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Issue 9, 2017
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Na2CdGe2Q6 (Q = S, Se): two metal-mixed chalcogenides with phase-matching abilities and large second-harmonic generation responses

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Abstract

In view of their inherent defects for commercial infrared nonlinear optical (IR NLO) materials, exploration for new IR NLO materials with excellent performance is an imperative and meaningful work. Herein, we report the successful design and synthesis of two metal-mixed chalcogenides containing divalent cations with d10 electronic configuration: Na2CdGe2S6 and Na2CdGe2Se6. Both of them crystallize in the polar Cc space group and exhibit three-dimensional tunnel structures constructed by the CdQ4 tetrahedra and [GeQ3]n chains with Na+ located in the tunnels. Furthermore, an interesting space group transformation between the monoclinic (Cc) and tetragonal (I4/mcm) systems from Na2CdGe2Se6 to Na2ZnGe2Se6 was discovered, which may arise from the different connection types of their building blocks (more flexible corner-sharing type in Cc while tightly edge-sharing type in I4/mcm). Remarkably, they exhibit type-I phase-matching abilities and large second harmonic generation (SHG) responses (0.8 and 2 times that of benchmark AgGaS2 at 2.09 μm fundamental light). Notably, Na2CdGe2S6 satisfies the essential requirements (coexistence of large NLO response and high laser damage threshold) as one excellent IR NLO material. The structure–property relationship has also been investigated through theoretical calculations and the results indicate that the origin of their NLO effects can be attributed to CdQ4 and GeQ4 units.

Graphical abstract: Na2CdGe2Q6 (Q = S, Se): two metal-mixed chalcogenides with phase-matching abilities and large second-harmonic generation responses

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Publication details

The article was received on 10 Jan 2017, accepted on 25 Jan 2017 and first published on 25 Jan 2017


Article type: Paper
DOI: 10.1039/C7DT00087A
Dalton Trans., 2017,46, 2778-2784

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    Na2CdGe2Q6 (Q = S, Se): two metal-mixed chalcogenides with phase-matching abilities and large second-harmonic generation responses

    G. Li, Q. Liu, K. Wu, Z. Yang and S. Pan, Dalton Trans., 2017, 46, 2778
    DOI: 10.1039/C7DT00087A

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