Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals
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In: ACS nano, Vol. 11.2017, No. 2, 02.2017, p. 1246-1256.
Research output: Contribution to journal › Article › Research › peer-review
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TY - JOUR
T1 - Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals
AU - Sytnykt, Mykhailo
AU - Yakunin, Sergii
AU - Schoefberger, Wolfgang
AU - Lechner, Rainer
AU - Burian, Max
AU - Ludescher, Lukas
AU - Killilea, Niall A.
AU - YousefiAmin, AmirAbbas
AU - Kriegner, Dominik
AU - Stangl, Julian
AU - Groiss, Heiko
AU - Heiss, Wolfgang
PY - 2017/2
Y1 - 2017/2
N2 - 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+)Hal6](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 × 1011 cm Hz 1/2/W with > 110 kHz bandwidth) was obtained with (CH3NH3)3BiI6 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 ∼1.3 cm2/(V s), a carrier lifetime of ∼70 μs, and a low residual carrier concentration of 2.6 × 1013 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.
AB - 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+)Hal6](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 × 1011 cm Hz 1/2/W with > 110 kHz bandwidth) was obtained with (CH3NH3)3BiI6 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 ∼1.3 cm2/(V s), a carrier lifetime of ∼70 μs, and a low residual carrier concentration of 2.6 × 1013 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.
KW - nanocrystals
KW - perovskite
KW - conductive ligands
KW - epitaxy
KW - photodetectors
KW - optoelectronics
KW - semiconductors
U2 - 10.1021/acsnano.6b04721
DO - 10.1021/acsnano.6b04721
M3 - Article
VL - 11.2017
SP - 1246
EP - 1256
JO - ACS nano
JF - ACS nano
SN - 1936-0851
IS - 2
ER -