skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: N-type organic electrochemical transistors with stability in water

Abstract

Organic electrochemical transistors (OECTs) are receiving significant attention due to their ability to efficiently transduce biological signals. A major limitation of this technology is that only p-type materials have been reported, which precludes the development of complementary circuits, and limits sensor technologies. Here, we report the first ever n-type OECT, with relatively balanced ambipolar charge transport characteristics based on a polymer that supports both hole and electron transport along its backbone when doped through an aqueous electrolyte and in the presence of oxygen. This new semiconducting polymer is designed specifically to facilitate ion transport and promote electrochemical doping. Stability measurements in water show no degradation when tested for 2 h under continuous cycling. Furthermore, this demonstration opens the possibility to develop complementary circuits based on OECTs and to improve the sophistication of bioelectronic devices.

Authors:
 [1];  [2];  [1];  [3];  [3];  [4];  [5];  [4];  [3];  [6];  [7]
  1. Imperial College, London (United Kingdom)
  2. Imperial College, London (United Kingdom); Queen Mary Univ. of London, London (United Kingdom)
  3. Ecole Nationale Superieure des Mines, Gardanne (France)
  4. King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)
  5. Stanford Univ., Stanford, CA (United States)
  6. Ecole Nationale Superieure des Mines, Gardanne (France); Palo Alto Research Center, Palo Alto, CA (United States)
  7. Imperial College, London (United Kingdom); King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1348869
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrochemistry; electronic devices

Citation Formats

Giovannitti, Alexander, Nielsen, Christian B., Sbircea, Dan -Tiberiu, Inal, Sahika, Donahue, Mary, Niazi, Muhammad R., Hanifi, David A., Amassian, Aram, Malliaras, George G., Rivnay, Jonathan, and McCulloch, Iain. N-type organic electrochemical transistors with stability in water. United States: N. p., 2016. Web. https://doi.org/10.1038/ncomms13066.
Giovannitti, Alexander, Nielsen, Christian B., Sbircea, Dan -Tiberiu, Inal, Sahika, Donahue, Mary, Niazi, Muhammad R., Hanifi, David A., Amassian, Aram, Malliaras, George G., Rivnay, Jonathan, & McCulloch, Iain. N-type organic electrochemical transistors with stability in water. United States. https://doi.org/10.1038/ncomms13066
Giovannitti, Alexander, Nielsen, Christian B., Sbircea, Dan -Tiberiu, Inal, Sahika, Donahue, Mary, Niazi, Muhammad R., Hanifi, David A., Amassian, Aram, Malliaras, George G., Rivnay, Jonathan, and McCulloch, Iain. Fri . "N-type organic electrochemical transistors with stability in water". United States. https://doi.org/10.1038/ncomms13066. https://www.osti.gov/servlets/purl/1348869.
@article{osti_1348869,
title = {N-type organic electrochemical transistors with stability in water},
author = {Giovannitti, Alexander and Nielsen, Christian B. and Sbircea, Dan -Tiberiu and Inal, Sahika and Donahue, Mary and Niazi, Muhammad R. and Hanifi, David A. and Amassian, Aram and Malliaras, George G. and Rivnay, Jonathan and McCulloch, Iain},
abstractNote = {Organic electrochemical transistors (OECTs) are receiving significant attention due to their ability to efficiently transduce biological signals. A major limitation of this technology is that only p-type materials have been reported, which precludes the development of complementary circuits, and limits sensor technologies. Here, we report the first ever n-type OECT, with relatively balanced ambipolar charge transport characteristics based on a polymer that supports both hole and electron transport along its backbone when doped through an aqueous electrolyte and in the presence of oxygen. This new semiconducting polymer is designed specifically to facilitate ion transport and promote electrochemical doping. Stability measurements in water show no degradation when tested for 2 h under continuous cycling. Furthermore, this demonstration opens the possibility to develop complementary circuits based on OECTs and to improve the sophistication of bioelectronic devices.},
doi = {10.1038/ncomms13066},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

The Application of Organic Electrochemical Transistors in Cell-Based Biosensors
journal, August 2010


Unconventional Face-On Texture and Exceptional In-Plane Order of a High Mobility n-Type Polymer
journal, July 2010

  • Rivnay, Jonathan; Toney, Michael F.; Zheng, Yan
  • Advanced Materials, Vol. 22, Issue 39
  • DOI: 10.1002/adma.201001202

