| 1. |
- Sensi, Matteo, et al.
(författare)
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Modulating the Faradic Operation of All-Printed Organic Electrochemical Transistors by Facile in Situ Modification of the Gate Electrode
- 2019
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Ingår i: ACS Omega. - : American Chemical Society (ACS). - 2470-1343. ; 4:3, s. 5374-5381
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Tidskriftsartikel (refereegranskat)abstract
- Organic electrochemical transistors (OECTs) operated in the faradic regime were shown as outperforming transducers of bioelectric signals in vitro and in vivo. Fabrication by additive manufacturing techniques fosters OECTs as ideal candidates for point-of-care applications, as well as imposes limitations on the choice of materials and their processing conditions. Here, we address the question of how the response of fully printed OECTs depends on gate electrode material. Toward this end, we investigate the redox processes underlying the operation of OECTs under faradic regime, to show OECTs with carbon gate (C-gate) that exhibit no current modulation gate voltages <1.2 V. This is a hallmark that no interference with the faradic operation of the device enabled by redox processes occurs when operating C-gate OECTs in the low-voltage range as label-free biosensors for the detection of electroactive (bio)molecules. To tune the faradic response of the device, we electrodeposited Au on the carbon gate (Au-C-gate), obtaining a device that operates at lower gate voltage values than C-gate OECT. The presence of gold on the gate allowed further modification of the electrical performances by functionalization of the Au-C-gate with different self-assembled monolayers by fast potential-pulse-assisted method. Moreover, we show that the presence in the electrolyte solution of an external redox probe can be used to drive the faradic response of both C- and Au-C-gate OECTs, impacting on the gate potential window that yields effective drain current modulation. The results presented here suggest possible new strategies for controlling the faradic operation regime of OECTs sensors by chemical modification of the gate surface.
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| 2. |
- Boschi, Alex, et al.
(författare)
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Mesoscopic 3D Charge Transport in Solution-Processed Graphene-Based Thin Films: A Multiscale Analysis
- 2023
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Ingår i: Small. - 1613-6810 .- 1613-6829. ; 19:42
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Tidskriftsartikel (refereegranskat)abstract
- Graphene and related 2D material (GRM) thin films consist of 3D assembly of billions of 2D nanosheets randomly distributed and interacting via van der Waals forces. Their complexity and the multiscale nature yield a wide variety of electrical characteristics ranging from doped semiconductor to glassy metals depending on the crystalline quality of the nanosheets, their specific structural organization ant the operating temperature. Here, the charge transport (CT) mechanisms are studied that are occurring in GRM thin films near the metal-insulator transition (MIT) highlighting the role of defect density and local arrangement of the nanosheets. Two prototypical nanosheet types are compared, i.e., 2D reduced graphene oxide and few-layer-thick electrochemically exfoliated graphene flakes, forming thin films with comparable composition, morphology and room temperature conductivity, but different defect density and crystallinity. By investigating their structure, morphology, and the dependence of their electrical conductivity on temperature, noise and magnetic-field, a general model is developed describing the multiscale nature of CT in GRM thin films in terms of hopping among mesoscopic bricks, i.e., grains. The results suggest a general approach to describe disordered van der Waals thin films.
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| 3. |
- Kovtun, Alessandro, et al.
(författare)
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Multiscale Charge Transport in van der Waals Thin Films: Reduced Graphene Oxide as a Case Study
- 2021
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 15:2, s. 2654-2667
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Tidskriftsartikel (refereegranskat)abstract
- Large area van der Waals (vdW) thin films are assembled materials consisting of a network of randomly stacked nanosheets. The multiscale structure and the two-dimensional (2D) nature of the building block mean that interfaces naturally play a crucial role in the charge transport of such thin films. While single or few stacked nanosheets (i.e., vdW heterostructures) have been the subject of intensive works, little is known about how charges travel through multilayered, more disordered networks. Here, we report a comprehensive study of a prototypical system given by networks of randomly stacked reduced graphene oxide 2D nanosheets, whose chemical and geometrical properties can be controlled independently, permitting to explore percolated networks ranging from a single nanosheet to some billions with room-temperature resistivity spanning from 10-5 to 10-1 ω·m. We systematically observe a clear transition between two different regimes at a critical temperature T*: Efros-Shklovskii variable-range hopping (ES-VRH) below T∗ and power law behavior above. First, we demonstrate that the two regimes are strongly correlated with each other, both depending on the charge localization length ζ, calculated by the ES-VRH model, which corresponds to the characteristic size of overlapping sp2 domains belonging to different nanosheets. Thus, we propose a microscopic model describing the charge transport as a geometrical phase transition, given by the metal-insulator transition associated with the percolation of quasi-one-dimensional nanofillers with length ζ, showing that the charge transport behavior of the networks is valid for all geometries and defects of the nanosheets, ultimately suggesting a generalized description on vdW and disordered thin films.
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| 4. |
- Xia, Zhenyuan, 1983, et al.
(författare)
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Dispersion Stability and Surface Morphology Study of Electrochemically Exfoliated Bilayer Graphene Oxide
- 2019
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 123:24, s. 15122-15130
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Tidskriftsartikel (refereegranskat)abstract
- During the last decade, electrochemical exfoliation of graphite has aroused great interest from both academia and industry for mass production of graphene sheets. Electrochemically exfoliated graphene oxide (EGO) features a much better tunability than chemically EGO, or even than graphene obtained with ultrasonic exfoliation. Chemical and electrical properties of EGO can be modified extensively, thanks to its step-controllable oxidation process, varying the electrolytes and/or the applied potential. It is thus possible, using tunable electrochemical oxidation, to produce low-defect EGO sheets, featuring both good electric conductivity and good dispersibility in common solvents (e.g., acetonitrile or isopropanol). This greatly facilitates its application in several fields, for example, in flexible electronics. In this work, we correlate the dispersion behavior of EGO with its chemical properties using the relative Hansen solubility parameter, zeta potential values, X-ray photoemission spectroscopy, and Raman analysis. A surface morphology study by atomic force microscopy and transmission electron microscopy analyses also reveals that EGO sheets are multiple structures of (partially oxidized) graphene bilayers. Conductive EGO films could be easily prepared by vacuum filtration on different substrates, obtaining electrical conductivity values of up to ∼104 S/m with no need for further reduction procedures.
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