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2. Automated Scanning Dielectric Microscopy Toolbox for Operando Nanoscale Electrical Characterization of Electrolyte‐Gated Organic Transistors.

Author

Tanwar, Shubham, Millan‐Solsona, Ruben, Ruiz‐Molina, Sara, Mas‐Torrent, Marta, Kyndiah, Adrica, and Gomila, Gabriel

Subjects
SEMICONDUCTORS, DIELECTRIC measurements, BIOLOGICAL monitoring, TRANSISTORS, HIGH voltages, ORGANIC semiconductors
Abstract

Electrolyte‐gated organic transistors (EGOTs) leveraging organic semiconductors' electronic and ionic transport characteristics are the key enablers for many biosensing and bioelectronic applications that can selectively sense, record, and monitor different biological and biochemical processes at the nanoscale and translate them into macroscopic electrical signals. Understanding such transduction mechanisms requires multiscale characterization tools to comprehensively probe local electrical properties and link them with device behavior across various bias points. Here, an automated scanning dielectric microscopy toolbox is demonstrated that performs operando in‐liquid scanning dielectric microscopy measurements on functional EGOTs and carries out extensive data analysis to unravel the evolution of local electrical properties in minute detail. This paper emphasizes critical experimental considerations permitting standardized, accurate, and reproducible data acquisition. The developed approach is validated with EGOTs based on blends of organic small molecule semiconductor and insulating polymer that work as accumulation‐mode field‐effect transistors. Furthermore, the degradation of local electrical characteristics at high gate voltages is probed, which is apparently driven by the destruction of local crystalline order due to undesirable electrochemical swelling of the organic semiconducting material near the source electrode edge. The developed approach paves the way for systematic probing of EGOT‐based technologies for targeted optimization and fundamental understanding. [ABSTRACT FROM AUTHOR]

Published
2024
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4. Efficient long-range conduction in cable bacteria through nickel protein wires

Author

Boschker, Henricus T. S., Cook, Perran L. M., Polerecky, Lubos, Eachambadi, Raghavendran Thiruvallur, Lozano, Helena, Hidalgo-Martinez, Silvia, Khalenkow, Dmitry, Spampinato, Valentina, Claes, Nathalie, Kundu, Paromita, Wang, Da, Bals, Sara, Sand, Karina K., Cavezza, Francesca, Hauffman, Tom, Bjerg, Jesper Tataru, Skirtach, Andre G., Kochan, Kamila, McKee, Merrilyn, Wood, Bayden, Bedolla, Diana, Gianoncelli, Alessandra, Geerlings, Nicole M. J., Van Gerven, Nani, Remaut, Han, Geelhoed, Jeanine S., Millan-Solsona, Ruben, Fumagalli, Laura, Nielsen, Lars Peter, Franquet, Alexis, Manca, Jean V., Gomila, Gabriel, and Meysman, Filip J. R.

Published
2021
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8. Nanoscale Operando Characterization of Electrolyte-Gated Organic Field-Effect Transistors Reveals Charge Transport Bottlenecks

Author

European Commission, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Generalitat de Catalunya, Tanwar, Shubham [0000-0002-9418-2532], Gomila, Gabriel [0000-0002-1949-1757], Tanwar, Shubham, Millan Solsona, Ruben, Ruiz Molina, Sara, Mas Torrent, Marta, Kyndiah, Adrica, Gomila, Gabriel, European Commission, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Generalitat de Catalunya, Tanwar, Shubham [0000-0002-9418-2532], Gomila, Gabriel [0000-0002-1949-1757], Tanwar, Shubham, Millan Solsona, Ruben, Ruiz Molina, Sara, Mas Torrent, Marta, Kyndiah, Adrica, and Gomila, Gabriel

