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<p>The development of electroluminochromic (ELC) materials capable of voltage-controlled emission modulation is crucial for advancing applications. However, achieving this remains challenging due to emission quenching during redox processes. While multi-component systems offer tunable emission, they suffer from complexities associated with intermolecular electron transfer and device architectures. Herein, we report three novel iridium(III) complexes incorporating methylpyridinium pendants, and investigate their electrochemical and photophysical properties. The complexes exhibit reversible pyridinium-based reductions at −0.92 to −1.07 V and irreversible ligand-based reduction at about −1.94 V. Upon photoexcitation, the complexes either remain non-emissive or emit in the near-infrared region. Interestingly, they show unique triple-state ELC performance in devices; twoelectron reduction at −2.3 V triggers orange-red emission, followed by a transition to yellowish-green emission upon increasing the voltage to −3.8 V. High-resolution mass spectrometry and density functional theory calculations indicate that the pyridiniumcontaining ligand undergoes reversible conformational change between twisted and coplanar geometries upon pyridinium-based redox reaction at −2.3 V, and becomes folded geometry upon dimerization at −3.8 V. These voltage-induced structural changes modify the electronic structure of the complexes, leading to remarkable modulation of their emission properties. The triple-state ELC properties of the complexes are utilized in proof-of-concept multicolor information display and encryption devices.</p>

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Triple-state electroluminochromism of iridium(III) complexes through redox-induced geometric transformations for information display and encryption

  • 期刊论文

  • 发表日期：

    2025年6月25日

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  • Xuecheng Wang,
  • Shuzi Wu,
  • Yongheng Wen,
  • Jun Yang,
  • Feiyang Li,
  • Qi Wu,
  • Pengcheng Wu,
  • Zhixin Ji,
  • Kenneth Yin Zhang,
  • Shujuan Liu,
  • Qiang Zhao

摘要

The development of electroluminochromic (ELC) materials capable of voltage-controlled emission modulation is crucial for advancing applications. However, achieving this remains challenging due to emission quenching during redox processes. While multi-component systems offer tunable emission, they suffer from complexities associated with intermolecular electron transfer and device architectures. Herein, we report three novel iridium(III) complexes incorporating methylpyridinium pendants, and investigate their electrochemical and photophysical properties. The complexes exhibit reversible pyridinium-based reductions at −0.92 to −1.07 V and irreversible ligand-based reduction at about −1.94 V. Upon photoexcitation, the complexes either remain non-emissive or emit in the near-infrared region. Interestingly, they show unique triple-state ELC performance in devices; twoelectron reduction at −2.3 V triggers orange-red emission, followed by a transition to yellowish-green emission upon increasing the voltage to −3.8 V. High-resolution mass spectrometry and density functional theory calculations indicate that the pyridiniumcontaining ligand undergoes reversible conformational change between twisted and coplanar geometries upon pyridinium-based redox reaction at −2.3 V, and becomes folded geometry upon dimerization at −3.8 V. These voltage-induced structural changes modify the electronic structure of the complexes, leading to remarkable modulation of their emission properties. The triple-state ELC properties of the complexes are utilized in proof-of-concept multicolor information display and encryption devices.