The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors

Binghao Wang; Gabriele Di Carlo; Riccardo Turrisi; Li Zeng; Katie Stallings; Wei Huang; Michael J. Bedzyk; Luca Beverina; Tobin J. Marks; Antonio Facchetti

doi:10.1021/acs.chemmater.7b03397

The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors

Binghao Wang, Gabriele Di Carlo, Riccardo Turrisi, Li Zeng, Katie Stallings, Wei Huang, Michael J. Bedzyk, Luca Beverina^*, Tobin J. Marks, Antonio Facchetti

^*Corresponding author for this work

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

17 Scopus citations

Abstract

We compare and contrast the properties of hybrid organic-inorganic self-assembled nanodielectrics (SANDs) based on alternating layers of solution-processed ZrO_x and either of two phosphonic acid-functionalized azastilbazolium π-units having opposite dipolar orientations. Conventional Zr-SAND and new inverted IZr-SAND are characterized by Kevin probe, optical spectroscopy, capacitance-voltage measurements, AFM, X-ray reflectivity, and electronic structure computation. The molecular dipolar orientation affects thin-film transistor (TFT) threshold and turn-on voltages for devices based on either p-channel pentacene or n-channel copper perfluorophthalocyanine. Specifically, Zr-SAND shifts the threshold and turn-on voltages to more positive values, whereas IZr-SAND shifts them in the opposite direction. Capping these SANDs with -SiMe₃ groups enhances the effect, affording a 1.3 V difference in turn-on voltage for IZr-SAND vs Zr-SAND-gated organic TFTs. Such tunability should facilitate the engineering of more complex circuits.

Original language	English (US)
Pages (from-to)	9974-9980
Number of pages	7
Journal	Chemistry of Materials
Volume	29
Issue number	23
DOIs	https://doi.org/10.1021/acs.chemmater.7b03397
State	Published - Dec 12 2017

ASJC Scopus subject areas

Chemistry(all)
Chemical Engineering(all)
Materials Chemistry

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10.1021/acs.chemmater.7b03397

Cite this

@article{703f3247e9354e98a533984d29968a85,

title = "The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors",

abstract = "We compare and contrast the properties of hybrid organic-inorganic self-assembled nanodielectrics (SANDs) based on alternating layers of solution-processed ZrOx and either of two phosphonic acid-functionalized azastilbazolium π-units having opposite dipolar orientations. Conventional Zr-SAND and new inverted IZr-SAND are characterized by Kevin probe, optical spectroscopy, capacitance-voltage measurements, AFM, X-ray reflectivity, and electronic structure computation. The molecular dipolar orientation affects thin-film transistor (TFT) threshold and turn-on voltages for devices based on either p-channel pentacene or n-channel copper perfluorophthalocyanine. Specifically, Zr-SAND shifts the threshold and turn-on voltages to more positive values, whereas IZr-SAND shifts them in the opposite direction. Capping these SANDs with -SiMe3 groups enhances the effect, affording a 1.3 V difference in turn-on voltage for IZr-SAND vs Zr-SAND-gated organic TFTs. Such tunability should facilitate the engineering of more complex circuits.",

author = "Binghao Wang and {Di Carlo}, Gabriele and Riccardo Turrisi and Li Zeng and Katie Stallings and Wei Huang and Bedzyk, {Michael J.} and Luca Beverina and Marks, {Tobin J.} and Antonio Facchetti",

note = "Funding Information: *E-mail: a-facchetti@northwestern.edu (A.F.). *E-mail: t-marks@northwestern.edu (T.J.M.). *E-mail: luca.beverina@mater.unimib.it (L.B.). ORCID Gabriele Di Carlo: 0000-0002-8782-7945 Li Zeng: 0000-0001-6390-0370 Wei Huang: 0000-0002-0973-8015 Michael J. Bedzyk: 0000-0002-1026-4558 Luca Beverina: 0000-0002-6450-545X Tobin J. Marks: 0000-0001-8771-0141 Funding This work was supported by the BSF (AGMT-2012250), the MRSEC program of the National Science Foundation (DMR-1121262), and ONR (MURI N00014-11-1-0690). A.F. thanks the Shenzhen Peacock Plan project (KQTD20140 630110339343) for financial support. This work made use of the J. B. Cohen X-ray Diffraction Facility, EPIC facility, Keck-II facility, and SPID facility of the NUANCE Center at Northwestern U., which received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. Notes The authors declare no competing financial interest. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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doi = "10.1021/acs.chemmater.7b03397",

language = "English (US)",

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T1 - The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors

