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Peer-reviewedCC BY-NC 3.0Chemical Science

CaM3Si4As11 (M = Ga, In): arsenide infrared nonlinear optical crystals enforced by novel [As2] linear motifs

  • Shusen Yang1
  • Qichao Zhao1
  • Xuemei Shi1
  • Guang Peng1,2
  • Ning Ye1,2
  • Jindong Chen1,2
  1. 1State Key Laboratory of Crystal Materials, Tianjin Key Laboratory of Functional Crystal Materials, Institute of Functional Crystal, College of Materials Science and Engineering, Tianjin University of Technology Tianjin 300384 China
  2. 2Tianjin Key Laboratory of Quantum Optics and Intelligent Photonics, School of Science, Tianjin University of Technology Tianjin 300384 China
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Abstract

Exploration of new arsenide-based infrared (IR) nonlinear optical (NLO) crystals has long been hindered by the narrow band gap limitations and the difficulty of achieving non-centrosymmetric (NCS) structures, despite their promising potential in the long-wave infrared region. By assembling MAs4 (M = Ga, In) tetrahedra and novel [As2] linear motifs, we designed and synthesized two new NCS arsenides, CaM3Si4As11 (M = Ga, In), featuring quasi-T3 M3Si4As11[As2]6 supertetrahedra decorated by [As2] motifs. CGSA and CISA exhibited strong SHG responses (1.7 and 2.5 × ZGP at 2900 nm), wide band gaps among arsenides (1.65 eV and 1.49 eV), broad IR transparency range (cutoff edge up to 12.5 µm), and large birefringence (0.122 and 0.128). Structure–property relationship analyses revealed that the wide band gap originated from the synergistic effect of the high average coordination number of As atoms induced by As–As bonding and the high excitation energy of SiAs4 tetrahedra. Furthermore, the [As2] motifs with highly polarizable π-interactions made a significant contribution to NLO effects and birefringence. This work demonstrates that arsenides with introduced [As2] units are promising systems for long-wave IR NLO materials.

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Cite

BibTeXRIS
BibTeX
@article{yang2026cam3si4as11,
  title = {{CaM3Si4As11 (M = Ga, In): arsenide infrared nonlinear optical crystals enforced by novel [As2] linear motifs}},
  author = {Shusen Yang and Qichao Zhao and Xuemei Shi and Guang Peng and Ning Ye and Jindong Chen},
  journal = {Chemical Science},
  year = {2026},
  month = sep,
  doi = {10.1039/d6sc04910a},
  url = {https://doi.org/10.1039/d6sc04910a},
  note = {CC BY-NC 3.0},
}
RIS
TY  - JOUR
TI  - CaM3Si4As11 (M = Ga, In): arsenide infrared nonlinear optical crystals enforced by novel [As2] linear motifs
AU  - Shusen Yang
AU  - Qichao Zhao
AU  - Xuemei Shi
AU  - Guang Peng
AU  - Ning Ye
AU  - Jindong Chen
PY  - 2026
DA  - 2026/09/10
JO  - Chemical Science
DO  - 10.1039/d6sc04910a
UR  - https://doi.org/10.1039/d6sc04910a
AB  - Exploration of new arsenide-based infrared (IR) nonlinear optical (NLO) crystals has long been hindered by the narrow band gap limitations and the difficulty of achieving non-centrosymmetric (NCS) structures, despite their promising potential in the long-wave infrared region. By assembling MAs4 (M = Ga, In) tetrahedra and novel [As2] linear motifs, we designed and synthesized two new NCS arsenides, CaM3Si4As11 (M = Ga, In), featuring quasi-T3 M3Si4As11[As2]6 supertetrahedra decorated by [As2] motifs. CGSA and CISA exhibited strong SHG responses (1.7 and 2.5 × ZGP at 2900 nm), wide band gaps among arsenides (1.65 eV and 1.49 eV), broad IR transparency range (cutoff edge up to 12.5 µm), and large birefringence (0.122 and 0.128). Structure–property relationship analyses revealed that the wide band gap originated from the synergistic effect of the high average coordination number of As atoms induced by As–As bonding and the high excitation energy of SiAs4 tetrahedra. Furthermore, the [As2] motifs with highly polarizable π-interactions made a significant contribution to NLO effects and birefringence. This work demonstrates that arsenides with introduced [As2] units are promising systems for long-wave IR NLO materials.
SN  - 2041-6520
SN  - 2041-6539
ER  -