Conjugated Polyelectrolyte Blends for Electrochromic and Electrochemical Transistor Devices
journal, August 2015


A High Transconductance Accumulation Mode Electrochemical Transistor
journal, October 2014

  • Inal, Sahika; Rivnay, Jonathan; Leleux, Pierre
  • Advanced Materials, Vol. 26, Issue 44
  • DOI: 10.1002/adma.201403150

A high-mobility electron-transporting polymer for printed transistors
journal, January 2009

  • Yan, He; Chen, Zhihua; Zheng, Yan
  • Nature, Vol. 457, Issue 7230, p. 679-686
  • DOI: 10.1038/nature07727

Stability of n-type doped conducting polymers and consequences for polymeric microelectronic devices
journal, February 1997


Electrocardiographic Recording with Conformable Organic Electrochemical Transistor Fabricated on Resorbable Bioscaffold
journal, March 2014

  • Campana, Alessandra; Cramer, Tobias; Simon, Daniel T.
  • Advanced Materials, Vol. 26, Issue 23
  • DOI: 10.1002/adma.201400263

Doping of organic semiconductors
journal, December 2012


Sodium and Potassium Ion Selective Conjugated Polymers for Optical Ion Detection in Solution and Solid State
journal, December 2015

  • Giovannitti, Alexander; Nielsen, Christian B.; Rivnay, Jonathan
  • Advanced Functional Materials, Vol. 26, Issue 4
  • DOI: 10.1002/adfm.201503791

Organic Electrochemical Transistors with Maximum Transconductance at Zero Gate Bias
journal, October 2013

  • Rivnay, Jonathan; Leleux, Pierre; Sessolo, Michele
  • Advanced Materials, Vol. 25, Issue 48
  • DOI: 10.1002/adma.201303080

Highly stable organic polymer field-effect transistor sensor for selective detection in the marine environment
journal, January 2014

  • Knopfmacher, Oren; Hammock, Mallory L.; Appleton, Anthony L.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms3954

Naphthalenedicarboximide- vs Perylenedicarboximide-Based Copolymers. Synthesis and Semiconducting Properties in Bottom-Gate N-Channel Organic Transistors
journal, January 2009

  • Chen, Zhihua; Zheng, Yan; Yan, He
  • Journal of the American Chemical Society, Vol. 131, Issue 1, p. 8-9
  • DOI: 10.1021/ja805407g

Conjugated Polymer Energy Level Shifts in Lithium-Ion Battery Electrolytes
journal, October 2014

  • Song, Charles Kiseok; Eckstein, Brian J.; Tam, Teck Lip Dexter
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 21
  • DOI: 10.1021/am505416m

Record High Electron Mobility of 6.3 cm 2 V −1 s −1 Achieved for Polymer Semiconductors Using a New Building Block
journal, March 2014


High mobility diketopyrrolopyrrole (DPP)-based organic semiconductor materials for organic thin film transistors and photovoltaics
journal, January 2013

  • Li, Yuning; Sonar, Prashant; Murphy, Leanne
  • Energy & Environmental Science, Vol. 6, Issue 6
  • DOI: 10.1039/c3ee00015j

Organic Electrochemical Transistors for Clinical Applications
journal, September 2014

  • Leleux, Pierre; Rivnay, Jonathan; Lonjaret, Thomas
  • Advanced Healthcare Materials, Vol. 4, Issue 1
  • DOI: 10.1002/adhm.201400356

Dramatic Inversion of Charge Polarity in Diketopyrrolopyrrole-Based Organic Field-Effect Transistors via a Simple Nitrile Group Substitution
journal, September 2014


The Rise of Organic Bioelectronics
journal, September 2013

  • Rivnay, Jonathan; Owens, Róisín M.; Malliaras, George G.
  • Chemistry of Materials, Vol. 26, Issue 1
  • DOI: 10.1021/cm4022003

Localized Neuron Stimulation with Organic Electrochemical Transistors on Delaminating Depth Probes
journal, June 2015

  • Williamson, Adam; Ferro, Marc; Leleux, Pierre
  • Advanced Materials, Vol. 27, Issue 30
  • DOI: 10.1002/adma.201500218

n- and p-Doped Poly(3,4-ethylenedioxythiophene):  Two Electronically Conducting States of the Polymer
journal, September 2000

