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Sonal Maroo, Yun Yu, [Takashi Taniguchi](https://orcid.org/0000-0002-1467-3105), [Kenji Watanabe](https://orcid.org/0000-0003-3701-8119), D. Kwabena Bediako

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[Decoupling Effects of Electrostatic Gating on Electronic Transport and Interfacial Charge-Transfer Kinetics at Few-Layer Molybdenum Disulfide](https://mdr.nims.go.jp/datasets/55a30d08-7d00-4e61-b566-97d3499110a2)

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Decoupling Effects of Electrostatic Gating on Electronic Transport and Interfacial Charge-Transfer Kinetics at Few-Layer Molybdenum DisulfideDecoupling Effects of Electrostatic Gating on Electronic Transportand Interfacial Charge-Transfer Kinetics at Few-Layer MolybdenumDisulfideSonal Maroo, Yun Yu, Takashi Taniguchi, Kenji Watanabe, and D. Kwabena Bediako*Cite This: ACS Nanosci. Au 2023, 3, 204−210 Read OnlineACCESS Metrics & More Article Recommendations *sı Supporting InformationABSTRACT: The electronic properties of electrode materials playa crucial role in defining their electrochemical behavior in energyconversion and storage devices. The assembly of van der Waalsheterostructures and fabrication into mesoscopic devices enable thedependence of an electrochemical response on electronic propertiesto be systematically interrogated. Here, we evaluate the effect ofcharge carrier concentration on heterogeneous electron transfer atfew-layer MoS2 electrodes by combining spatially resolved electro-chemical measurements with field-effect electrostatic manipulationof band alignment. Steady-state cyclic voltammograms and finite-element simulations reveal a strong modulation of the measuredelectrochemical response for outer-sphere charge transfer at theelectrostatic gate voltage. In addition, spatially resolved voltammetric responses, obtained at a series of locations at the surface offew-layer MoS2, reveal the governing role of in-plane charge transport on the electrochemical behavior of 2D electrodes, especiallyunder conditions of low carrier densities.KEYWORDS: SECCM, electrostatic gating, field-effect transistor, 2D MoS2, electrochemistryIncreasing societal energy demand requires the developmentof systems that efficiently interconvert electrical andchemical energy.1 Since electron transfer and electrontransport constitute key steps in these interfacial processes,2,3a deep understanding of the factors that underpin heteroge-neous electron transfer and chemical reactivity is required.Marcus theory4 provides a powerful framework for under-standing homogeneous outer-sphere electron-transfer reactionsbetween two chemical species. Likewise, Gerischer’s formula-tion5,6 describes the heterogeneous ET rate constant, kET, inthe weak coupling (outer-sphere) limit. For a reductionreaction, kET is expressed ask f W( ) ( ) ( ) ( , ) dET n ox=+where νn is the nuclear frequency factor, ε(ϵ) is theproportionality function, f(ϵ) is the Fermi function, ρ(ϵ) isthe density of states of the electrode, Wox(λ, ϵ) is theprobability density function of the reactant (oxidized species,ox), and λ is the reorganization energy. Schmickler’s theory forelectrocatalysis describes how electrochemical reactions in thestrong-coupling (inner-sphere) limit, involving the adsorptionof an intermediate at the electrode, are also significantlyimpacted by the structure and dispersion of the electronicbands in the electrode near the Fermi level, ϵF.7 Indeed, severalstudies have reported the amplification of the interfacialcharge-transfer processes caused by defects, edge sites, andgrain boundaries on the electrode surface,8−10 which can beattributed to the localized enhancement in electronic stateswithin their proximity to ϵF. These theoretical andexperimental studies underscore that interfacial reactivitymay be strongly affected by modulating electronic structure.Field-effect transistors (FETs) are the essential components ofcontemporary electronics, serving as switches and amplifiers ina wide range of applications from smartphones and laptops tosensors and actuators.11−13 In these devices, an electric fieldapplied via a gate electrode (i.e., electrostatic “gating”) is usedto modulate the flow of current in the active semiconductorchannels. For bulk semiconductors, applying an electric fieldperturbation alters the alignment of ϵF with the conduction/valence bands (and consequently the charge-carrier density) atthe semiconductor−dielectric interface but not in the bulk ofthe material, producing the well-known “band bending”effect.14 In low-dimensional semiconductors, including two-Received: December 29, 2022Revised: February 14, 2023Accepted: February 15, 2023Published: February 20, 2023Letterpubs.acs.org/nanoau© 2023 The Authors. Published byAmerican Chemical Society204https://doi.org/10.1021/acsnanoscienceau.2c00064ACS Nanosci. Au 2023, 3, 204−210Downloaded via NATL INST FOR MATLS SCIENCE (NIMS) on June 24, 2023 at 02:20:33 (UTC).See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.https://pubs.acs.org/action/doSearch?field1=Contrib&text1="Sonal+Maroo"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Yun+Yu"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Takashi+Taniguchi"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Kenji+Watanabe"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="D.+Kwabena+Bediako"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/showCitFormats?doi=10.1021/acsnanoscienceau.2c00064&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?goto=articleMetrics&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?goto=recommendations&?ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?goto=supporting-info&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=tgr1&ref=pdfhttps://pubs.acs.org/toc/anaccx/3/3?ref=pdfhttps://pubs.acs.org/toc/anaccx/3/3?ref=pdfhttps://pubs.acs.org/toc/anaccx/3/3?ref=pdfhttps://pubs.acs.org/toc/anaccx/3/3?ref=pdfpubs.acs.org/nanoau?ref=pdfhttps://pubs.acs.org?ref=pdfhttps://pubs.acs.org?ref=pdfhttps://doi.org/10.1021/acsnanoscienceau.2c00064?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-ashttps://pubs.acs.org/nanoau?ref=pdfhttps://pubs.acs.org/nanoau?ref=pdfhttps://creativecommons.org/licenses/by/4.0/https://creativecommons.org/licenses/by/4.0/https://acsopenscience.org/open-access/licensing-options/https://pubs.acs.org/page/policy/editorchoice/index.htmldimensional (2D) layers, electrostatic gating controls the bandalignments and densities of charge carriers throughout thematerial.15−17 2H-Molybdenum disulfide is a van der Waals(vdW) layered semiconductor with an electronic band gap of1.29 eV for bulk crystals and 1.8 eV in the monolayerlimit.18−20 Applying an electric field destabilizes the electronicbands with respect to ϵF, thereby altering the density ofelectronic states at ϵF as depicted in Figure 1a. The electronicproperty manipulation by this FET approach is highlycontrollable and therefore can provide a powerful means ofsystematically studying the influence of the density ofelectronic states on interfacial charge transfer kinetics thatmay be explained in the framework of the Marcus−Gerischermodel; the applied electrostatic gate controls the alignment ofthe band edges with respect to ϵF, and the electrochemicalpolarization generally controls the alignment of ϵF with respectto the solution redox couple (Figure 1b), although we notethat the electrochemical polarization can also further gate thesemiconductor.21,22Along these lines, previous studies have demonstrated thatthe heterogeneous charge-transfer kinetics at MoS2 monolayerscan be strongly modulated by applying an external electric fieldon the working electrodes,23,24 allowing charge-transferkinetics at monolayer MoS2 electrodes to be continuouslyand reversibly tuned from irreversible to nearly reversible(controlling the standard rate constant over 100-fold) with anapplied bottom-gate bias (VBG). Changes in electronicconductivity with electrostatic gating13,22,25 have also beenimplicated in affecting the interfacial reactivity. The surfaceconductance of MoS2 crystals has been strongly correlated withelectrocatalytic activity in electrochemical systems via a “self-gating” effect of the electrochemical polarization itself thatproduces a highly conductive surface.22,25 Together, thesestudies suggest that in an electrochemical system involvingsemiconducting electrodes, electrostatic gating (whether by theelectrolyte itself or a solid-state gate) can affect both intrinsicinterfacial electrokinetic behavior (as described formally by theMarcus−Gerischer equation) and in-plane electronic transport(conductivity), resulting in the net electrochemical response ofthe system. However, these effects have yet to be deconvolutedin a single set of experiments.Here we decouple the effects of in-plane charge transportand intrinsic electrokinetics by employing the scanningelectrochemical cell microscopy (SECCM) technique26,27 inan FET configuration. Our FET-SECCM approach enables theacquisition of electrochemical measurements exclusively inselect nanoscale