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Heterometallic Ge-O-Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared
Cihai Hong1, Aoge Yao2, Chunlan Tang1,3
1Institute of Chemical Materials, China Academy of Engineering Physics, Mianyang621900, P. R. China.
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Developing infrared (IR) nonlinear optical (NLO) materials that combine strong frequency-conversion capability with sufficiently wide band gaps remains a significant challenge. Herein, two new heterometallic oxychalcogenides, Sr3GeSnO4Q3 (Q = S, Se), were successfully designed and synthesized. Both compounds crystallize in the noncentrosymmetric space group R3m. Their structures are characterized by highly polarized heterometallic [GeSnO4Q3] dimers, formed by the corner-sharing of [GeO4] and [SnOQ3] tetrahedra through a Ge-O-Sn bridge. Diffuse reflectance measurements reveal wide band gaps of 3.20 and 2.90 eV for Sr3GeSnO4S3 and Sr3GeSnO4Se3, respectively, while powder second-harmonic-generation (SHG) measurements at 2090 nm give responses of 0.34 × AgGaS2 and 0.23 × AgGaS2, respectively. Theoretical calculations indicate that the NLO response is mainly governed by heterometallic [GeSnO4Q3] (Q = S, Se) dimers, in which the Ge-O-Sn oxy bridge plays a significant role in achieving regulation between heteroanion coordination and Ge/Sn heterometallic polarization. This work demonstrates that the heterometallic oxy-bridged [GeSnO4Q3] dimers can serve as effective basic building blocks, providing a useful approach for exploring new functional oxychalcogenides.
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