  • Ahonen, Harri J.; Lukkari, Jukka; Kankare, Jouko
  • Macromolecules, Vol. 33, Issue 18
  • DOI: 10.1021/ma0004312

Tuning Orbital Energetics in Arylene Diimide Semiconductors. Materials Design for Ambient Stability of n-Type Charge Transport
journal, December 2007

  • Jones, Brooks A.; Facchetti, Antonio; Wasielewski, Michael R.
  • Journal of the American Chemical Society, Vol. 129, Issue 49
  • DOI: 10.1021/ja075242e

High-performance transistors for bioelectronics through tuning of channel thickness
journal, May 2015


A Fluorinated Phenylene Unit as a Building Block for High-Performance n-Type Semiconducting Polymer
journal, March 2013

  • Park, Jung Ha; Jung, Eui Hyuk; Jung, Jae Woong
  • Advanced Materials, Vol. 25, Issue 18
  • DOI: 10.1002/adma.201205320

N-type doping of an electron-transport material by controlled gas-phase incorporation of cobaltocene
journal, November 2006


A Water-Gate Organic Field-Effect Transistor
journal, May 2010

  • Kergoat, Loig; Herlogsson, Lars; Braga, Daniele
  • Advanced Materials, Vol. 22, Issue 23
  • DOI: 10.1002/adma.200904163

In vivo recordings of brain activity using organic transistors
journal, March 2013

  • Khodagholy, Dion; Doublet, Thomas; Quilichini, Pascale
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2573

High-Mobility Air-Stable n-Type Semiconductors with Processing Versatility: Dicyanoperylene-3,4:9,10-bis(dicarboximides)
journal, November 2004

  • Jones, Brooks A.; Ahrens, Michael J.; Yoon, Myung-Han
  • Angewandte Chemie, Vol. 116, Issue 46
  • DOI: 10.1002/ange.200461324

Air-stable n-channel organic field-effect transistors based on a sulfur rich π-electron acceptor
journal, January 2015

  • Filatre-Furcate, Agathe; Higashino, Toshiki; Lorcy, Dominique
  • Journal of Materials Chemistry C, Vol. 3, Issue 15
  • DOI: 10.1039/C5TC00253B

High Performance Weak Donor–Acceptor Polymers in Thin Film Transistors: Effect of the Acceptor on Electronic Properties, Ambipolar Conductivity, Mobility, and Thermal Stability
journal, December 2011

  • Yuen, Jonathan D.; Fan, Jian; Seifter, Jason
  • Journal of the American Chemical Society, Vol. 133, Issue 51
  • DOI: 10.1021/ja205566w

Very Low Degree of Energetic Disorder as the Origin of High Mobility in an n-channel Polymer Semiconductor
journal, July 2011

  • Caironi, Mario; Bird, Matt; Fazzi, Daniele
  • Advanced Functional Materials, Vol. 21, Issue 17
  • DOI: 10.1002/adfm.201100592

High transconductance organic electrochemical transistors
journal, July 2013

  • Khodagholy, Dion; Rivnay, Jonathan; Sessolo, Michele
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3133

Role of Polymer Structure on the Conductivity of N-Doped Polymers
journal, March 2016

  • Naab, Benjamin D.; Gu, Xiaodan; Kurosawa, Tadanori
  • Advanced Electronic Materials, Vol. 2, Issue 5
  • DOI: 10.1002/aelm.201600004

High-Mobility Air-Stable n-Type Semiconductors with Processing Versatility: Dicyanoperylene-3,4:9,10-bis(dicarboximides)
journal, November 2004

  • Jones, Brooks A.; Ahrens, Michael J.; Yoon, Myung-Han
  • Angewandte Chemie International Edition, Vol. 43, Issue 46
  • DOI: 10.1002/anie.200461324

High-performance transistors for bioelectronics through tuning of channel thickness.
text, January 2015

  • Rivnay, Jonathan; Leleux, Pierre; Ferro, Marc
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.21507

High transconductance organic electrochemical transistors.
text, January 2013

  • Khodagholy, Dion; Rivnay, Jonathan; Sessolo, Michele
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.21514

In vivo recordings of brain activity using organic transistors.
text, January 2013

  • Khodagholy, Dion; Doublet, Thomas; Quilichini, Pascale
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.21515

    Works referencing / citing this record:

    Materials in Organic Electrochemical Transistors for Bioelectronic Applications: Past, Present, and Future
    journal, December 2018