regions of the MoS2 basal plane while keepingthe remainder of the flake dry and isolated from concomitantelectrostatic gating and conductivity changes by the electro-chemical polarization itself; instead, the conductivity of theflake is controlled by the separate electrostatic gate. We obtainspatially resolved voltammetric responses at a series oflocations at the surface of few-layer MoS2 as a function ofthe gating voltage. Our results reveal the crucial role of in-planecharge transport in governing the electrochemical responses of2D semiconducting electrodes, especially under conditions oflow carrier densities. The experimental approach and resultspresented here also emphasize the versatility of 2D materialsand vdW heterostructures as platforms for probing thephysicochemical principles that underpin interfacial electron-transfer reactions.The atomically thin MoS2, graphene, and boron nitride(hBN) flakes used in this work were mechanically exfoliatedonto SiO2 (285 nm)/Si substrates from their bulk crystalsusing the Scotch tape method.28,29 Flake thicknesses wereevaluated using optical contrast (SI Figure 1)30,31 and atomicforce microscopy, AFM (SI Figure 2). The thicknesses ofMoS2 flakes were verified using confocal Raman spectroscopyand photoluminescence spectroscopy (SI Figure 3). Specifi-cally, monolayers of MoS2 were identified by their strongphotoluminescence that arises from a direct band gap in themonolayer limit.18,32,33 In all electrochemical measurements,the MoS2 electrodes were fabricated in a field-effect transistor(FET) configuration, as depicted in Figure 2a. Graphite, hBN,and MoS2 flakes were sequentially stacked over each other byusing the vdW dry-transfer method.34 Further details onsample preparation are provided in the Supporting Informa-tion. MoS2 flakes with thicknesses of one to three layers wereassembled on top of an hBN crystal (20−50 nm) as anatomically flat dielectric and a graphite flake as the bottom gateelectrode. Figure 2b shows an optical micrograph of a typicalvdW heterostructure MoS2-based FET device used in thiswork.The voltage (VBG) applied to the graphite bottom gate wasused to alter the carrier density and exert control over the bandalignment. Specifically, the position of ϵF shifts either towardor away from the conduction band edge when VBG ismodulated as illustrated in Figure 1a. Figure 2c shows thesource-to-drain current profile obtained for different VBGvalues from −0.25 to +2.0 V. The observation of substantialIDS at VBG = 0 V implies that our MoS2 flakes used in thesedevices are n-doped possibly due to S vacancies, as is typicallythe case in transition-metal dichalcogenides.35 This assertion isfurther confirmed by the A- and B-exciton peak intensity ratiosobtained from the PL spectra (SI Figure 3b). Figure 2c showsthat, as expected, the electrical conductance, G, of the MoS2layers in these devices (G = IDS/VDS) increases with VBG,corresponding to electron accumulation at MoS2. G saturatesat higher VBG as ϵF resides well within the conduction band(Figure 2c inset).Figure 1. (a) Illustration of the shift in the band edge positions of asemiconducting material relative to ϵF upon applying an electrostaticgate voltage, VBG. (b) “Gerischer” schematic illustrating ϵF of thesemiconducting electrode in relation to the probability distributionsof occupied (Wred) and empty (Wox) states in solution at equilibriumand after applying an electrostatic gate voltage, VBG, followed by acathodic overpotential, η.ACS Nanoscience Au pubs.acs.org/nanoau Letterhttps://doi.org/10.1021/acsnanoscienceau.2c00064ACS Nanosci. Au 2023, 3, 204−210205https://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig1&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig1&ref=pdfpubs.acs.org/nanoau?ref=pdfhttps://doi.org/10.1021/acsnanoscienceau.2c00064?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asIn an electrochemical measurement for such an FET device,we would expect that in addition to tuning the conductance,the position of ϵF controlled by VBG would also affect theextent of overlap between filled electronic states of thesemiconductor electrode and the probability distributionfunctions of redox molecules residing in an electrolyte incontact with the semiconductor (Figure 1b). Therefore, in anelectrochemical measurement, we would also expect VBG tomodulate the intrinsic interfacial electron-transfer kinetics. Toprobe this effect, we performed SECCM measurements ofMoS2-based devices in the FET configuration. SECCM is ascanning probe technique that enables the