Scholarlink

<p>In this study, a series of novel chromophores based on cyclopentadienyl furan-fused (CpFu) conjugated bridges with strong push-pull effects were designed, and their nonlinear optical properties were systematically investigated. This work pioneers the exploration of the control mechanism of nonlinear optical properties in double-stranded ladder-type heteroaromatic chromophores through strategic control of cyclopentadiene/furan ring parameters, acceptor strength, and dielectric environment on the conjugated bridge using multiple advanced research approaches. The fundamental correlation between aromaticity, resonance hybrid states, nonlinear optical performance and excited-state characteristics in new CpFu-type double-stranded heterocyclic π-system was established‌. The results revealed that increasing the number of furan rings on the CpFu-type conjugated bridge significantly enhances chromophore aromaticity and effectively tunes the resonance hybrid state from charge-separated to neutral resonance forms, thereby causing the β<sub>prj</sub> value to undergo a sharp transition from negative to highly positive‌. Thus, DN-CpFu5-AS and DN-CpFu3-AO achieved remarkable β<sub>prj</sub> values of 4001.3✕10<sup>-30</sup> esu and 3331.6✕10<sup>-30</sup> esu in chloroform solvent, respectively. Through synergistic application of DOS analysis, hole-electron analysis, and TSM analysis, this study elucidated the influence mechanisms of various resonance hybrid states in CpFu-type chromophores on charge transfer processes, electron backflow, transition dipole moment squared, and dipole moment differences during excitation from ground to crucial states. Beyond being promising high-performance nonlinear optical materials, the innovative CpFu-type conjugated bridge chromophores allow comprehensive investigation of resonance hybrid state effects on nonlinear optical performance in double-stranded heteroaromatic systems. Such insights are essential for building quantitative high-throughput prediction models for double-stranded ladder-type aromatic conjugated frameworks.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Resonance hybrid state in novel cyclopentadienyl furan-fused systems: a key determinant for nonlinear optical properties optimization

  • 期刊论文

  • 发表日期：

    2026年3月3日

查看全文
  • Hejing Sun

摘要

In this study, a series of novel chromophores based on cyclopentadienyl furan-fused (CpFu) conjugated bridges with strong push-pull effects were designed, and their nonlinear optical properties were systematically investigated. This work pioneers the exploration of the control mechanism of nonlinear optical properties in double-stranded ladder-type heteroaromatic chromophores through strategic control of cyclopentadiene/furan ring parameters, acceptor strength, and dielectric environment on the conjugated bridge using multiple advanced research approaches. The fundamental correlation between aromaticity, resonance hybrid states, nonlinear optical performance and excited-state characteristics in new CpFu-type double-stranded heterocyclic π-system was established‌. The results revealed that increasing the number of furan rings on the CpFu-type conjugated bridge significantly enhances chromophore aromaticity and effectively tunes the resonance hybrid state from charge-separated to neutral resonance forms, thereby causing the βprj value to undergo a sharp transition from negative to highly positive‌. Thus, DN-CpFu5-AS and DN-CpFu3-AO achieved remarkable βprj values of 4001.3✕10-30 esu and 3331.6✕10-30 esu in chloroform solvent, respectively. Through synergistic application of DOS analysis, hole-electron analysis, and TSM analysis, this study elucidated the influence mechanisms of various resonance hybrid states in CpFu-type chromophores on charge transfer processes, electron backflow, transition dipole moment squared, and dipole moment differences during excitation from ground to crucial states. Beyond being promising high-performance nonlinear optical materials, the innovative CpFu-type conjugated bridge chromophores allow comprehensive investigation of resonance hybrid state effects on nonlinear optical performance in double-stranded heteroaromatic systems. Such insights are essential for building quantitative high-throughput prediction models for double-stranded ladder-type aromatic conjugated frameworks.