Meng Lingyao, Duwal Sakun, Lane J Matthew D, Ao Tommy, Stoltzfus Brian, Knudson Marcus, Park Changyong, Chow Paul, Xiao Yuming, Fan Hongyou, Qin Yang
Center for Micro-Engineered Materials, University of New Mexico, Albuquerque, New Mexico 87131, United States.
Sandia National Laboratories, Albuquerque, New Mexico 87123, United States.
J Am Chem Soc. 2021 Feb 24;143(7):2688-2693. doi: 10.1021/jacs.0c13350. Epub 2021 Feb 12.
We report here pressure induced nanocrystal coalescence of ordered lead chalcogenide nanocrystal arrays into one-dimensional (1D) and 2D nanostructures. In particular, atomic crystal phase transitions and mesoscale coalescence of PbS and PbSe nanocrystals have been observed and monitored in situ respectively by wide- and small-angle synchrotron X-ray scattering techniques. At the atomic scale, both nanocrystals underwent reversible structural transformations from cubic to orthorhombic at significantly higher pressures than those for the corresponding bulk materials. At the mesoscale, PbS nanocrystal arrays displayed a superlattice transformation from face-centered cubic to lamellar structures, while no clear mesoscale lattice transformation was observed for PbSe nanocrystal arrays. Intriguingly, transmission electron microscopy showed that the applied pressure forced both spherical nanocrystals to coalesce into single crystalline 2D nanosheets and 1D nanorods. Our results confirm that pressure can be used as a straightforward approach to manipulate the interparticle spacing and engineer nanostructures with specific morphologies and, therefore, provide insights into the design and functioning of new semiconductor nanocrystal structures under high-pressure conditions.
我们在此报告了压力诱导有序硫属铅化物纳米晶体阵列的纳米晶体聚结,形成一维(1D)和二维(2D)纳米结构。具体而言,分别通过广角和小角同步加速器X射线散射技术原位观察和监测了PbS和PbSe纳米晶体的原子晶体相变和中尺度聚结。在原子尺度上,两种纳米晶体在比相应块体材料显著更高的压力下都经历了从立方到正交晶系的可逆结构转变。在中尺度上,PbS纳米晶体阵列显示出从面心立方到层状结构的超晶格转变,而对于PbSe纳米晶体阵列未观察到明显的中尺度晶格转变。有趣的是,透射电子显微镜显示施加的压力迫使两种球形纳米晶体聚结成单晶二维纳米片和一维纳米棒。我们的结果证实,压力可作为一种直接的方法来操纵粒子间间距并设计具有特定形态的纳米结构,因此,为高压条件下新型半导体纳米晶体结构的设计和功能提供了见解。