Abstract

Charge transport in electrolyte-gated organic field-effect transistors (EGOFETs) is governed by the microstructural property of the semiconducting thin film that is in direct contact with the electrolyte. Therefore, a comprehensive nanoscale operando characterization of the active channel is crucial to pinpoint various charge transport bottlenecks for rational and targeted optimization of the devices. Here, the local electrical properties of EGOFETs are systematically probed by in-liquid scanning dielectric microscopy (in-liquid SDM) and a direct picture of their functional mechanism at the nanoscale is provided across all operational regimes, starting from subthreshold, linear to saturation, until the onset of pinch-off. To this end, a robust interpretation framework of in-liquid SDM is introduced that enables quantitative local electric potential mapping directly from raw experimental data without requiring calibration or numerical simulations. Based on this development, a straightforward nanoscale assessment of various charge transport bottlenecks is performed, like contact access resistances, inter- and intradomain charge transport, microstructural inhomogeneities, and conduction anisotropy, which have been inaccessible earlier. Present results contribute to the fundamental understanding of charge transport in electrolyte-gated transistors and promote the development of direct structure-property-function relationships to guide future design rules.

Published
2023

10. Additional file 1 of Dielectric properties and lamellarity of single liposomes measured by in-liquid scanning dielectric microscopy

Author

Di Muzio, Martina, Millan-Solsona, Ruben, Dols-Perez, Aurora, Borrell, Jordi H., Fumagalli, Laura, and Gomila, Gabriel

Abstract

Additional file 1. Comparison of the distribution of the spherical equivalent radii of the liposomes assuming a constant area and volume. Additional data for Fig. 2. Equivalent complex permittivity of uni- and bi-lamellar core–shell spheroidal liposomes in an external uniform ac electric field. S4. Calibration curve on the substrate and extracted tip geometry. S5. Dependence of the capacitance gradient on the specific membrane capacitance. S6. Additional data for Fig. 7. S7. Geometrical model for the adsorbed liposomes.

Published
2021
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15. Efficient long-range conduction in cable bacteria through nickel protein wires

Author

Boschker, Henricus T.S., Cook, Perran L.M., Polerecky, Lubos, Eachambadi, Raghavendran Thiruvallur, Lozano, Helena, Hidalgo-Martinez, Silvia, Khalenkow, Dmitry, Spampinato, Valentina, Claes, Nathalie, Kundu, Paromita, Wang, Da, Bals, Sara, Sand, Karina K., Cavezza, Francesca, Hauffman, Tom, Bjerg, Jesper Tataru, Skirtach, Andre G., Kochan, Kamila, McKee, Merrilyn, Wood, Bayden, Bedolla, Diana, Gianoncelli, Alessandra, Geerlings, Nicole M.J., Van Gerven, Nani, Remaut, Han, Geelhoed, Jeanine S., Millan-Solsona, Ruben, Fumagalli, Laura, Nielsen, Lars Peter, Franquet, Alexis, Manca, Jean V., Gomila, Gabriel, Meysman, Filip J.R., Boschker, Henricus T.S., Cook, Perran L.M., Polerecky, Lubos, Eachambadi, Raghavendran Thiruvallur, Lozano, Helena, Hidalgo-Martinez, Silvia, Khalenkow, Dmitry, Spampinato, Valentina, Claes, Nathalie, Kundu, Paromita, Wang, Da, Bals, Sara, Sand, Karina K., Cavezza, Francesca, Hauffman, Tom, Bjerg, Jesper Tataru, Skirtach, Andre G., Kochan, Kamila, McKee, Merrilyn, Wood, Bayden, Bedolla, Diana, Gianoncelli, Alessandra, Geerlings, Nicole M.J., Van Gerven, Nani, Remaut, Han, Geelhoed, Jeanine S., Millan-Solsona, Ruben, Fumagalli, Laura, Nielsen, Lars Peter, Franquet, Alexis, Manca, Jean V., Gomila, Gabriel, and Meysman, Filip J.R.

