<p>New phenolic organic salt crystals exhibiting large macroscopic second-order optical nonlinearities have been developed. Two molecular anions, 4-bromobenzenesulfonate (BBS) and naphthalene-2-sulfonate (N2S), were incorporated with highly efficient nonlinear optical 2-(4-hydroxy-3-methylstyryl)-1-methylquinolinium (OMQ) cationic chromophores into crystals. Both OMQ-BBS and OMQ-N2S crystals demonstrated second harmonic generation, which confirms their non-centrosymmetric molecular arrangement. Particularly, the OMQ-BBS crystals possess a non-centrosymmetric space group symmetry <i>Cc</i> with a high-order parameter due to a small molecular ordering angle of approximately 21°, resulting in a very large macroscopic second-order nonlinear optical susceptibility, with the effective first hyperpolarizability of about 105 × 10<sup>–30</sup> esu. Furthermore, the non-centrosymmetric crystal phase of the OMQ-BBS crystals exhibits remarkable thermal stability up to its melting temperature of 304&#xa0;°C.</p> Graphical abstract <p>Newly designed phenolic organic styryl salt crystal, 2-(4-hydroxy-3-methylstyryl)-1-methylquinolinium 4-bromobenzenesulfonate (OMQ-BBS), exhibits a large macroscopic second-order nonlinear optical susceptibility (105&#xa0;× 10<sup>-30</sup> esu).</p> <p></p>

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New phenolic organic salt crystals with large optical nonlinearity

  • Yu-Jin Park,
  • Jung-Wook Park,
  • Chaeyoon Kim,
  • Mojca Jazbinsek,
  • Woojin Yoon,
  • Hoseop Yun,
  • Fabian Rotermund,
  • O-Pil Kwon

摘要

New phenolic organic salt crystals exhibiting large macroscopic second-order optical nonlinearities have been developed. Two molecular anions, 4-bromobenzenesulfonate (BBS) and naphthalene-2-sulfonate (N2S), were incorporated with highly efficient nonlinear optical 2-(4-hydroxy-3-methylstyryl)-1-methylquinolinium (OMQ) cationic chromophores into crystals. Both OMQ-BBS and OMQ-N2S crystals demonstrated second harmonic generation, which confirms their non-centrosymmetric molecular arrangement. Particularly, the OMQ-BBS crystals possess a non-centrosymmetric space group symmetry Cc with a high-order parameter due to a small molecular ordering angle of approximately 21°, resulting in a very large macroscopic second-order nonlinear optical susceptibility, with the effective first hyperpolarizability of about 105 × 10–30 esu. Furthermore, the non-centrosymmetric crystal phase of the OMQ-BBS crystals exhibits remarkable thermal stability up to its melting temperature of 304 °C.

Graphical abstract

Newly designed phenolic organic styryl salt crystal, 2-(4-hydroxy-3-methylstyryl)-1-methylquinolinium 4-bromobenzenesulfonate (OMQ-BBS), exhibits a large macroscopic second-order nonlinear optical susceptibility (105 × 10-30 esu).