以 DNA 分子为模板的 ZnxCd1-xS 和 Cu:ZnxCd1-xS 的结构和光学特性

Andres Aldana, Andrew Houlton, Benjamin R Horrocks
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摘要

一维 ZnxCd1-xS 和 Cu:以 DNA 为模板制备了 ZnxCd1-xS 纳米结构,以促进其沿分子轴生长。利用 X 射线衍射和拉曼光谱验证了具有立方锌混合型结构的均匀合金纳米晶体的形成。X 射线光发射光谱显示,在掺杂的 Cu:ZnxCd1-xS纳米晶体中存在Cu(I)。原子力显微镜(AFM)和电子显微镜(TEM)证明了 DNA 模板引导半导体在一维生长的有效性。纳米结构呈现颗粒状形态,由平均直径为 14 nm 的纳米颗粒组成,这些颗粒由尺寸为 2.0 nm 的较小晶体组装而成。通过蒸发诱导的自组装,获得了平均直径为 48 纳米、长度达数百微米的绳状集合体。紫外可见吸收光谱和发射光谱显示,通过改变 Zn/Cd 前体的摩尔比,可以精确控制 DNA 微型纳米晶体的光带隙(2.89-4.00eV)和光致发光峰(608-819 nm)。掺入 Cu(I)可提高光致发光强度,并产生 0.23 eV 的红移,这与成分无关。制备以 DNA 为模板的 ZnxCd1-xS 和 Cu:ZnxCd1-xS 的制备提供了一种简单的低温路线,可制备出具有可控光隙的无机材料水分散体。
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Structure and optical properties of ZnxCd1-xS and Cu:ZnxCd1-xS templated on DNA molecules
One-dimensional ZnxCd1−xS and Cu: Zn x Cd1−x S nanostructures were prepared using DNA as a template to promote growth along the molecular axis. The formation of homogeneously alloyed nanocrystals with cubic zinc blende-type structures was verified using x-ray diffraction and Raman spectroscopy. X-ray photoemission spectra revealed the presence of Cu(I) in the doped Cu: Zn x Cd1−x S nanocrystals. The effectiveness of the DNA template to direct the semiconductor growth in one dimension was demonstrated by AFM and TEM. The nanostructures displayed a granular morphology comprising nanoparticles with an average diameter of 14 nm composed of assemblies of smaller crystallites of 2.0 nm in size. Rope-like assemblies with an average diameter of 48 nm and extending in length to several hundred micrometres were obtained by evaporation-induced self-assembly. UV-Vis absorption and emission spectra indicated that the optical bandgaps (2.89–4.00eV) and photoluminescence peaks (608–819 nm) of the DNA-templated nanocrystals could be precisely controlled by modifying the molar ratios of their Zn/Cd precursors. Doping with Cu(I) gave an increase in photoluminescence intensity and a composition-independent red-shift of 0.23 eV. The preparation of DNA-templated Zn x Cd1−x S and Cu: Zn x Cd1−x S provides a simple, low-temperature route to aqueous dispersions of inorganic materials with controlled optical gap.
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