van Overbeek Carlo, Peters Joep L, van Rossum Susan A P, Smits Marc, van Huis Marijn A, Vanmaekelbergh Daniel
Debye Institute for Nanomaterials Science, University of Utrecht, Princetonplein 1, 3584 CC Utrecht, The Netherlands.
J Phys Chem C Nanomater Interfaces. 2018 Jun 14;122(23):12464-12473. doi: 10.1021/acs.jpcc.8b01876. Epub 2018 May 14.
The realization of materials with new optoelectronic properties draws much scientific attention toward the field of nanocrystal superstructures. Low-dimensional superstructures created by interfacial assembly and oriented attachment of PbSe nanocrystals are a striking example because theory showed that PbSe sheets with a honeycomb geometry possess non-trivial flat bands and Dirac cones in the valence and conduction bands. Here, we report on the formation of one-dimensional linear and zigzag structures and two-dimensional (2D) square and honeycomb structures for the entire lead chalcogenide family: PbX (X = S, Se, Te). We observe that PbTe, with a lower bulk melting temperature and enthalpy of formation than those of PbSe, shows a higher nanocrystal surface reactivity, such that the surface must be passivated and the reaction conditions moderated to obtain reasonably ordered superstructures. The present findings constitute a step forward in the realization of a larger family of atomically coherent 2D superstructures with variable IV-VI and II-VI compositions and with electronic properties dictated by the nanogeometry.
具有新型光电特性的材料的实现,引起了科学界对纳米晶体超结构领域的广泛关注。由PbSe纳米晶体的界面组装和定向附着形成的低维超结构就是一个显著的例子,因为理论表明,具有蜂窝几何形状的PbSe薄片在价带和导带中具有非平凡的平带和狄拉克锥。在此,我们报告了整个硫族铅化物家族PbX(X = S、Se、Te)的一维线性和锯齿形结构以及二维(2D)方形和蜂窝状结构的形成。我们观察到,与PbSe相比,PbTe的体相熔化温度和生成焓更低,表现出更高的纳米晶体表面反应活性,因此必须对表面进行钝化处理,并调节反应条件以获得合理有序的超结构。目前的研究结果是实现更大的具有可变IV-VI和II-VI组成且电子特性由纳米几何结构决定的原子相干二维超结构家族的一个进步。