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<p>Nonlinear optical (NLO) and birefringent crystals are pivotal for advancing photonic technologies, enabling critical functions from laser frequency conversion to quantum information processing. To address the pressing need for miniaturized devices with enhanced optical anisotropy, we strategically select 5-hydroxy-2-pyridinecarboxylic acid (C<sub>6</sub>H<sub>5</sub>NO<sub>3</sub>), a low-toxicity, cost-effective organic molecule featuring a pyridine-derived <i>π</i>-conjugated system marginally expanded beyond benzene, as NLO functional motif. This molecular design incorporates dual-functional OH/COOH groups that synergistically extend <i>π</i>-delocalization within the planar six-membered ring and provide two anionic states ([C<sub>6</sub>H<sub>4</sub>NO<sub>3</sub>]<sup>−</sup> and [C<sub>6</sub>H<sub>3</sub>NO<sub>3</sub>]<sup>2−</sup>), facilitating diverse supramolecular assemblies with alkali/alkalineearth metal ions. Through confined assembly optimization, we discovered a crystal Na<sub>2</sub>(C<sub>6</sub>H<sub>3</sub>NO<sub>3</sub>)·H<sub>2</sub>O, which achieves an excellent ultraviolet (UV) NLO performance: phase-matched second harmonic generation (SHG) intensity (14.0 × KH<sub>2</sub>PO<sub>4</sub> (KDP) at 1064 nm, the highest among planar mono-six-membered-ring systems), giant birefringence (0.487 at 546 nm), and a UV cutoff edge (321 nm). Multimodal analyses confirm the planar organic anion [C<sub>6</sub>H<sub>3</sub>NO<sub>3</sub>]<sup>2−</sup> as the origin of these exceptional optical responses, where ionic bonding and N–O/N layer confinement enforce optimal alignment.</p>

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Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Chunmei Huang,
  • Xuan Pang,
  • Fuming Li,
  • Shumei Cao,
  • Shilie Pan,
  • Miriding Mutailipu

摘要

Nonlinear optical (NLO) and birefringent crystals are pivotal for advancing photonic technologies, enabling critical functions from laser frequency conversion to quantum information processing. To address the pressing need for miniaturized devices with enhanced optical anisotropy, we strategically select 5-hydroxy-2-pyridinecarboxylic acid (C6H5NO3), a low-toxicity, cost-effective organic molecule featuring a pyridine-derived π-conjugated system marginally expanded beyond benzene, as NLO functional motif. This molecular design incorporates dual-functional OH/COOH groups that synergistically extend π-delocalization within the planar six-membered ring and provide two anionic states ([C6H4NO3]− and [C6H3NO3]2−), facilitating diverse supramolecular assemblies with alkali/alkalineearth metal ions. Through confined assembly optimization, we discovered a crystal Na2(C6H3NO3)·H2O, which achieves an excellent ultraviolet (UV) NLO performance: phase-matched second harmonic generation (SHG) intensity (14.0 × KH2PO4 (KDP) at 1064 nm, the highest among planar mono-six-membered-ring systems), giant birefringence (0.487 at 546 nm), and a UV cutoff edge (321 nm). Multimodal analyses confirm the planar organic anion [C6H3NO3]2− as the origin of these exceptional optical responses, where ionic bonding and N–O/N layer confinement enforce optimal alignment.