    • Moser, Maximilian; Ponder, James F.; Wadsworth, Andrew
    • Advanced Functional Materials, Vol. 29, Issue 21
    • DOI: 10.1002/adfm.201807033

    Role of the Anion on the Transport and Structure of Organic Mixed Conductors
    journal, December 2018

    • Cendra, Camila; Giovannitti, Alexander; Savva, Achilleas
    • Advanced Functional Materials, Vol. 29, Issue 5
    • DOI: 10.1002/adfm.201807034

    Ultimately Sensitive Organic Bioelectronic Transistor Sensors by Materials and Device Structure Design
    journal, September 2019

    • Picca, Rosaria Anna; Manoli, Kyriaki; Macchia, Eleonora
    • Advanced Functional Materials, Vol. 30, Issue 20
    • DOI: 10.1002/adfm.201904513

    Polar Side Chains Enhance Processability, Electrical Conductivity, and Thermal Stability of a Molecularly p-Doped Polythiophene
    journal, April 2017

    • Kroon, Renee; Kiefer, David; Stegerer, Dominik
    • Advanced Materials, Vol. 29, Issue 24
    • DOI: 10.1002/adma.201700930

    Enhancing Molecular n-Type Doping of Donor-Acceptor Copolymers by Tailoring Side Chains
    journal, January 2018


    Complementary Logic Circuits Based on High-Performance n-Type Organic Electrochemical Transistors
    journal, January 2018


    Dynamic and Tunable Threshold Voltage in Organic Electrochemical Transistors
    journal, March 2018

    • Doris, Sean E.; Pierre, Adrien; Street, Robert A.
    • Advanced Materials, Vol. 30, Issue 15
    • DOI: 10.1002/adma.201706757

    Active Materials for Organic Electrochemical Transistors
    journal, July 2018


    Ion Electron–Coupled Functionality in Materials and Devices Based on Conjugated Polymers
    journal, January 2019

    • Berggren, Magnus; Crispin, Xavier; Fabiano, Simone
    • Advanced Materials, Vol. 31, Issue 22
    • DOI: 10.1002/adma.201805813

    Conjugated Polymers for Assessing and Controlling Biological Functions
    journal, March 2019

    • Zeglio, Erica; Rutz, Alexandra L.; Winkler, Thomas E.
    • Advanced Materials, Vol. 31, Issue 22
    • DOI: 10.1002/adma.201806712

    On the Role of Contact Resistance and Electrode Modification in Organic Electrochemical Transistors
    journal, July 2019

    • Paterson, Alexandra F.; Faber, Hendrik; Savva, Achilleas
    • Advanced Materials, Vol. 31, Issue 37
    • DOI: 10.1002/adma.201902291

    Molecular Semiconductors for Logic Operations: Dead‐End or Bright Future?
    journal, January 2020

    • Schweicher, Guillaume; Garbay, Guillaume; Jouclas, Rémy
    • Advanced Materials, Vol. 32, Issue 10
    • DOI: 10.1002/adma.201905909

    Solvent Engineering for High‐Performance n‐Type Organic Electrochemical Transistors
    journal, June 2019

    • Savva, Achilleas; Ohayon, David; Surgailis, Jokubas
    • Advanced Electronic Materials, Vol. 5, Issue 8
    • DOI: 10.1002/aelm.201900249

    Principles of Structural Design of Conjugated Polymers Showing Excellent Charge Transport toward Thermoelectrics and Bioelectronics Applications
    journal, March 2019

    • Goel, Mahima; Heinrich, C. David; Krauss, Gert
    • Macromolecular Rapid Communications, Vol. 40, Issue 10
    • DOI: 10.1002/marc.201800915

    Organic electrochemical transistors
    journal, January 2018


    Influence of PEDOT:PSS crystallinity and composition on electrochemical transistor performance and long-term stability
    journal, September 2018


    Ion buffering and interface charge enable high performance electronics with organic electrochemical transistors
    journal, July 2019

    • Romele, Paolo; Ghittorelli, Matteo; Kovács-Vajna, Zsolt Miklós
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-11073-4

    Double doping of conjugated polymers with monomer molecular dopants
    journal, January 2019


    Biofuel powered glucose detection in bodily fluids with an n-type conjugated polymer
    journal, December 2019


    The role of chemical design in the performance of organic semiconductors
    journal, January 2020

