Enhanced Carrier Transport in Strongly Coupled, Epitaxially Fused CdSe Nanocrystal Solids
Qinghua Zhao, Guillaume Gouget, Jiacen Guo, Shengsong Yang, Tianshuo Zhao, Daniel B. Straus, Chengyang Qian, Nuri Oh, Han Wang, Christopher B. Murray, Cherie R. Kagan
Abstract
Strongly coupled, epitaxially fused colloidal nanocrystal (NC) solids are promising solution-processable semiconductors to realize optoelectronic devices with high carrier mobilities. Here, we demonstrate sequential, solid-state cation exchange reactions to transform epitaxially connected PbSe NC thin films into Cu2Se nanostructured thin-film intermediates and then successfully to achieve zinc-blende, CdSe NC solids with wide epitaxial necking along {100} facets. Transient photoconductivity measurements probe carrier transport at nanometer length scales and show a photoconductance of 0.28(1) cm2 V–1 s–1, the highest among CdSe NC solids reported. Atomic-layer deposition of a thin Al2O3 layer infiltrates and protects the structure from fusing into a polycrystalline thin film during annealing and further improves the photoconductance to 1.71(5) cm2 V–1 s–1 and the diffusion length to 760 nm. We fabricate field-effect transistors to study carrier transport at micron length scales and realize high electron mobilities of 35(3) cm2 V–1 s–1 with on–off ratios of 106 after doping.