AU - Wang, Binghao

AU - Di Carlo, Gabriele

AU - Turrisi, Riccardo

AU - Zeng, Li

AU - Stallings, Katie

AU - Huang, Wei

AU - Bedzyk, Michael J.

AU - Beverina, Luca

AU - Marks, Tobin J.

AU - Facchetti, Antonio

N1 - Funding Information: *E-mail: a-facchetti@northwestern.edu (A.F.). *E-mail: t-marks@northwestern.edu (T.J.M.). *E-mail: luca.beverina@mater.unimib.it (L.B.). ORCID Gabriele Di Carlo: 0000-0002-8782-7945 Li Zeng: 0000-0001-6390-0370 Wei Huang: 0000-0002-0973-8015 Michael J. Bedzyk: 0000-0002-1026-4558 Luca Beverina: 0000-0002-6450-545X Tobin J. Marks: 0000-0001-8771-0141 Funding This work was supported by the BSF (AGMT-2012250), the MRSEC program of the National Science Foundation (DMR-1121262), and ONR (MURI N00014-11-1-0690). A.F. thanks the Shenzhen Peacock Plan project (KQTD20140 630110339343) for financial support. This work made use of the J. B. Cohen X-ray Diffraction Facility, EPIC facility, Keck-II facility, and SPID facility of the NUANCE Center at Northwestern U., which received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. Notes The authors declare no competing financial interest. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/12/12

Y1 - 2017/12/12

N2 - We compare and contrast the properties of hybrid organic-inorganic self-assembled nanodielectrics (SANDs) based on alternating layers of solution-processed ZrOx and either of two phosphonic acid-functionalized azastilbazolium π-units having opposite dipolar orientations. Conventional Zr-SAND and new inverted IZr-SAND are characterized by Kevin probe, optical spectroscopy, capacitance-voltage measurements, AFM, X-ray reflectivity, and electronic structure computation. The molecular dipolar orientation affects thin-film transistor (TFT) threshold and turn-on voltages for devices based on either p-channel pentacene or n-channel copper perfluorophthalocyanine. Specifically, Zr-SAND shifts the threshold and turn-on voltages to more positive values, whereas IZr-SAND shifts them in the opposite direction. Capping these SANDs with -SiMe3 groups enhances the effect, affording a 1.3 V difference in turn-on voltage for IZr-SAND vs Zr-SAND-gated organic TFTs. Such tunability should facilitate the engineering of more complex circuits.

AB - We compare and contrast the properties of hybrid organic-inorganic self-assembled nanodielectrics (SANDs) based on alternating layers of solution-processed ZrOx and either of two phosphonic acid-functionalized azastilbazolium π-units having opposite dipolar orientations. Conventional Zr-SAND and new inverted IZr-SAND are characterized by Kevin probe, optical spectroscopy, capacitance-voltage measurements, AFM, X-ray reflectivity, and electronic structure computation. The molecular dipolar orientation affects thin-film transistor (TFT) threshold and turn-on voltages for devices based on either p-channel pentacene or n-channel copper perfluorophthalocyanine. Specifically, Zr-SAND shifts the threshold and turn-on voltages to more positive values, whereas IZr-SAND shifts them in the opposite direction. Capping these SANDs with -SiMe3 groups enhances the effect, affording a 1.3 V difference in turn-on voltage for IZr-SAND vs Zr-SAND-gated organic TFTs. Such tunability should facilitate the engineering of more complex circuits.

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The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors

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CCDC 1817468: Experimental Crystal Structure Determination

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The Dipole Moment Inversion Effects in Self-Assembled Nanodielectrics for Organic Transistors

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CCDC 1817468: Experimental Crystal Structure Determination

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