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Self-assembled binary multichromophore dendrimers with enhanced electro-optic coefficients and alignment stability†
Materials Chemistry Frontiers ( IF 6.0 ) Pub Date : 2019-09-09 , DOI: 10.1039/c9qm00508k Huajun Xu 1, 2, 3, 4 , Jianpeng Liu 5, 6, 7, 8 , Jun Liu 8, 9, 10, 11, 12 , Canwen Yu 5, 6, 7, 8 , Zhaofen Zhai 5, 6, 7, 8 , Gangzhi Qin 5, 6, 7, 8 , Fenggang Liu 5, 6, 7, 8
Materials Chemistry Frontiers ( IF 6.0 ) Pub Date : 2019-09-09 , DOI: 10.1039/c9qm00508k Huajun Xu 1, 2, 3, 4 , Jianpeng Liu 5, 6, 7, 8 , Jun Liu 8, 9, 10, 11, 12 , Canwen Yu 5, 6, 7, 8 , Zhaofen Zhai 5, 6, 7, 8 , Gangzhi Qin 5, 6, 7, 8 , Fenggang Liu 5, 6, 7, 8
Affiliation
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Novel binary self-assembled electro-optic (EO) dendrimers were developed to maximize the acentric order of chromophores with large hyperpolarizabilities and strong dipole–dipole interactions. To achieve high EO coefficient, a multichromophore dendritic structure and supramolecular self-assembly strategy through π–π stacking of fluoroaromatics and aromatics were adopted to minimize dipole–dipole interaction of the chromophores at high loading density. In these dendrimers, three tetraene chromophores were substituted with an aromatic dendron (HD) or a fluoroaromatic dendron (FD) on the donor ends as the peripheral groups. The neat dendrimer films show excellent film-forming ability and a higher refractive index (n = 1.81 for FDSD and n = 1.86 for HDSD at 1310 nm) compared with guest–host EO polymers (n ≈ 1.6, 1310 nm). Higher n is beneficial for reducing the driving voltage for Mach–Zehnder modulators. By doping a secondary chromophore (HJD, 25 wt%) into neat dendrimers and blending two dendrimers together with 1 : 1 ratio (wt), three kinds of binary EO materials were prepared to afford better EO performance and larger index of refraction without phase separation. Due to supramolecular self-assembly through FD–HD π–π interactions, the poled binary film of 1 : 1 HDSD : FDSD exhibited a very large EO coefficient value up to 289 pm V−1 together with a large refractive index (n = 2.01) at 1310 nm, which represents a very high n3r33 figure-of-merit of 2347 pm V−1 at 1310 nm. Meanwhile, a non-covalently crosslinked network was formed by the HD–FD π–π interactions which afforded an improved long-term alignment stability. After annealing at room temperature for 1000 h, about 97% of the initial r33 values could be still maintained for the poled films of 1 : 1 HDSD : FDSD. The high poling efficiency and temporal EO stability combined with refractive index make them promising candidates for application in photonic devices.
中文翻译：
自组装二元多色团树状聚合物，具有增强的电光系数和排列稳定性†
开发了新型的二元自组装电光（EO）树状聚合物，以最大化具有大超极化性和强偶极-偶极相互作用的生色团的无心顺序。为了获得较高的EO系数，采用了多发色团的树枝状结构和通过氟-芳族化合物和芳族化合物的π-π堆积的超分子自组装策略，以最大程度地降低高负载密度下发色团的偶极-偶极相互作用。在这些树枝状聚合物中，三个四烯生色团被供体端上的芳族树枝状分子（HD）或氟代芳族树枝状分子（FD）取代为外围基团。整齐的树枝状聚合物膜显示出优异的成膜能力和更高的折射率（Ñ = 1.81 FDSD和Ñ= 1.86 HDSD在1310nm）与宾主EO聚合物（比较Ñ ≈1.6，1310纳米）。较高的n有助于降低Mach–Zehnder调制器的驱动电压。通过将次级生色团（HJD，25 wt％）掺杂到纯树状大分子中，并将两种树状大分子以1：1的比例（wt）混合，制备了三种二元EO材料，可提供更好的EO性能和更大的折射率而不发生相分离。由于通过FD-HDπ-π相互作用的超分子自组装，极化的二元膜1：HDSD：FDSD在289 pm V -1处显示出非常大的EO系数值，并且折射率很大（n = 2.01 ）在1310 nm处，代表非常高的n 3 r在1310 nm处的2347 pm V -1的33品质因数。同时，通过HD-FDπ-π相互作用形成了非共价交联网络，从而改善了长期对准稳定性。在室温下退火1000小时后，对于1：1 HDSD：FDSD的极化薄膜，仍可以保持约97％的初始r 33值。高极化效率和暂时的EO稳定性以及折射率使其成为光子器件应用的有希望的候选者。
更新日期：2019-12-19
中文翻译：
自组装二元多色团树状聚合物，具有增强的电光系数和排列稳定性†
开发了新型的二元自组装电光（EO）树状聚合物，以最大化具有大超极化性和强偶极-偶极相互作用的生色团的无心顺序。为了获得较高的EO系数，采用了多发色团的树枝状结构和通过氟-芳族化合物和芳族化合物的π-π堆积的超分子自组装策略，以最大程度地降低高负载密度下发色团的偶极-偶极相互作用。在这些树枝状聚合物中，三个四烯生色团被供体端上的芳族树枝状分子（HD）或氟代芳族树枝状分子（FD）取代为外围基团。整齐的树枝状聚合物膜显示出优异的成膜能力和更高的折射率（Ñ = 1.81 FDSD和Ñ= 1.86 HDSD在1310nm）与宾主EO聚合物（比较Ñ ≈1.6，1310纳米）。较高的n有助于降低Mach–Zehnder调制器的驱动电压。通过将次级生色团（HJD，25 wt％）掺杂到纯树状大分子中，并将两种树状大分子以1：1的比例（wt）混合，制备了三种二元EO材料，可提供更好的EO性能和更大的折射率而不发生相分离。由于通过FD-HDπ-π相互作用的超分子自组装，极化的二元膜1：HDSD：FDSD在289 pm V -1处显示出非常大的EO系数值，并且折射率很大（n = 2.01 ）在1310 nm处，代表非常高的n 3 r在1310 nm处的2347 pm V -1的33品质因数。同时，通过HD-FDπ-π相互作用形成了非共价交联网络，从而改善了长期对准稳定性。在室温下退火1000小时后，对于1：1 HDSD：FDSD的极化薄膜，仍可以保持约97％的初始r 33值。高极化效率和暂时的EO稳定性以及折射率使其成为光子器件应用的有希望的候选者。
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