Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals

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Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals. / Sytnykt, Mykhailo; Yakunin, Sergii; Schoefberger, Wolfgang et al.
In: ACS nano, Vol. 11.2017, No. 2, 02.2017, p. 1246-1256.

Research output: Contribution to journalArticleResearchpeer-review

Harvard

Sytnykt, M, Yakunin, S, Schoefberger, W, Lechner, R, Burian, M, Ludescher, L, Killilea, NA, YousefiAmin, A, Kriegner, D, Stangl, J, Groiss, H & Heiss, W 2017, 'Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals', ACS nano, vol. 11.2017, no. 2, pp. 1246-1256. https://doi.org/10.1021/acsnano.6b04721

APA

Sytnykt, M., Yakunin, S., Schoefberger, W., Lechner, R., Burian, M., Ludescher, L., Killilea, N. A., YousefiAmin, A., Kriegner, D., Stangl, J., Groiss, H., & Heiss, W. (2017). Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals. ACS nano, 11.2017(2), 1246-1256. https://doi.org/10.1021/acsnano.6b04721

Vancouver

Sytnykt M, Yakunin S, Schoefberger W, Lechner R, Burian M, Ludescher L et al. Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals. ACS nano. 2017 Feb;11.2017(2):1246-1256. doi: 10.1021/acsnano.6b04721

Author

Sytnykt, Mykhailo ; Yakunin, Sergii ; Schoefberger, Wolfgang et al. / Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals. In: ACS nano. 2017 ; Vol. 11.2017, No. 2. pp. 1246-1256.

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@article{d49977c5d3d148f3bac3b7073bdce180,
title = "Quasi-epitaxial Metal-Halide Perovskite Ligand Shells on PbS Nanocrystals",
abstract = "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.",
keywords = "nanocrystals, perovskite, conductive ligands, epitaxy, photodetectors, optoelectronics, semiconductors",
author = "Mykhailo Sytnykt and Sergii Yakunin and Wolfgang Schoefberger and Rainer Lechner and Max Burian and Lukas Ludescher and Killilea, {Niall A.} and AmirAbbas YousefiAmin and Dominik Kriegner and Julian Stangl and Heiko Groiss and Wolfgang Heiss",
year = "2017",
month = feb,
doi = "10.1021/acsnano.6b04721",
language = "English",
volume = "11.2017",
pages = "1246--1256",
journal = "ACS nano",
issn = "1936-0851",
publisher = "American Chemical Society",
number = "2",

}

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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 -