Bis(4-dialkylaminophenyl)heteroarylamino donor chromophores exhibiting exceptional hyperpolarizabilities
Bis(4-dialkylaminophenyl)heteroarylamino donor chromophores exhibiting exceptional hyperpolarizabilities
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DOI：
10.1039/d0tc05700b
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发表时间：
2021-03
影响因子：
6.4
通讯作者：
Huajun Xu;L. Johnson;Yovan de Coene;D. Elder;S. Hammond;K. Clays;L. Dalton;B. Robinson
中科院分区：
文献类型：
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作者：
Huajun Xu;L. Johnson;Yovan de Coene;D. Elder;S. Hammond;K. Clays;L. Dalton;B. Robinson
有机电光（EO）材料纳入硅-有机混合和等离子体-有机混合装置，使新的记录在EO调制性能。我们报道了一系列新的非线性光学生色团工程的理论指导设计，利用双（4-二烷基氨基苯基）杂芳氨基供体部分，大大提高分子的超极化率。通过超瑞利散射测量验证了使用密度泛函理论预测的超极化率，显示出较强的预测/实验一致性和静态超极化率超过最佳先前发色团的>2倍的进步。这些发色团的电场极化薄膜表现出显着增强的EO系数（r33）和极化效率（r33/Ep）在低发色团浓度相比，国家的最先进的发色团，如JRD 1。性能最高的混合物仅含有10wt%的新型发色团BTP 7，与JRD 1相比，每单位浓度的极化效率提高了12倍。我们的研究结果表明，进一步提高发色团的超极化率是可行的，而不会出现不可接受的光学损耗或稳定性的折衷。
Organic electro-optic (EO) materials incorporated into silicon-organic hybrid and plasmonic-organic hybrid devices have enabled new records in EO modulation performance. We report a new series of nonlinear optical chromophores engineered by theory-guided design, utilizing bis(4-dialkylaminophenyl)heteroarylamino donor moieties to greatly enhance molecular hyperpolarizabilities. Hyperpolarizabilities predicted using density functional theory were validated by hyper-Rayleigh scattering measurements, showing strong prediction/experiment agreement and >2-fold advancement in static hyperpolarizability over the best prior chromophores. Electric field poled thin films of these chromophores showed significantly enhanced EO coefficients (r33) and poling efficiencies (r33/Ep) at low chromophore concentrations compared with state-of-the-art chromophores such as JRD1. The highest performing blend, containing just 10 wt% of the novel chromophore BTP7, showed a 12-fold enhancement in poling efficiency per unit concentration vs.JRD1. Our results suggest that further improvement in chromophore hyperpolarizability is feasible without unacceptable tradeoffs with optical loss or stability.