Lopez Diana, Zhou Yinong, Cordova Dmitri Leo Mesoza, Milligan Griffin M, Ogura Kaleolani S, Wu Ruqian, Arguilla Maxx Q
Department of Chemistry, University of California Irvine, Irvine, California 92697, United States.
Department of Physics and Astronomy, University of California Irvine, Irvine, California 92697, United States.
J Am Chem Soc. 2024 Aug 21;146(33):22863-22868. doi: 10.1021/jacs.4c05730. Epub 2024 Aug 8.
The rediscovery of one-dimensional (1D) and quasi-1D (q-1D) van der Waals (vdW) crystals ushered the realization of nascent physical properties in 1D that are suitable for applications in photonics, electronics, and sensing. However, despite renewed interest in the creation and understanding of the physical properties of 1D and q-1D vdW crystals, the lack of accessible synthetic pathways for growing well-defined nanostructures that extend across several length scales remains. Using the highly anisotropic 1D vdW NbS-I crystal as a model phase, we present a catalyst-free and bottom-up synthetic approach to access ultralong nanowires, with lengths reaching up to 7.9 mm and with uniform thicknesses ranging from 13 to 160 nm between individual nanowires. Control over the synthetic parameters enabled the modulation of intra- and interchain growth modalities to selectively yield only 1D nanowires or quasi-2D nanoribbons. Comparative synthetic and density functional theory (DFT) studies with a closely related nondimerized phase, ZrS, show that the unusual preferential growth along 1D can be correlated to the strongly anisotropic bonding and dimeric nature of NbS-I.
一维（1D）和准一维（q-1D）范德华（vdW）晶体的重新发现，使人们认识到一维中适合用于光子学、电子学和传感领域的新物理特性。然而，尽管人们对一维和准一维范德华晶体物理特性的创造和理解重新产生了兴趣，但仍然缺乏可用于生长跨越多个长度尺度的明确纳米结构的合成途径。我们以高度各向异性的一维范德华NbS-I晶体为模型相，提出了一种无催化剂的自下而上的合成方法来制备超长纳米线，其长度可达7.9毫米，单根纳米线之间的均匀厚度在13至160纳米之间。对合成参数的控制能够调节链内和链间的生长模式，从而选择性地仅产生一维纳米线或准二维纳米带。与密切相关的非二聚相ZrS进行的对比合成和密度泛函理论（DFT）研究表明，沿一维方向异常的优先生长可能与NbS-I的强各向异性键合和二聚性质有关。
