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<p>Nonlinear optical (NLO) materials enable direct second-harmonic generation (SHG) of coherent ultraviolet (UV) light, yet achieving phase matching (PM) in systems dominated by non-π-conjugated units remains a critical bottleneck. Herein, we present the first rare-earth nitrate sulfamate, La(SO<sub>3</sub>NH<sub>2</sub>)<sub>2</sub>NO<sub>3</sub>·H<sub>2</sub>O, designed through synergistic anion engineering by integrating La<sup>3+</sup> with π-conjugated [NO<sub>3</sub>] units and heteroleptic tetrahedra [SO<sub>3</sub>NH<sub>2</sub>]. This crystal achieves a short PM wavelength (258 nm) and UV cutoff edge (234 nm), a large SHG response (1 × KH<sub>2</sub>PO<sub>4</sub>), and a record birefringence (0.077@546 nm), overcoming the transparency-anisotropy-SHG response trade-offs in inorganic sulfamate-based materials. The results demonstrate that the heteroleptic tetrahedra [SO<sub>3</sub>NH<sub>2</sub>] play a key role in modulating the band gap of La(SO<sub>3</sub>NH<sub>2</sub>)<sub>2</sub>NO<sub>3</sub>·H<sub>2</sub>O, while the (d-p)π interaction between the La and [NO<sub>3</sub>] units further enhances optical anisotropy. Our work establishes synergistic anion engineering as a paradigm for developing high-performance UV NLO materials through a rational combination of heteroleptic tetrahedra and π-conjugated motifs.</p>

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La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics

  • 期刊论文

  • 发表日期：

    2025年8月8日

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  • Huan Zhou,
  • Meng Cheng,
  • Shilie Pan,
  • Zhihua Yang

摘要

Nonlinear optical (NLO) materials enable direct second-harmonic generation (SHG) of coherent ultraviolet (UV) light, yet achieving phase matching (PM) in systems dominated by non-π-conjugated units remains a critical bottleneck. Herein, we present the first rare-earth nitrate sulfamate, La(SO3NH2)2NO3·H2O, designed through synergistic anion engineering by integrating La3+ with π-conjugated [NO3] units and heteroleptic tetrahedra [SO3NH2]. This crystal achieves a short PM wavelength (258 nm) and UV cutoff edge (234 nm), a large SHG response (1 × KH2PO4), and a record birefringence (0.077@546 nm), overcoming the transparency-anisotropy-SHG response trade-offs in inorganic sulfamate-based materials. The results demonstrate that the heteroleptic tetrahedra [SO3NH2] play a key role in modulating the band gap of La(SO3NH2)2NO3·H2O, while the (d-p)π interaction between the La and [NO3] units further enhances optical anisotropy. Our work establishes synergistic anion engineering as a paradigm for developing high-performance UV NLO materials through a rational combination of heteroleptic tetrahedra and π-conjugated motifs.