Self-Assembly of Chiral Nanoparticles into Semiconductor Helices with Tunable near-Infrared Optical Activity,Chemistry of Materials

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Self-Assembly of Chiral Nanoparticles into Semiconductor Helices with Tunable near-Infrared Optical Activity
Chemistry of Materials ( IF 7.2 ) Pub Date : 2019-12-31 , DOI: 10.1021/acs.chemmater.9b04143
Jiao Yan _{1,

2} , Wenchun Feng ₃ , Ji-Young Kim , Jun Lu , Prashant Kumar , Zhengzhi Mu ₄ , Xiaochun Wu ₁ , Xiaoming Mao , Nicholas A. Kotov

Affiliation

Unique optical, electrical, and mechanical properties of continuous semiconductor helices with nanoscale and mesoscale dimensions represent a previously unexplored materials platform for various applications requiring near-infrared (NIR) optical activity. However, current methods of their synthesis limit the spectrum of chiral geometries, charge transport, and spectral response. Furthermore, the requirements of nearly perfect enantioselectivity, high uniformity, and high yield need to be attained as well. Here, we show that continuous semiconductor helices with tunable spectral response and high monodispersity can be made via self-assembly of semiconductor nanoparticles (NPs). Unraveling the interdependent effects of solvent, pH, ligand density, and coordination bridges between NPs allowed us to maximize the chiral bias for face-to-face particle–particle interactions, control of the geometry of the helices, and increase assembly efficiency by 3 orders of magnitude. The self-limiting nature of NP association results in consistency of their geometries over the entire synthetic ensemble. The helices show chiroptical activity across a broad range of wavelengths from 300 to 1300 nm, and the maximum/sign of their polarization rotation in NIR part can be modulated by varying their pitch. The method described in this study can be extended to chiral semiconductor materials from a variety of other NPs and their combinations.

中文翻译：

手性纳米粒子自组装成具有可调近红外光学活性的半导体螺旋

具有纳米和中尺度尺寸的连续半导体螺旋的独特光学，电学和机械性能代表了以前未开发的材料平台，可用于需要近红外（NIR）光学活性的各种应用。但是，当前的合成方法限制了手性几何结构的光谱，电荷传输和光谱响应。此外，还需要达到近乎完美的对映选择性，高均匀性和高产率的要求。在这里，我们表明可以通过半导体纳米粒子（NPs）的自组装制备具有可调光谱响应和高单分散性的连续半导体螺旋。揭示溶剂，pH，配体密度，NP之间的配位桥使我们能够最大程度地提高手性，以面对面地进行粒子间相互作用，控制螺旋的几何形状，并将组装效率提高3个数量级。NP关联的自限制性质导致其几何形状在整个合成集合中保持一致。螺旋线在300至1300 nm的宽波长范围内均显示出整脊活性，并且可以通过改变其螺距来调节其近红外部分的偏振旋转的最大/正负号。本研究中描述的方法可以扩展到来自多种其他NP及其组合的手性半导体材料。NP关联的自限制性质导致其几何形状在整个合成集合中保持一致。螺旋线在300至1300 nm的宽波长范围内均显示出整脊活性，并且可以通过改变其螺距来调节其近红外部分的偏振旋转的最大/正负号。本研究中描述的方法可以扩展到来自多种其他NP及其组合的手性半导体材料。NP关联的自限制性质导致其几何形状在整个合成集合中保持一致。螺旋线在300至1300 nm的宽波长范围内均显示出整脊活性，并且可以通过改变其螺距来调节其近红外部分的偏振旋转的最大/正负号。本研究中描述的方法可以扩展到来自多种其他NP及其组合的手性半导体材料。

更新日期：2019-12-31

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