Journal of the American Chemical Society, volume 137, issue 5, pages 1862-1874

Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry

Loredana Protesescu ^{1, 2}

Maarten Nachtegaal ³

Oleksandr Voznyy ⁴

Olga Borovinskaya ¹

Aaron J. Rossini ⁵

Lyndon Emsley ⁵

Christophe Copéret ¹

D. Günther ¹

Edward H Sargent ⁴

Maksym V. Kovalenko ^{1, 2}

Hide authors affiliations Show authors affiliations: 5 affiliations

Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, Zurich CH-8093, Switzerland |

Empa-Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, Dübendorf CH-8600, Switzerland |

Paul Scherrer Institute, 5232 Villigen PSI, Switzerland |

⁴

Department of Electrical and Computer Engineering, University of Toronto, 10 King’s College Road, Toronto, Ontario M5S 3G4, Canada |

⁵

Centre de RMN à Trés Hauts Champs, Institut de Sciences Analytiques (CNRS/ENS Lyon/UCB Lyon 1), Université de Lyon, 69100 Villeurbanne, France |

Publication type: Journal Article

Publication date: 2015-01-29

American Chemical Society (ACS)

Journal: Journal of the American Chemical Society

Quartile SCImago

Quartile WOS

Impact factor: 15

ISSN: 00027863, 15205126

DOI: 10.1021/ja510862c

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General Chemistry

Catalysis

Biochemistry

Colloid and Surface Chemistry

Abstract

Colloidal semiconductor nanocrystals (NCs) are widely studied as building blocks for novel solid-state materials. Inorganic surface functionalization, used to displace native organic capping ligands from NC surfaces, has been a major enabler of electronic solid-state devices based on colloidal NCs. At the same time, very little is known about the atomistic details of the organic-to-inorganic ligand exchange and binding motifs at the NC surface, severely limiting further progress in designing all-inorganic NCs and NC solids. Taking thiostannates (K4SnS4, K4Sn2S6, K6Sn2S7) as typical examples of chalcogenidometallate ligands and oleate-capped CdSe NCs as a model NC system, in this study we address these questions through the combined application of solution (1)H NMR spectroscopy, solution and solid-state (119)Sn NMR spectroscopy, far-infrared and X-ray absorption spectroscopies, elemental analysis, and by DFT modeling. We show that through the X-type oleate-to-thiostannate ligand exchange, CdSe NCs retain their Cd-rich stoichiometry, with a stoichiometric CdSe core and surface Cd adatoms serving as binding sites for terminal S atoms of the thiostannates ligands, leading to all-inorganic (CdSe)core[Cdm(Sn2S7)yK(6y-2m)]shell (taking Sn2S7(6-) ligand as an example). Thiostannates SnS4(4-) and Sn2S7(6-) retain (distorted) tetrahedral SnS4 geometry upon binding to NC surface. At the same time, experiments and simulations point to lower stability of Sn2S6(4-) (and SnS3(2-)) in most solvents and its lower adaptability to the NC surface caused by rigid Sn2S2 rings.

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American Chemical Society (ACS)	American Chemical Society (ACS), 22, 44% American Chemical Society (ACS) 22 publications, 44%
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American Association for the Advancement of Science (AAAS)	American Association for the Advancement of Science (AAAS), 1, 2% American Association for the Advancement of Science (AAAS) 1 publication, 2%
Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii	Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii, 1, 2% Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii 1 publication, 2%
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Protesescu L. et al. Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry // Journal of the American Chemical Society. 2015. Vol. 137. No. 5. pp. 1862-1874.

GOST all authors (up to 50) Copy

Protesescu L., Nachtegaal M., Voznyy O., Borovinskaya O., Rossini A. J., Emsley L., Copéret C., Günther D., Sargent E. H., Kovalenko M. V. Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry // Journal of the American Chemical Society. 2015. Vol. 137. No. 5. pp. 1862-1874.

RIS |

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RIS Copy

TY - JOUR

DO - 10.1021/ja510862c

UR - https://doi.org/10.1021/ja510862c

TI - Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry

T2 - Journal of the American Chemical Society

AU - Borovinskaya, Olga

AU - Protesescu, Loredana

AU - Nachtegaal, Maarten

AU - Voznyy, Oleksandr

AU - Rossini, Aaron J.

AU - Emsley, Lyndon

AU - Copéret, Christophe

AU - Günther, D.

AU - Sargent, Edward H

AU - Kovalenko, Maksym V.

PY - 2015

DA - 2015/01/29 00:00:00

PB - American Chemical Society (ACS)

SP - 1862-1874

IS - 5

VL - 137

SN - 0002-7863

SN - 1520-5126

ER -

BibTex |

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@article{2015_Protesescu,

author = {Olga Borovinskaya and Loredana Protesescu and Maarten Nachtegaal and Oleksandr Voznyy and Aaron J. Rossini and Lyndon Emsley and Christophe Copéret and D. Günther and Edward H Sargent and Maksym V. Kovalenko},

title = {Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry},

journal = {Journal of the American Chemical Society},

year = {2015},

volume = {137},

publisher = {American Chemical Society (ACS)},

month = {jan},

url = {https://doi.org/10.1021/ja510862c},

number = {5},

pages = {1862--1874},

doi = {10.1021/ja510862c}

}

MLA

Cite this

MLA Copy

Protesescu, Loredana, et al. “Atomistic Description of Thiostannate-Capped CdSe Nanocrystals: Retention of Four-Coordinate SnS4 Motif and Preservation of Cd-Rich Stoichiometry.” Journal of the American Chemical Society, vol. 137, no. 5, Jan. 2015, pp. 1862-1874. https://doi.org/10.1021/ja510862c.

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American Chemical Society (ACS)

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Journal of the American Chemical Society

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Quartile WOS

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00027863 (Print)
15205126 (Electronic)