which is of great significance for the research of infrared nonlinear optical materials.
Multinary rare-earth chalcogenides with d-block transition metals have attracted considerable attention owing to their intriguing structural architectures and promising practical applications. In this work, three quaternary rare-earth sulfides, Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb), have been obtained by the high-temperature solid-state method. These compounds are isostructural and belong to the noncentrosymmetric orthorhombic space group Cmc2(1) (No. 36). The basic structural unit contains unique two-dimensional anionic [RE2Cd3S10](8-) layers, which are separated by Ba2+ cations. Remarkably, Ba4Sm2Cd3S10 exhibits a high second-harmonic-generation intensity (1.8 times that of AgGaS2) and a significantly higher laser-induced damage threshold (14.3 times that of AgGaS2), which is the first case possessing an infrared (IR) nonlinear optical (NLO) property in the quaternary AE/RE/TM/Q (AE = alkaline-earth metals; RE = rare-earth metals; TM = d-block transition metals; and Q = chalcogen) systems. Moreover, theoretical investigations of the structure-property relationship indicate that the combined action of various types of NLO-active units makes the main contribution to the SHG activity. This discovery may shed light on broadening the frontiers of IR-NLO materials.

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