Abstract

Filamentous cable bacteria display long-range electron transport, generating electrical currents over centimeter distances through a highly ordered network of fibers embedded in their cell envelope. The conductivity of these periplasmic wires is exceptionally high for a biological material, but their chemical structure and underlying electron transport mechanism remain unresolved. Here, we combine high-resolution microscopy, spectroscopy, and chemical imaging on individual cable bacterium filaments to demonstrate that the periplasmic wires consist of a conductive protein core surrounded by an insulating protein shell layer. The core proteins contain a sulfur-ligated nickel cofactor, and conductivity decreases when nickel is oxidized or selectively removed. The involvement of nickel as the active metal in biological conduction is remarkable, and suggests a hitherto unknown form of electron transport that enables efficient conduction in centimeter-long protein structures.

Published
2021

16. Efficient long-range conduction in cable bacteria through nickel protein wires

Author

Geochemistry, Bio-, hydro-, and environmental geochemistry, Boschker, Henricus T.S., Cook, Perran L.M., Polerecky, Lubos, Eachambadi, Raghavendran Thiruvallur, Lozano, Helena, Hidalgo-Martinez, Silvia, Khalenkow, Dmitry, Spampinato, Valentina, Claes, Nathalie, Kundu, Paromita, Wang, Da, Bals, Sara, Sand, Karina K., Cavezza, Francesca, Hauffman, Tom, Bjerg, Jesper Tataru, Skirtach, Andre G., Kochan, Kamila, McKee, Merrilyn, Wood, Bayden, Bedolla, Diana, Gianoncelli, Alessandra, Geerlings, Nicole M.J., Van Gerven, Nani, Remaut, Han, Geelhoed, Jeanine S., Millan-Solsona, Ruben, Fumagalli, Laura, Nielsen, Lars Peter, Franquet, Alexis, Manca, Jean V., Gomila, Gabriel, Meysman, Filip J.R., Geochemistry, Bio-, hydro-, and environmental geochemistry, Boschker, Henricus T.S., Cook, Perran L.M., Polerecky, Lubos, Eachambadi, Raghavendran Thiruvallur, Lozano, Helena, Hidalgo-Martinez, Silvia, Khalenkow, Dmitry, Spampinato, Valentina, Claes, Nathalie, Kundu, Paromita, Wang, Da, Bals, Sara, Sand, Karina K., Cavezza, Francesca, Hauffman, Tom, Bjerg, Jesper Tataru, Skirtach, Andre G., Kochan, Kamila, McKee, Merrilyn, Wood, Bayden, Bedolla, Diana, Gianoncelli, Alessandra, Geerlings, Nicole M.J., Van Gerven, Nani, Remaut, Han, Geelhoed, Jeanine S., Millan-Solsona, Ruben, Fumagalli, Laura, Nielsen, Lars Peter, Franquet, Alexis, Manca, Jean V., Gomila, Gabriel, and Meysman, Filip J.R.

Published
2021

17. Nanoscale Mapping of the Conductivity and Interfacial Capacitance of an Electrolyte‐Gated Organic Field‐Effect Transistor under Operation

Author

European Commission, Ministerio de Economía y Competitividad (España), Agencia Estatal de Investigación (España), Generalitat de Catalunya, Ministerio de Ciencia, Innovación y Universidades (España), European Research Council, Kyndiah, Adrica, Checa, Martí, Leonardi, Francesca, Millan Solsona, Ruben, Muzio, Martina Di, Tanwar, Shubham, Fumagalli, Laura, Mas Torrent, Marta, Gomila, Gabriel, European Commission, Ministerio de Economía y Competitividad (España), Agencia Estatal de Investigación (España), Generalitat de Catalunya, Ministerio de Ciencia, Innovación y Universidades (España), European Research Council, Kyndiah, Adrica, Checa, Martí, Leonardi, Francesca, Millan Solsona, Ruben, Muzio, Martina Di, Tanwar, Shubham, Fumagalli, Laura, Mas Torrent, Marta, and Gomila, Gabriel

