期刊
ACS NANO
卷 11, 期 2, 页码 1246-1256出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.6b04721
关键词
nanocrystals; perovskite; conductive ligands; epitaxy; photodetectors; optoelectronics; semiconductors
类别
资金
- Aufbruch Bayern initiative of the state of Bavaria
- Osterreichische Forschungsforderungsgesellschaft FFG [843598]
- Austrian Science Fund [FWF-P28167, J3317-N27]
- European Research Council via the EFRE INTERREG IV ETC-AT-CZ program [M00146]
- European Research Council via the Marie-Sklodowska Curie action Phonsi [H2020-MSCA-ITN-642656]
Epitaxial growth techniques enable nearly defect free heterostructures with coherent interfaces, which are of utmost importance for high performance electronic devices. While high-vacuum technology-based growth techniques are state-of-the art, here we pursue a purely solution processed approach to obtain nanocrystals with eptaxially coherent and quasi-lattice matched inorganic ligand shells. Octahedral metal-halide clusters, respectively 0-dimensional perovskites, were employed as ligands to match the coordination geometry of the PbS cubic rock-salt lattice. Different clusters (CH3NH3+)((6-x))[M((x+))Hal(6)]((6-x))-(Mx+ = Pb(II), Bi(III), Mn(II), In(III), Hal = Cl, I) were attached to the nanocrystal surfaces via a scalable phase transfer procedure. The ligand attachment and coherence of the formed PbS/ligand core/shell interface was confirmed by combining the results from transmission electron microscopy, small-angle X-ray scattering, nuclear magnetic resonance spectroscopy and powder X-ray diffraction. The lattice mismatch between ligand shell and nanocrystal core plays a key role in performance. In photoconducting devices the best performance (detectivity of 2 X 10(11) cm Hz (1/2)/W with > 110 kHz bandwidth) was obtained with (CH3NH3)(3)BiI6 ligands, providing the smallest relative lattice mismatch of ca. -1%. PbS nanocrystals with such ligands exhibited in millimeter sized bulk samples in the form of pressed pellets a relatively high carrier mobility for nanocrystal solids of similar to 1.3 cm(2)/(V s), a carrier lifetime of similar to 70 mu s, and a low residual carrier concentration of 2.6 X 10(13) cm(-3). Thus, by selection of ligands with appropriate geometry and bond lengths optimized quasi-epitaxial ligand shells were formed on nanocrystals, which are beneficial for applications in optoelectronics.
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