High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework

Renhao Dong; Peng Han; Himani Arora; Marco Ballabio; Melike Karakus; Zhe Zhang; Chandra Shekhar; Peter Adler; Petko St Petkov; Artur Erbe; Stefan C.B. Mannsfeld; Claudia Felser; Thomas Heine; Mischa Bonn; Xinliang Feng; Enrique Cánovas

doi:10.1038/s41563-018-0189-z

High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework

Renhao Dong, Peng Han, Himani Arora, Marco Ballabio, Melike Karakus, Zhe Zhang, Chandra Shekhar, Peter Adler, Petko St Petkov, Artur Erbe, Stefan C.B. Mannsfeld, Claudia Felser, Thomas Heine, Mischa Bonn, Xinliang Feng, Enrique Cánovas

Department of Chemistry

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

134 Citations (Scopus)

Abstract

Metal–organic frameworks (MOFs) are hybrid materials based on crystalline coordination polymers that consist of metal ions connected by organic ligands. In addition to the traditional applications in gas storage and separation or catalysis, the long-range crystalline order in MOFs, as well as the tunable coupling between the organic and inorganic constituents, has led to the recent development of electrically conductive MOFs as a new generation of electronic materials. However, to date, the nature of charge transport in the MOFs has remained elusive. Here we demonstrate, using high-frequency terahertz photoconductivity and Hall effect measurements, Drude-type band-like transport in a semiconducting, π–d conjugated porous Fe ₃ (THT) ₂ (NH ₄ ) ₃ (THT, 2,3,6,7,10,11-triphenylenehexathiol) two-dimensional MOF, with a room-temperature mobility up to ~ 220 cm ² V ^–1 s ^–1 . The temperature-dependent conductivity reveals that this mobility represents a lower limit for the material, as mobility is limited by impurity scattering. These results illustrate the potential for high-mobility semiconducting MOFs as active materials in thin-film optoelectronic devices.

Original language	English
Pages (from-to)	1027-1032
Number of pages	6
Journal	Nature materials
Volume	17
Issue number	11
DOIs	https://doi.org/10.1038/s41563-018-0189-z
Publication status	Published - 2018 Nov 1

Bibliographical note

Funding Information:
This work was financially supported by the ERC Grant on 2DMATER, HIPER-G and EU Graphene Flagship, European Science Foundation (ESF), Coordination Networks: Building Blocks for Functional Systems (SPP 1928, COORNET) and the German Science Council. Financial support by the Max Planck Society is also acknowledged. We acknowledge the CFAED (Center for Advancing Electronics Dresden). E.C. acknowledges financial support from the Max Planck Graduate Center and the Regional Government of Comunidad de Madrid under project 2017-T1/AMB-5207. R.D. gratefully appreciates funding from the Alexander von Humboldt-Foundation. H.A. and A.E. are grateful to the Initiative and Networking Fund of the Helmholtz Association of German Research Centers through the International Helmholtz Research School for Nanoelectronic Networks, IHRS NANONET (VH-KO-606). We appreciate LPKF Laser & Electronics for the fabrication of the Hall bar geometry by laser ablation. We acknowledge the Dresden Center for Nanoanalysis (DCN) at TUD and P. Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities, and we appreciate X. Zhang, T. Zhang, F. Ortmann and K. S. Schellhammer for the helpful discussion. P.P. and T.H. thank ZIH Dresden for providing high-performance computing facilities.

Publisher Copyright:
© 2018, The Author(s), under exclusive licence to Springer Nature Limited.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/s41563-018-0189-z

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Dong, R., Han, P., Arora, H., Ballabio, M., Karakus, M., Zhang, Z., Shekhar, C., Adler, P., Petkov, P. S., Erbe, A., Mannsfeld, S. C. B., Felser, C., Heine, T., Bonn, M., Feng, X., & Cánovas, E. (2018). High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework. Nature materials, 17(11), 1027-1032. https://doi.org/10.1038/s41563-018-0189-z

Dong, Renhao ; Han, Peng ; Arora, Himani ; Ballabio, Marco ; Karakus, Melike ; Zhang, Zhe ; Shekhar, Chandra ; Adler, Peter ; Petkov, Petko St ; Erbe, Artur ; Mannsfeld, Stefan C.B. ; Felser, Claudia ; Heine, Thomas ; Bonn, Mischa ; Feng, Xinliang ; Cánovas, Enrique. / High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework. In: Nature materials. 2018 ; Vol. 17, No. 11. pp. 1027-1032.

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title = "High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework",

abstract = " Metal–organic frameworks (MOFs) are hybrid materials based on crystalline coordination polymers that consist of metal ions connected by organic ligands. In addition to the traditional applications in gas storage and separation or catalysis, the long-range crystalline order in MOFs, as well as the tunable coupling between the organic and inorganic constituents, has led to the recent development of electrically conductive MOFs as a new generation of electronic materials. However, to date, the nature of charge transport in the MOFs has remained elusive. Here we demonstrate, using high-frequency terahertz photoconductivity and Hall effect measurements, Drude-type band-like transport in a semiconducting, π–d conjugated porous Fe 3 (THT) 2 (NH 4 ) 3 (THT, 2,3,6,7,10,11-triphenylenehexathiol) two-dimensional MOF, with a room-temperature mobility up to ~ 220 cm 2 V –1 s –1 . The temperature-dependent conductivity reveals that this mobility represents a lower limit for the material, as mobility is limited by impurity scattering. These results illustrate the potential for high-mobility semiconducting MOFs as active materials in thin-film optoelectronic devices. ",