interrogation ofelectron-transfer reactions at the nanoscale using an electro-lyte-filled nanopipette that is positioned/scanned over thesample, allowing a micro/nanoelectrochemical cell to beestablished by contact of the electrolyte meniscus at the baseof the pipette and the sample surface.26,27 As depicted inFigure 3a, we employed quartz nanopipette probes of diameter∼500 nm (SI Figure 4) that were filled with an aqueouselectrolyte of 1 mM hexaammineruthenium(III) chloride and100 mM potassium chloride to make meniscus contact withthe gate-tunable MoS2 surface, creating an enclosed electro-chemical cell in which localized voltammetry is performed for aseries of VBG values. (See the Supporting Information foradditional details of the measurement.) The radii and taperangles of nanopipettes were determined from transmissionelectron micrographs (SI Figure 4). Figure 3b shows an opticalmicrograph of a monolayer MoS2 device measured in thismanner, using an hBN flake of 20 nm thickness as the gatedielectric.Experimental SECCM cyclic voltammograms of Ru-(NH3)63+ reduction obtained with nanopipettes probing thecenter of the gated monolayer MoS2 flake are shown on the leftof Figure 3c. Initially, even at VBG = 0 V, the cyclicvoltammogram of Ru(NH3)63+ exhibits nearly reversiblecharacteristics, which are attributed to the pre-existing n-doping of MoS2 discussed above. As VBG is increased to 0.25 V,signifying further electron doping, the reaction shows ameasurable enhancement in the apparent interfacial kinetics,displaying a fully electrochemically reversible response, withthe plateau (diffusion-limited) current density equaling that ofbulk graphite (see SI Figure 5). As VBG is varied from 0.25 to−0.75 V, which involves p-doping (or equivalently, a reductionin n-doping), we observe an anodic shift of the oxidation waveand a decrease in the plateau current in each voltammogram(green to blue). A similar response was observed in the case ofthe 1 mM ferrocene methanol redox couple (SI Figure 5a).This behavior can be ascribed to an upward shift in theconduction band edge position relative to ϵF. This shift of ϵFtoward the band gap necessarily reduces the charge-carrierconcentration, which would substantially impact the electronicdensity of states available to mediate the interfacial electrontransfer as well as the energy state overlap integral betweenempty (occupied) states of Ru(NH3)63+(2+) and an occupied(empty) state of the same energy in the MoS2 electrode. Thesefactors would relate to the intrinsic electrokinetic behavior ofthe material. However, changes in the conductance of MoS2should also be expected.To understand the contributions of intrinsic electrokineticsas well as electronic transport to the electrochemical responses,we used finite-element simulations (COMSOL Multiphysicsv.5.6)36 to model the voltammetric responses and estimateelectrochemical rate constants (k0) and conductance values(G) in our system (SI Figures 6−8). The axisymmetricgeometry of the electrochemical cell was modeled with acylindrical meniscus and a nanopipette, with dimensionsdetermined from TEM images and the limiting currentdensity. The chemical and electron-transfer kinetics of theFigure 2. (a) Schematic of the FET device used for electrochemicalmeasurements in this work. VDS: drain−source potential. VBG:bottom-gate voltage. (b) Optical micrograph of a representativebottom-gated monolayer MoS2 FET device. (c) Two-probe IDS vs VDScurves as a function of VBG at a monolayer MoS2. The inset shows thetwo-probe conductance, G, measured as IDS/VDS. Figure 3. (a) Schematic of a local voltammetric measurement in theSECCM setup. (b) Optical micrograph of a bottom-gated monolayerMoS2 electrode (hBN thickness: 20 nm). (c) Left: experimental cyclicvoltammograms of 1 mM Ru(NH3)63+ in 0.1 M KCl solution as afunction of VBG. Scan rate: 200 mV/s. Right: simulated voltammo-grams using parameters in Table 1.ACS Nanoscience Au pubs.acs.org/nanoau Letterhttps://doi.org/10.1021/acsnanoscienceau.2c00064ACS Nanosci. Au 2023, 3, 204−210206https://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig2&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig3&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig3&ref=pdfpubs.acs.org/nanoau?ref=pdfhttps://doi.org/10.1021/acsnanoscienceau.2c00064?