Nucleation-Dependent Surface Diffusion in Anisotropic Growth of III–V Nanostructures

IF 3.2 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Crystal Growth & Design Pub Date : 2024-07-25 DOI:10.1021/acs.cgd.4c00723
Vladimir G. Dubrovskii
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Abstract

Vertical growth rate of highly anisotropic III–V nanostructures, including the vapor–liquid–solid or catalyst-free nanowires and quasi-one-dimensional nanomembranes obtained by selective area epitaxy, is largely influenced by surface diffusion of group III adatoms. Here, we present a growth model which is based on the self-consistent calculation of the diffusion flux depending on the nucleation rate on the top facet. It is shown that the magnitude and even the direction of surface diffusion flux is controlled by the position and shape-dependent mononucleation of two-dimensional islands on the top facet of the structures, and is sensitive to the V/III flux ratio during growth. Group III adatoms diffuse from the sidewalls to the top of the structures if the nucleation-mediated growth rate is larger than the direct vapor flux of group III atoms. This “positive” diffusion results in superlinear evolution of height with time. When the nucleation-mediated growth rate is smaller than the direct flux of group III atoms, the direction of the diffusion flux is reversed to “negative”, resulting in sublinear increase of height with time. Positive diffusion usually occurs in symmetrical III–V nanowires, while negative diffusion suppresses selective area growth of elongated GaAs nanomembranes with tapered sidewalls on their short sides. The model sheds more light on the general growth properties of anisotropic nanostructures and should be useful for morphological design of such structures in different epitaxy techniques.

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III-V 纳米结构各向异性生长过程中的成核依赖性表面扩散
高度各向异性的 III-V 族纳米结构(包括气-液-固或无催化剂纳米线以及通过选择性面积外延获得的准一维纳米膜)的垂直生长速率在很大程度上受到 III 族原子表面扩散的影响。在此,我们提出了一个生长模型,该模型基于对顶面成核率的扩散通量的自洽计算。结果表明,表面扩散通量的大小甚至方向都受控于结构顶面二维孤岛的位置和形状,并对生长过程中的 V/III 通量比敏感。如果成核介导的生长速率大于 III 族原子的直接蒸汽通量,III 族原子就会从侧壁扩散到结构顶部。这种 "正 "扩散导致高度随时间的超线性演变。当成核介导的生长率小于 III 族原子的直接通量时,扩散通量的方向就会逆转为 "负",从而导致高度随时间呈亚线性增长。正向扩散通常发生在对称的 III-V 族纳米线中,而负向扩散会抑制短边侧壁呈锥形的细长 GaAs 纳米膜的选择性面积增长。该模型进一步揭示了各向异性纳米结构的一般生长特性,并有助于在不同的外延技术中对此类结构进行形态设计。
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来源期刊
Crystal Growth & Design
Crystal Growth & Design 化学-材料科学:综合
CiteScore
6.30
自引率
10.50%
发文量
650
审稿时长
1.9 months
期刊介绍: The aim of Crystal Growth & Design is to stimulate crossfertilization of knowledge among scientists and engineers working in the fields of crystal growth, crystal engineering, and the industrial application of crystalline materials. Crystal Growth & Design publishes theoretical and experimental studies of the physical, chemical, and biological phenomena and processes related to the design, growth, and application of crystalline materials. Synergistic approaches originating from different disciplines and technologies and integrating the fields of crystal growth, crystal engineering, intermolecular interactions, and industrial application are encouraged.
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