Charge transport and localization in atomically coherent quantum dot solids

Kevin Whitham; Jun Yang; Benjamin H. Savitzky; Lena F. Kourkoutis; Frank Wise; Tobias Hanrath

doi:10.1038/NMAT4576

Charge transport and localization in atomically coherent quantum dot solids

Kevin Whitham, Jun Yang, Benjamin H. Savitzky, Lena F. Kourkoutis, Frank Wise, Tobias Hanrath

Research output: Contribution to journal › Article › peer-review

248 Scopus citations

Abstract

Epitaxial attachment of quantum dots into ordered superlattices enables the synthesis of quasi-two-dimensional materials that theoretically exhibit features such as Dirac cones and topological states, and have major potential for unprecedented optoelectronic devices. Initial studies found that disorder in these structures causes localization of electrons within a few lattice constants, and highlight the critical need for precise structural characterization and systematic assessment of the effects of disorder on transport. Here we fabricated superlattices with the quantum dots registered to within a single atomic bond length (limited by the polydispersity of the quantum dot building blocks), but missing a fraction (20%) of the epitaxial connections. Calculations of the electronic structure including the measured disorder account for the electron localization inferred from transport measurements. The calculations also show that improvement of the epitaxial connections will lead to completely delocalized electrons and may enable the observation of the remarkable properties predicted for these materials.

Original language	English (US)
Pages (from-to)	557-+
Number of pages	556
Journal	NATURE MATERIALS
Volume	15
Issue number	5
DOIs	https://doi.org/10.1038/NMAT4576
State	Published - Feb 22 2016
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2022-06-01
Acknowledged KAUST grant number(s): KUS-C1-018-02
Acknowledgements: This research was supported by the Cornell Center for Materials Research with funding from the NSF MRSEC program (DMR-1120296). K.W. and J.Y. were supported by the Basic Energy Sciences Division of the Department of Energy through Grant DE-SC0006647 'Charge Transfer Across the Boundary of Photon-Harvesting Nanocrystals'. B.H.S. was supported by the NSF IGERT grant DGE-0903653 and NSF GRFP grant DGE-1144153. This work was based on research conducted at the Cornell High Energy Synchrotron Source (CHESS), which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF award DMR-1332208. Charge transport measurements were performed in a facility supported by Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST). The authors wish to thank CHESS staff scientist Detlef Smilgies for assistance with X-ray scattering experiments.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

Mechanics of Materials
General Materials Science
General Chemistry
Mechanical Engineering
Condensed Matter Physics

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title = "Charge transport and localization in atomically coherent quantum dot solids",

abstract = "Epitaxial attachment of quantum dots into ordered superlattices enables the synthesis of quasi-two-dimensional materials that theoretically exhibit features such as Dirac cones and topological states, and have major potential for unprecedented optoelectronic devices. Initial studies found that disorder in these structures causes localization of electrons within a few lattice constants, and highlight the critical need for precise structural characterization and systematic assessment of the effects of disorder on transport. Here we fabricated superlattices with the quantum dots registered to within a single atomic bond length (limited by the polydispersity of the quantum dot building blocks), but missing a fraction (20%) of the epitaxial connections. Calculations of the electronic structure including the measured disorder account for the electron localization inferred from transport measurements. The calculations also show that improvement of the epitaxial connections will lead to completely delocalized electrons and may enable the observation of the remarkable properties predicted for these materials.",

author = "Kevin Whitham and Jun Yang and Savitzky, {Benjamin H.} and Kourkoutis, {Lena F.} and Frank Wise and Tobias Hanrath",

note = "KAUST Repository Item: Exported on 2022-06-01 Acknowledged KAUST grant number(s): KUS-C1-018-02 Acknowledgements: This research was supported by the Cornell Center for Materials Research with funding from the NSF MRSEC program (DMR-1120296). K.W. and J.Y. were supported by the Basic Energy Sciences Division of the Department of Energy through Grant DE-SC0006647 'Charge Transfer Across the Boundary of Photon-Harvesting Nanocrystals'. B.H.S. was supported by the NSF IGERT grant DGE-0903653 and NSF GRFP grant DGE-1144153. This work was based on research conducted at the Cornell High Energy Synchrotron Source (CHESS), which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF award DMR-1332208. Charge transport measurements were performed in a facility supported by Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST). The authors wish to thank CHESS staff scientist Detlef Smilgies for assistance with X-ray scattering experiments. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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AU - Hanrath, Tobias

N1 - KAUST Repository Item: Exported on 2022-06-01 Acknowledged KAUST grant number(s): KUS-C1-018-02 Acknowledgements: This research was supported by the Cornell Center for Materials Research with funding from the NSF MRSEC program (DMR-1120296). K.W. and J.Y. were supported by the Basic Energy Sciences Division of the Department of Energy through Grant DE-SC0006647 'Charge Transfer Across the Boundary of Photon-Harvesting Nanocrystals'. B.H.S. was supported by the NSF IGERT grant DGE-0903653 and NSF GRFP grant DGE-1144153. This work was based on research conducted at the Cornell High Energy Synchrotron Source (CHESS), which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF award DMR-1332208. Charge transport measurements were performed in a facility supported by Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST). The authors wish to thank CHESS staff scientist Detlef Smilgies for assistance with X-ray scattering experiments. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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N2 - Epitaxial attachment of quantum dots into ordered superlattices enables the synthesis of quasi-two-dimensional materials that theoretically exhibit features such as Dirac cones and topological states, and have major potential for unprecedented optoelectronic devices. Initial studies found that disorder in these structures causes localization of electrons within a few lattice constants, and highlight the critical need for precise structural characterization and systematic assessment of the effects of disorder on transport. Here we fabricated superlattices with the quantum dots registered to within a single atomic bond length (limited by the polydispersity of the quantum dot building blocks), but missing a fraction (20%) of the epitaxial connections. Calculations of the electronic structure including the measured disorder account for the electron localization inferred from transport measurements. The calculations also show that improvement of the epitaxial connections will lead to completely delocalized electrons and may enable the observation of the remarkable properties predicted for these materials.

AB - Epitaxial attachment of quantum dots into ordered superlattices enables the synthesis of quasi-two-dimensional materials that theoretically exhibit features such as Dirac cones and topological states, and have major potential for unprecedented optoelectronic devices. Initial studies found that disorder in these structures causes localization of electrons within a few lattice constants, and highlight the critical need for precise structural characterization and systematic assessment of the effects of disorder on transport. Here we fabricated superlattices with the quantum dots registered to within a single atomic bond length (limited by the polydispersity of the quantum dot building blocks), but missing a fraction (20%) of the epitaxial connections. Calculations of the electronic structure including the measured disorder account for the electron localization inferred from transport measurements. The calculations also show that improvement of the epitaxial connections will lead to completely delocalized electrons and may enable the observation of the remarkable properties predicted for these materials.

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Charge transport and localization in atomically coherent quantum dot solids

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