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asredox couples Ru(NH3)6+3/+2 and FcMeOH3+/2+ weremodeled using the Nernst−Planck model and Butler−Volmerequations. The in-plane resistance of the electrode was takeninto account by modeling it as a resistive film. The initialguesses of G were informed from the measurements describedin Figure 2c, after which k0 and G were then iterativelyoptimized. The simulated voltammograms were compared toexperimental data to refine the simulation parameters. Furtherdetails on the finite-element simulation parameters and theprocedures for estimating kinetic and transport parameters canbe found in the Supporting Information. Table 1 details theresultant dependence of k0 and G on VBG for Ru(NH3)6+3/+2.For comparisons among devices, we also compute and tabulatethe electric field = VBG/dhBN, where dhBN is the thickness ofthe hBN dielectric used in device fabrication (determined fromAFM, SI Figure 2), which typically varies from device todevice. These data suggest that the response of the system toelectrostatic gating involves the intertwined effects of changingconductivity, and hence conductance, and the intrinsicinterfacial kinetics, owing to modulation in electronic densitiesof states as well as the overlap between the energy states of thereactant and electrode.These insights notwithstanding, a stronger segregation of thecontributions of interfacial kinetics and electronic transport onthe electrochemical response required a measurement schemethat provided greater orthogonality in the manipulation of Gand k0. To gain a deeper understanding of the independentimpact of G on the overall electrochemical response, weacquired spatially resolved voltammetric responses by position-ing nanopipettes filled with 2.0 mM hexaammineruthenium-(III) chloride, 1.0 mM ferrocene methanol, and 100 mMaqueous potassium chloride at a series of locations at thesurface of a bottom-gated trilayer MoS2 electrode (Figure 4a).We note thatG AL=where σ is the conductivity, L is the length of the channel awayfrom the electrical contact, and A is the cross-sectional area ofthe channel. We can then define a surface conductivity, σ′, asσ′ = σA. Accordingly, for a fixed VBG, σ′ would remainconstant, yet as we move the pipette from one position toanother, G would change as L is varied. Figure 4b shows cyclicvoltammograms of ferrocene methanol and hexaammine-ruthenium(III/II) obtained at a series of points at the MoS2surface with changing distances of 1.4, 9.4, and 16.6 μm fromthe point of SECCM measurement to the terminal graphitecontact.At VBG = 0 V, voltammograms of FcMeOH and Ru(NH3)63+exhibit electrochemically reversible responses at all threelocations, consistent with an MoS2 surface that is natively n-doped with sufficient charge carriers to mediate theheterogeneous electron-transfer reactions and also conductelectrical charge without a substantial ohmic drop across theflake. As VBG was varied toward −1.5 V, hole doping via theelectric field effect caused pronounced differences in theelectrochemical responses at different locations at the MoS2surface. The voltammogram at location 1, 1.4 μm away fromthe graphite contact, remained largely unaffected, exhibitingelectrochemical reversibility, while the voltammogram atlocation 3, ∼17 μm away from the graphite contact, displayeda substantial decrease in the Faradaic current associated withboth FcMeOH and Ru(NH3)63+, producing ostensiblyirreversible responses by VBG = −1.50 V.Table 1. Values of G and k0 for Ru(NH3)6+3/+2 from theSimulation of CVs at Monolayer MoS2VBG (V) (mV/nm) k0 (cm/s) G (nS)0.25 12.5 0.6 ≥2.50.0 0 0.4 ≥2.0−0.25 −12.5 0.2 0.43−0.50 −25.0 0.02 0.09−0.75 −37.5 0.004 0.05Figure 4. (a) Optical image of a gated three-layer MoS2 electrode using an hBN dielectric of thickness 40 nm. Marked spots 1−3 represent thelocations probed by SECCM, varying the distance, L, from measurement to the graphite electric contact. (b) Cyclic voltammograms of 1 mMFcMeOH and 2 mM Ru(NH3)63+ in 0.1 M KCl solution as a function of VBG at locations 1 (left), 2 (middle), and 3 (right). Scan rate = 200 mV/s.(c) Simulated cyclic voltammograms (scan rate = 200 mV/s) using the values of k0 and G are detailed in Table 2. The effects of VBG areincorporated via a changing surface conductivity, σ' = σA.ACS Nanoscience Au pubs.acs.org/nanoau Letterhttps://doi.org/10.1021/acsnanoscienceau.2c00064ACS Nanosci. Au 2023, 3, 204−210207https://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig4&ref=pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?fig=fig4&ref=pdfpubs.acs.org/nanoau?ref=pdfhttps://doi.org/10.1021/acsnanoscienceau.2c00064?