Abstract

Probing nanoscale electrical properties of organic semiconducting materials at the interface with an electrolyte solution under externally applied voltages is key in the field of organic bioelectronics. It is demonstrated that the conductivity and interfacial capacitance of the active channel of an electrolyte‐gated organic field‐effect transistor (EGOFET) under operation can be probed at the nanoscale using scanning dielectric microscopy in force detection mode in liquid environment. Local electrostatic force versus gate voltage transfer characteristics are obtained on the device and correlated with the global current–voltage transfer characteristics of the EGOFET. Nanoscale maps of the conductivity of the semiconducting channel show the dependence of the channel conductivity on the gate voltage and its variation along the channel due to the space charge limited conduction. The maps reveal very small electrical heterogeneities, which correspond to local interfacial capacitance variations due to an ultrathin non‐uniform insulating layer resulting from a phase separation in the organic semiconducting blend. Present results offer insights into the transduction mechanism at the organic semiconductor/electrolyte interfaces at scales down to ≈100 nm, which can bring substantial optimization of organic electronic devices for bioelectronic applications such as electrical recording on excitable cells or label‐free biosensing.

Published
2021

20. Efficient long-range conduction in cable bacteria through nickel protein wires

Author

Boschker, Henricus T. S., primary, Cook, Perran L.M., additional, Polerecky, Lubos, additional, Eachambadi, Raghavendran Thiruvallur, additional, Lozano, Helena, additional, Hidalgo-Martinez, Silvia, additional, Khalenkow, Dmitry, additional, Spampinato, Valentina, additional, Claes, Nathalie, additional, Kundu, Paromita, additional, Wang, Da, additional, Bals, Sara, additional, Sand, Karina K., additional, Cavezza, Francesca, additional, Hauffman, Tom, additional, Bjerg, Jesper Tataru, additional, Skirtach, Andre G., additional, Kochan, Kamila, additional, McKee, Merrilyn, additional, Wood, Bayden, additional, Bedolla, Diana, additional, Gianoncelli, Alessandra, additional, Geerlings, Nicole M.J., additional, Gerven, Nani Van, additional, Remaut, Han, additional, Geelhoed, Jeanine S., additional, Millan-Solsona, Ruben, additional, Fumagalli, Laura, additional, Nielsen, Lars-Peter, additional, Franquet, Alexis, additional, Manca, Jean V., additional, Gomila, Gabriel, additional, and Meysman, Filip J. R., additional

Published
2020
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22. Bioelectronic Recordings of Cardiomyocytes with Accumulation Mode Electrolyte 1 Gated Organic Field Effect Transistors

Author

Kyndiah, Adrica, Leonardi, Francesca, Tarantino, Carolina, Cramer, Tobias, Millan Solsona, Ruben, Garreta, Elena, Montserrat, Núria, Mas Torrent, Marta, Gomila, Gabriel, European Commission, Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Dirección General de Investigación Científica y Técnica, DGICT (España), Centro de Investigación Biomédica en Red Bioingeniería, Biomateriales y Nanomedicina (España), European Research Council, Asociación Española Contra el Cáncer, and Instituto de Salud Carlos III

Subjects
Bioelectronics, Organic electronics, education, Organic semiconducting blend, Cardiac cells, Organic field effect transistors
Abstract