    • Bronstein, Hugo; Nielsen, Christian B.; Schroeder, Bob C.
    • Nature Reviews Chemistry, Vol. 4, Issue 2
    • DOI: 10.1038/s41570-019-0152-9

    Dithienylbenzodiimide: a new electron-deficient unit for n-type polymer semiconductors
    journal, January 2017

    • Chen, Jianhua; Zhang, Xianhe; Wang, Gang
    • Journal of Materials Chemistry C, Vol. 5, Issue 37
    • DOI: 10.1039/c7tc02903a

    Design and evaluation of conjugated polymers with polar side chains as electrode materials for electrochemical energy storage in aqueous electrolytes
    journal, January 2019

    • Moia, Davide; Giovannitti, Alexander; Szumska, Anna A.
    • Energy & Environmental Science, Vol. 12, Issue 4
    • DOI: 10.1039/c8ee03518k

    Morphological effects on polymeric mixed ionic/electronic conductors
    journal, January 2019

    • Onorato, Jonathan W.; Luscombe, Christine K.
    • Molecular Systems Design & Engineering, Vol. 4, Issue 2
    • DOI: 10.1039/c8me00093j

    A Na + conducting hydrogel for protection of organic electrochemical transistors
    journal, January 2018

    • del Agua, I.; Porcarelli, L.; Curto, V. F.
    • Journal of Materials Chemistry B, Vol. 6, Issue 18
    • DOI: 10.1039/c8tb00201k

    Lipid bilayer formation on organic electronic materials
    journal, January 2018

    • Zhang, Yi; Wustoni, Shofarul; Savva, Achilleas
    • Journal of Materials Chemistry C, Vol. 6, Issue 19
    • DOI: 10.1039/c8tc00370j

    n-Type organic electrochemical transistors: materials and challenges
    journal, January 2018

    • Sun, Hengda; Gerasimov, Jennifer; Berggren, Magnus
    • Journal of Materials Chemistry C, Vol. 6, Issue 44
    • DOI: 10.1039/c8tc03185a

    Organic semiconductors for biological sensing
    journal, January 2019

    • Borges-González, Jorge; Kousseff, Christina J.; Nielsen, Christian B.
    • Journal of Materials Chemistry C, Vol. 7, Issue 5
    • DOI: 10.1039/c8tc05900d

    Oligo(ethylene glycol) as side chains of conjugated polymers for optoelectronic applications
    journal, January 2020

    • Meng, Bin; Liu, Jun; Wang, Lixiang
    • Polymer Chemistry, Vol. 11, Issue 7
    • DOI: 10.1039/c9py01469a

    Controlling intermolecular redox-doping of naphthalene diimides
    journal, January 2019

    • Schmidt, Simon B.; Biskup, Till; Jiao, Xuechen
    • Journal of Materials Chemistry C, Vol. 7, Issue 15
    • DOI: 10.1039/c9tc00721k

    Emerging research directions for n-type conjugated polymers
    journal, January 2019

    • Jia, Hanyu; Lei, Ting
    • Journal of Materials Chemistry C, Vol. 7, Issue 41
    • DOI: 10.1039/c9tc02632k

    Electrolyte-gated transistors for synaptic electronics, neuromorphic computing, and adaptable biointerfacing
    journal, March 2020

    • Ling, Haifeng; Koutsouras, Dimitrios A.; Kazemzadeh, Setareh
    • Applied Physics Reviews, Vol. 7, Issue 1
    • DOI: 10.1063/1.5122249

    Review on water quality sensors
    journal, April 2018


    Ultra-sensitive protein detection with organic electrochemical transistors printed on plastic substrates
    journal, July 2018

    • Macchia, Eleonora; Romele, Paolo; Manoli, Kyriaki
    • Flexible and Printed Electronics, Vol. 3, Issue 3
    • DOI: 10.1088/2058-8585/aad0cb

    Recent advances in modeling organic electrochemical transistors
    journal, January 2020

    • Colucci, Renan; Barbosa, Henrique Frulani de Paula; Günther, Florian
    • Flexible and Printed Electronics, Vol. 5, Issue 1
    • DOI: 10.1088/2058-8585/ab601b

    A fully inkjet-printed disposable glucose sensor on paper
    journal, December 2018

    • Bihar, Eloïse; Wustoni, Shofarul; Pappa, Anna Maria
    • npj Flexible Electronics, Vol. 2, Issue 1
    • DOI: 10.1038/s41528-018-0044-y