author = "Renhao Dong and Peng Han and Himani Arora and Marco Ballabio and Melike Karakus and Zhe Zhang and Chandra Shekhar and Peter Adler and Petkov, {Petko St} and Artur Erbe and Mannsfeld, {Stefan C.B.} and Claudia Felser and Thomas Heine and Mischa Bonn and Xinliang Feng and Enrique C{\'a}novas",

note = "Funding Information: This work was financially supported by the ERC Grant on 2DMATER, HIPER-G and EU Graphene Flagship, European Science Foundation (ESF), Coordination Networks: Building Blocks for Functional Systems (SPP 1928, COORNET) and the German Science Council. Financial support by the Max Planck Society is also acknowledged. We acknowledge the CFAED (Center for Advancing Electronics Dresden). E.C. acknowledges financial support from the Max Planck Graduate Center and the Regional Government of Comunidad de Madrid under project 2017-T1/AMB-5207. R.D. gratefully appreciates funding from the Alexander von Humboldt-Foundation. H.A. and A.E. are grateful to the Initiative and Networking Fund of the Helmholtz Association of German Research Centers through the International Helmholtz Research School for Nanoelectronic Networks, IHRS NANONET (VH-KO-606). We appreciate LPKF Laser & Electronics for the fabrication of the Hall bar geometry by laser ablation. We acknowledge the Dresden Center for Nanoanalysis (DCN) at TUD and P. Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) for the use of facilities, and we appreciate X. Zhang, T. Zhang, F. Ortmann and K. S. Schellhammer for the helpful discussion. P.P. and T.H. thank ZIH Dresden for providing high-performance computing facilities. Publisher Copyright: {\textcopyright} 2018, The Author(s), under exclusive licence to Springer Nature Limited.",

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doi = "10.1038/s41563-018-0189-z",

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Dong, R, Han, P, Arora, H, Ballabio, M, Karakus, M, Zhang, Z, Shekhar, C, Adler, P, Petkov, PS, Erbe, A, Mannsfeld, SCB, Felser, C, Heine, T, Bonn, M, Feng, X & Cánovas, E 2018, 'High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework', Nature materials, vol. 17, no. 11, pp. 1027-1032. https://doi.org/10.1038/s41563-018-0189-z

High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework. / Dong, Renhao; Han, Peng; Arora, Himani; Ballabio, Marco; Karakus, Melike; Zhang, Zhe; Shekhar, Chandra; Adler, Peter; Petkov, Petko St; Erbe, Artur; Mannsfeld, Stefan C.B.; Felser, Claudia; Heine, Thomas; Bonn, Mischa; Feng, Xinliang; Cánovas, Enrique.

In: Nature materials, Vol. 17, No. 11, 01.11.2018, p. 1027-1032.

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

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AU - Zhang, Zhe

AU - Shekhar, Chandra

AU - Adler, Peter

AU - Petkov, Petko St

AU - Erbe, Artur

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AU - Heine, Thomas

AU - Bonn, Mischa

AU - Feng, Xinliang

AU - Cánovas, Enrique

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PY - 2018/11/1

Y1 - 2018/11/1

N2 - Metal–organic frameworks (MOFs) are hybrid materials based on crystalline coordination polymers that consist of metal ions connected by organic ligands. In addition to the traditional applications in gas storage and separation or catalysis, the long-range crystalline order in MOFs, as well as the tunable coupling between the organic and inorganic constituents, has led to the recent development of electrically conductive MOFs as a new generation of electronic materials. However, to date, the nature of charge transport in the MOFs has remained elusive. Here we demonstrate, using high-frequency terahertz photoconductivity and Hall effect measurements, Drude-type band-like transport in a semiconducting, π–d conjugated porous Fe 3 (THT) 2 (NH 4 ) 3 (THT, 2,3,6,7,10,11-triphenylenehexathiol) two-dimensional MOF, with a room-temperature mobility up to ~ 220 cm 2 V –1 s –1 . The temperature-dependent conductivity reveals that this mobility represents a lower limit for the material, as mobility is limited by impurity scattering. These results illustrate the potential for high-mobility semiconducting MOFs as active materials in thin-film optoelectronic devices.

AB - Metal–organic frameworks (MOFs) are hybrid materials based on crystalline coordination polymers that consist of metal ions connected by organic ligands. In addition to the traditional applications in gas storage and separation or catalysis, the long-range crystalline order in MOFs, as well as the tunable coupling between the organic and inorganic constituents, has led to the recent development of electrically conductive MOFs as a new generation of electronic materials. However, to date, the nature of charge transport in the MOFs has remained elusive. Here we demonstrate, using high-frequency terahertz photoconductivity and Hall effect measurements, Drude-type band-like transport in a semiconducting, π–d conjugated porous Fe 3 (THT) 2 (NH 4 ) 3 (THT, 2,3,6,7,10,11-triphenylenehexathiol) two-dimensional MOF, with a room-temperature mobility up to ~ 220 cm 2 V –1 s –1 . The temperature-dependent conductivity reveals that this mobility represents a lower limit for the material, as mobility is limited by impurity scattering. These results illustrate the potential for high-mobility semiconducting MOFs as active materials in thin-film optoelectronic devices.

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High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework

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