Organic electronic materials offer an untapped potential for novel tools for low-invasive electrophysiological recording and stimulation devices. Such materials combine semiconducting properties with tailored surface chemistry, elastic mechanical properties and chemical stability in water. In this work, we investigate solution processed Electrolyte Gated Organic Field Effect Transistors (EGOFETs) based on a small molecule semiconductor. We demonstrate that EGOFETs based on a blend of soluble organic semiconductor 2,8-Difluoro-5,11-bis(triethylsilylethynyl)anthradithiophene (diF-TES-ADT) combined with an insulating polymer show excellent sensitivity and long-term recording under electrophysiological applications. Our devices can stably record the extracellular potential of human pluripotent stem cell derived cardiomyocyte cells (hPSCs-CMs) for several weeks. In addition, cytotoxicity tests of pharmaceutical drugs, such as Norepinephrine and Verapamil was achieved with excellent sensitivity. This work demonstrates that organic transistors based on organic blends are excellent bioelectronics transducer for extracellular electrical recording of excitable cells and tissues thus providing a valid alternative to electrochemical transistors., This work has been partially supported by the BEST Postdoctoral Programme funded by the European Commission under Horizon 2020's Marie Curie Sklodowska-Curie Actions COFUND scheme (GA 712754) and the Severo Ochoa programme of the Spanish Ministry of Science and Competitiveness (SEV-2014-0425 (2015–2019) and SEV-2015-0496) and the BORGES project (Marie Curie Skłodowska European Training Network (MSCA-ITN-ETN)) under the GrantAgreement (GA) No: 813863. G. G. acknowledges support from an ICREA Academia award from the Generalitat de Catalunya and from the Agencia Estatal de Investigación (Nanoelectrophys project, TEC2016-79156-P). The authors also thank the DGI (Spain) project FANCY CTQ2016-80030-R, the Generalitat de Catalunya (2017-SGR-918) and the Networking Research Center on Bioengineering, Biomaterials, and Nanomedicine (CIBER-BBN). Dr. F. Leonardi gratefully acknowledges the “Juan de la Cierva” programme. The authors thank S. Ricci for her help on the samples preparation. This work has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (StG-2014-640525_REGMAMKID to C.T. and N.M.). NM has received funding from the Spanish Ministry of Economy and Competitiveness/FEDER (SAF2015-72617-EXP and SAF2017-89782-), the Generalitat de Catalunya and CERCA programme (2017 SGR 1306), Asociación Española contra el Cáncer (LABAE16006 to N.M.) and by CardioCel (TerCel, Instituto de Salud Carlos III). IBEC is the recipient of a Severo Ochoa Award of Excellence from MINECO.

Published
2020

23. Bioelectronic Recordings of Cardiomyocytes with Accumulation Mode Electrolyte 1 Gated Organic Field Effect Transistors

Author

European Commission, Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Dirección General de Investigación Científica y Técnica, DGICT (España), Centro de Investigación Biomédica en Red Bioingeniería, Biomateriales y Nanomedicina (España), European Research Council, Asociación Española Contra el Cáncer, Instituto de Salud Carlos III, Kyndiah, Adrica, Leonardi, Francesca, Tarantino, Carolina, Cramer, Tobias, Millan Solsona, Ruben, Garreta, Elena, Montserrat, Núria, Mas Torrent, Marta, Gomila, Gabriel, European Commission, Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Dirección General de Investigación Científica y Técnica, DGICT (España), Centro de Investigación Biomédica en Red Bioingeniería, Biomateriales y Nanomedicina (España), European Research Council, Asociación Española Contra el Cáncer, Instituto de Salud Carlos III, Kyndiah, Adrica, Leonardi, Francesca, Tarantino, Carolina, Cramer, Tobias, Millan Solsona, Ruben, Garreta, Elena, Montserrat, Núria, Mas Torrent, Marta, and Gomila, Gabriel

