超晶格
量子点
外延
材料科学
化学物理
纳米技术
散射
相(物质)
电子衍射
半导体
凝聚态物理
结晶学
衍射
光电子学
化学
图层(电子)
物理
光学
有机化学
作者
Alex Abelson,Caroline Qian,Trenton Salk,Zhongyue Luan,Kevin Fu,Jian‐Guo Zheng,Jenna L. Wardini,Matt Law
标识
DOI:10.1038/s41563-019-0485-2
摘要
Epitaxially fused colloidal quantum dot (QD) superlattices (epi-SLs) may enable a new class of semiconductors that combine the size-tunable photophysics of QDs with bulk-like electronic performance, but progress is hindered by a poor understanding of epi-SL formation and surface chemistry. Here we use X-ray scattering and correlative electron imaging and diffraction of individual SL grains to determine the formation mechanism of three-dimensional PbSe QD epi-SL films. We show that the epi-SL forms from a rhombohedrally distorted body centred cubic parent SL via a phase transition in which the QDs translate with minimal rotation (~10°) and epitaxially fuse across their {100} facets in three dimensions. This collective epitaxial transformation is atomically topotactic across the 103–105 QDs in each SL grain. Infilling the epi-SLs with alumina by atomic layer deposition greatly changes their electrical properties without affecting the superlattice structure. Our work establishes the formation mechanism of three-dimensional QD epi-SLs and illustrates the critical importance of surface chemistry to charge transport in these materials. A structural investigation on the formation of 3D superlattices of colloidal PbSe quantum dots reveals a topotactic transition from the self-assembled phase of ligand-capped quantum dots to the epitaxially fused phase typical of conductive solids.
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