Pb3.5GeS4Br3: the first phase-matching thiogermanate halide infrared nonlinear optical material

Zhou, Jiazheng; Wang, Hongshan; Liu, Junjie; Su, Xin; Chu, Yu; Qu, Jiale; Jiang, Xiangzhan

doi:10.1039/d4qi00293h

Inorg. Chem. Front.

2024

DOI: 10.1039/d4qi00293h

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Pb_3.5GeS₄Br₃: the first phase-matching thiogermanate halide infrared nonlinear optical material

Jiazheng Zhou,

Hongshan Wang,

Junjie Liu

et al.

Abstract: Two new thiohalides Pb3GeS4Br2 and Pb3.5GeS4Br3 have been synthesized by introducing Pb2+ into the thiogermanate system. The compounds crystallize in centrosymmetric P21/c (Pb3GeS4Br2) and non-centrosymmetric P63 (Pb3.5GeS4Br3) space groups, respectively....

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Cited by 4 publications

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Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Bu,

Wu,

et al. 2024

Adv Funct Materials

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Non‐centrosymmetric (NCS) structures are of great importance for the development of symmetry‐dependent functional properties, yet their rational structural design remains a great challenge. Herein, a strategy driven by a highly promising honeycomb structure framework that draws from nature has been proposed for designing three new NCS structures, La4O4(BO3)3·ClSr3 and Sr2Y(BO3)4·XSr3 (X = Cl, Br). They exhibit excellent nonlinear optical (NLO) properties, including strong second‐harmonic‐generation (SHG) responses (2.4–5.4 × KH2PO4 (KDP)), short ultraviolet (UV) cut‐off edges (λcut‐off < 200 nm), and stable physicochemical properties, which make them promising UV NLO crystals. Furthermore, comparing their structures and properties with other compounds in the Gaudefroyite family, it has been found that they all have honeycomb‐like structures. With the continuous modification of their compositions, these structures can achieve not only structural transformation from centrosymmetric (CS) to NCS but also gradual doubling of SHG responses from Ba4(BO3)3X4·XBa3 series (≈1 × KDP) to Sr2Y(BO3)4·XSr3 series (≈2 × KDP) to La4O4(BO3)3·ClSr3 series (≈6 × KDP). Moreover, the ON–OFF of their chiral structures can be achieved through modulating a honeycomb‐like framework and their infilling as observed in La4O4(BO3)3·BrBa3 (P63mc), La4O4(BO3)3·ClSr3 (P63) and Sr2Y(BO3)4·ClSr3 (P63mc). These indicate that honeycomb is an ideal structural template for achieving the design of NCS structures.

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Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Bu,

Wu,

et al. 2024

Adv Funct Materials

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Pb₂TeV₂O₁₀: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups

Ding,

Zhu,

Wang

et al. 2024

Inorg. Chem.

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Birefringent materials as the key materials in laser science and technology have attracted continuous attention due to their ability to modulate polarized light. Herein, a new lead vanadate tellurate, Pb 2 TeV 2 O 10 , has been synthesized through the rational integration of different kinds of birefringence-active functional units. Pb 2 TeV 2 O 10 features a unique two-dimensional (2D) [TeV 2 O 10 ] ∞ layered structure consisting of [VO 6 ] 7− and [TeO 6 ] 6− octahedra, and Pb 2+ cations reside between the [TeV 2 O 10 ] ∞ layers. In addition, the rare edge-sharing mode of [VO 6 ] 7− and [TeO 6 ] 6− octahedra was found in this structure. Attributed to the high polarizability and appropriate arrangement of PbO 8 , VO 6 , and TeO 6 units, Pb 2 TeV 2 O 10 possesses a great theoretical birefringence of 0.275 at 532 nm, which is the largest among the vanadate tellurate family. The spectral tests also prove that Pb 2 TeV 2 O 10 showcases a broad transparency window (439 nm−10 μm), covering an important mid-infrared (IR) atmospheric window (3−5 μm). In addition, in order to improve the transparency, alkali and alkaline earth metal cations were introduced by the substitution strategy, and then the compound K 2 Sr 2 Te 2 O 9 was synthesized. It owns a shorter ultraviolet (UV) cutoff edge of 234 nm and a wider transparency window (234 nm− 13.8 μm). The findings of Pb 2 TeV 2 O 10 and K 2 Sr 2 Te 2 O 9 enrich the structure chemistry of the tellurate family and provide new insights for designing new compounds with large optical anisotropy and wide spectral transparency.

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Pb₆Ba₃Si₂S₈I₁₀: a new thiohalide with a quasi-two-dimensional structure and wide band gap

Zhao,

Zhou,

Wang

et al. 2024

Dalton Trans.

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Pb_3.5GeS₄Br₃: the first phase-matching thiogermanate halide infrared nonlinear optical material

Abstract: Two new thiohalides Pb3GeS4Br2 and Pb3.5GeS4Br3 have been synthesized by introducing Pb2+ into the thiogermanate system. The compounds crystallize in centrosymmetric P21/c (Pb3GeS4Br2) and non-centrosymmetric P63 (Pb3.5GeS4Br3) space groups, respectively....

Cited by 4 publications

References 81 publications

Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Pb₂TeV₂O₁₀: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups

Pb₆Ba₃Si₂S₈I₁₀: a new thiohalide with a quasi-two-dimensional structure and wide band gap

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Pb3.5GeS4Br3: the first phase-matching thiogermanate halide infrared nonlinear optical material

Abstract: Two new thiohalides Pb3GeS4Br2 and Pb3.5GeS4Br3 have been synthesized by introducing Pb2+ into the thiogermanate system. The compounds crystallize in centrosymmetric P21/c (Pb3GeS4Br2) and non-centrosymmetric P63 (Pb3.5GeS4Br3) space groups, respectively....

Cited by 4 publications

References 81 publications

Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

Pb2TeV2O10: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups

Pb6Ba3Si2S8I10: a new thiohalide with a quasi-two-dimensional structure and wide band gap

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Pb_3.5GeS₄Br₃: the first phase-matching thiogermanate halide infrared nonlinear optical material

Pb₂TeV₂O₁₀: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups

Pb₆Ba₃Si₂S₈I₁₀: a new thiohalide with a quasi-two-dimensional structure and wide band gap