Abstract

Organic electronic materials offer an untapped potential for novel tools for low-invasive electrophysiological recording and stimulation devices. Such materials combine semiconducting properties with tailored surface chemistry, elastic mechanical properties and chemical stability in water. In this work, we investigate solution processed Electrolyte Gated Organic Field Effect Transistors (EGOFETs) based on a small molecule semiconductor. We demonstrate that EGOFETs based on a blend of soluble organic semiconductor 2,8-Difluoro-5,11-bis(triethylsilylethynyl)anthradithiophene (diF-TES-ADT) combined with an insulating polymer show excellent sensitivity and long-term recording under electrophysiological applications. Our devices can stably record the extracellular potential of human pluripotent stem cell derived cardiomyocyte cells (hPSCs-CMs) for several weeks. In addition, cytotoxicity tests of pharmaceutical drugs, such as Norepinephrine and Verapamil was achieved with excellent sensitivity. This work demonstrates that organic transistors based on organic blends are excellent bioelectronics transducer for extracellular electrical recording of excitable cells and tissues thus providing a valid alternative to electrochemical transistors.

Published
2020

27. Nanoscale Mapping of the Conductivity and Interfacial Capacitance of an Electrolyte‐Gated Organic Field‐Effect Transistor under Operation.

Author

Kyndiah, Adrica, Checa, Martí, Leonardi, Francesca, Millan‐Solsona, Ruben, Di Muzio, Martina, Tanwar, Shubham, Fumagalli, Laura, Mas‐Torrent, Marta, and Gomila, Gabriel

Subjects
ORGANIC field-effect transistors, SEMICONDUCTORS, SCANNING force microscopy, ELECTRIC capacity, ORGANIC semiconductors, SPACE charge, ELECTROLYTE solutions
Abstract

Probing nanoscale electrical properties of organic semiconducting materials at the interface with an electrolyte solution under externally applied voltages is key in the field of organic bioelectronics. It is demonstrated that the conductivity and interfacial capacitance of the active channel of an electrolyte‐gated organic field‐effect transistor (EGOFET) under operation can be probed at the nanoscale using scanning dielectric microscopy in force detection mode in liquid environment. Local electrostatic force versus gate voltage transfer characteristics are obtained on the device and correlated with the global current–voltage transfer characteristics of the EGOFET. Nanoscale maps of the conductivity of the semiconducting channel show the dependence of the channel conductivity on the gate voltage and its variation along the channel due to the space charge limited conduction. The maps reveal very small electrical heterogeneities, which correspond to local interfacial capacitance variations due to an ultrathin non‐uniform insulating layer resulting from a phase separation in the organic semiconducting blend. Present results offer insights into the transduction mechanism at the organic semiconductor/electrolyte interfaces at scales down to ≈100 nm, which can bring substantial optimization of organic electronic devices for bioelectronic applications such as electrical recording on excitable cells or label‐free biosensing. [ABSTRACT FROM AUTHOR]

Published
2021
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29. Revealing Fast Cu-Ion Transport and Enhanced Conductivity at the CuInP 2 S 6 -In 4/3 P 2 S 6 Heterointerface.

Author

Checa M, Jin X, Millan-Solsona R, Neumayer SM, Susner MA, McGuire MA, O'Hara A, Gomila G, Maksymovych P, Pantelides ST, and Collins L

Abstract

Van der Waals layered ferroelectrics, such as CuInP 2 S 6 (CIPS), offer a versatile platform for miniaturization of ferroelectric device technologies. Control of the targeted composition and kinetics of CIPS synthesis enables the formation of stable self-assembled heterostructures of ferroelectric CIPS and nonferroelectric In 4/3 P 2 S 6 (IPS). Here, we use quantitative scanning probe microscopy methods combined with density functional theory (DFT) to explore in detail the nanoscale variability in dynamic functional properties of the CIPS-IPS heterostructure. We report evidence of fast ionic transport which mediates an appreciable out-of-plane electromechanical response of the CIPS surface in the paraelectric phase. Further, we map the nanoscale dielectric and ionic conductivity properties as we thermally stimulate the ferroelectric-paraelectric phase transition, recovering the local dielectric behavior during this phase transition. Finally, aided by DFT, we reveal a substantial and tunable conductivity enhancement at the CIPS/IPS interface, indicating the possibility of engineering its interfacial properties for next generation device applications.

Published
2022
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