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Electro-Optic Activity in Excess of 1000 pm V−1 Achieved via Theory-Guided Organic Chromophore Design
Advanced Materials ( IF 27.4 ) Pub Date : 2021-09-20 , DOI: 10.1002/adma.202104174 Huajun Xu 1 , Delwin L Elder 1, 2 , Lewis E Johnson 1, 2 , Yovan de Coene 3 , Scott R Hammond 1, 2 , Wouter Vander Ghinst 3 , Koen Clays 3 , Larry R Dalton 1 , Bruce H Robinson 1
Advanced Materials ( IF 27.4 ) Pub Date : 2021-09-20 , DOI: 10.1002/adma.202104174 Huajun Xu 1 , Delwin L Elder 1, 2 , Lewis E Johnson 1, 2 , Yovan de Coene 3 , Scott R Hammond 1, 2 , Wouter Vander Ghinst 3 , Koen Clays 3 , Larry R Dalton 1 , Bruce H Robinson 1
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High performance organic electro-optic (OEO) materials enable ultrahigh bandwidth, small footprint, and extremely low drive voltage in silicon-organic hybrid and plasmonic-organic hybrid photonic devices. However, practical OEO materials under device-relevant conditions are generally limited to performance of ≈300 pm V−1 (10× the EO response of lithium niobate). By means of theory-guided design, a new series of OEO chromophores is demonstrated, based on strong bis(4-dialkylaminophenyl)phenylamino electron donating groups, capable of EO coefficients (r33) in excess of 1000 pm V−1. Density functional theory modeling and hyper-Rayleigh scattering measurements are performed and confirm the large improvement in hyperpolarizability due to the stronger donor. The EO performance of the exemplar chromophore in the series, BAY1, is evaluated neat and at various concentrations in polymer host and shows a nearly linear increase in r33 and poling efficiency (r33/Ep, Ep is poling field) with increasing chromophore concentration. 25 wt% BAY1/polymer composite shows a higher poling efficiency (3.9 ± 0.1 nm2 V−2) than state-of-the-art neat chromophores. Using a high-ε charge blocking layer with BAY1, a record-high r33 (1100 ± 100 pm V−1) and poling efficiency (17.8 ± 0.8 nm2 V−2) at 1310 nm are achieved. This is the first reported OEO material with electro-optic response larger than thin-film barium titanate.
中文翻译：
通过理论引导的有机发色团设计实现超过 1000 pm V-1 的电光活性
高性能有机电光 (OEO) 材料可在硅-有机杂化和等离子体-有机杂化光子器件中实现超高带宽、小尺寸和极低的驱动电压。然而，设备相关条件下的实际OEO材料通常限于≈300 pm V -1（10倍铌酸锂的EO响应）的性能。通过理论指导设计，展示了一系列基于强双（4-二烷基氨基苯基）苯基氨基给电子基团的新系列 OEO 发色团，能够使 EO 系数 ( r 33 ) 超过 1000 pm V -1. 执行密度泛函理论建模和超瑞利散射测量，并确认由于更强的供体，超极化率的大幅提高。该系列中示例发色团 BAY1 的 EO 性能在聚合物主体中以不同浓度进行评估，显示r 33和极化效率（r 33 /E p，E p是极化场）几乎线性增加发色团浓度。25 wt% BAY1/聚合物复合材料显示出比最先进的纯生色团更高的极化效率（3.9 ± 0.1 nm 2 V -2）。BAY1 使用高 ε 电荷阻挡层，创历史新高r 33 (1100 ± 100 pm V -1 ) 和极化效率 (17.8 ± 0.8 nm 2 V -2 ) 在 1310 nm 处实现。这是第一个报道的光电响应大于薄膜钛酸钡的 OEO 材料。
更新日期：2021-11-09
中文翻译：
通过理论引导的有机发色团设计实现超过 1000 pm V-1 的电光活性
高性能有机电光 (OEO) 材料可在硅-有机杂化和等离子体-有机杂化光子器件中实现超高带宽、小尺寸和极低的驱动电压。然而，设备相关条件下的实际OEO材料通常限于≈300 pm V -1（10倍铌酸锂的EO响应）的性能。通过理论指导设计，展示了一系列基于强双（4-二烷基氨基苯基）苯基氨基给电子基团的新系列 OEO 发色团，能够使 EO 系数 ( r 33 ) 超过 1000 pm V -1. 执行密度泛函理论建模和超瑞利散射测量，并确认由于更强的供体，超极化率的大幅提高。该系列中示例发色团 BAY1 的 EO 性能在聚合物主体中以不同浓度进行评估，显示r 33和极化效率（r 33 /E p，E p是极化场）几乎线性增加发色团浓度。25 wt% BAY1/聚合物复合材料显示出比最先进的纯生色团更高的极化效率（3.9 ± 0.1 nm 2 V -2）。BAY1 使用高 ε 电荷阻挡层，创历史新高r 33 (1100 ± 100 pm V -1 ) 和极化效率 (17.8 ± 0.8 nm 2 V -2 ) 在 1310 nm 处实现。这是第一个报道的光电响应大于薄膜钛酸钡的 OEO 材料。
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