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-asThe set of measurements displayed in Figure 4b provides ameans of systematically probing the effects of electrostaticgating on conductivity and intrinsic charge-transfer kinetics byiterative comparison with finite-element simulations. Insimulations, the effect of electrostatic gating was incorporatedthrough a VBG-dependent but location-independent set of k0and σ′ values while further considering changes to the in-planeelectronic transport via a location-dependent (inverselyproportional to L) set of G values at each site. CV simulationswithin this framework (SI Figures 8 and 9) are instructive,revealing that at low conductance levels (G ≤ 0.05 nS)increasing k0 even by 2 orders of magnitude does notsubstantially influence the current profile. Instead, G over-whelmingly governs the rate of interfacial electron transfer inthis regime. However, as G increases, both G and k0 contributesubstantially to the overall electrochemical behavior. SI Figures8 and 9 show that ultimately for G ≥ 0.5 nS increasing Gfurther does not influence the current profile and k0 solelydetermines the overall interfacial electron-transfer rate.Against this backdrop, we iteratively optimized k0 and G toreproduce the experimental data in Figure 4b. The simulationparameters that were found to most closely replicate theexperimental data are detailed in Table 2, and the simulatedvoltammograms are presented in Figure 4c. We find goodreplication of the redox behavior for both FcMeOH andRu(NH3)63+/2+ using effectively identical k0 values, which arethe singular k0 values presented in Table 2. We note that forthe reasons described above, in some locations and at somevalues of VBG, we can rigorously provide only lower-limit valuesof k0 and/or G. Nevertheless, these results provide aninstructive illustration of the interplay between in-plane chargetransport and intrinsic interfacial electrokinetics.In conclusion, electrostatic gating of semiconductingelectrodes results in the modulation of intrinsic electro-chemical kinetics as well as the electronic transport properties.The FET scheme provides an orthogonal knob to controlinterfacial charge transfer, distinct from the applied electro-chemical bias, but the effects of in-plane transport must beconsidered. This work demonstrates that vdW heterostructuresof few-layer MoS2, graphite, and hBN provide a distinctiveplatform for interrogating charge-transfer kinetics andelectronic transport effects when coupled with SECCM.SECCM enables the exclusion of electrochemical gating effectson in-plane transport, allowing electronic transport to becontrolled exclusively by the solid-state gate. Combinedexperimental measurements and finite-element simulationsshow how in-plane charge transport has a pronounced effecton the apparent electron-transfer kinetics at semiconductingelectrodes, especially at lower charge-carrier densities.■ ASSOCIATED CONTENT*sı Supporting InformationThe Supporting Information is available free of charge athttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064.General methods, additional experimental data, andfinite element simulations (PDF)■ AUTHOR INFORMATIONCorresponding AuthorD. Kwabena Bediako − Department of Chemistry, Universityof California, Berkeley, California 94720, United States;Chemical Sciences Division, Lawrence Berkeley NationalLaboratory, Berkeley, California 94720, United States;orcid.org/0000-0003-0064-9814; Email: bediako@berkeley.eduAuthorsSonal Maroo − Department of Chemistry, University ofCalifornia, Berkeley, California 94720, United StatesYun Yu − Department of Chemistry, University of California,Berkeley, California 94720, United States; PresentAddress: Department of Chemistry, George MasonUniversity, Fairfax, Virginia 22030, United States;orcid.org/0000-0002-0204-1012Takashi Taniguchi − International Center for MaterialsNanoarchitectonics, National Institute for Materials Science,Tsukuba 305-0044, Japan; orcid.org/0000-0002-1467-3105Kenji Watanabe − Research Center for Functional Materials,National Institute for Materials Science, Tsukuba 305-0044,Japan; orcid.org/0000-0003-3701-8119Complete contact information is available at:https://pubs.acs.org/10.1021/acsnanoscienceau.2c00064Author ContributionsCRediT: Sonal Maroo conceptualization (equal), datacuration (lead), formal analysis (equal), writing-original draft(equal), writing-review & editing (equal); Yun Yu conceptu-alization (equal), data curation (equal), writing-review &editing (equal); Takashi Taniguchi resources (equal); KenjiWatanabe resources (equal); D. Kwabena Bediako conceptu-alization (equal), funding acquisition (lead), project admin-istration (lead), writing-review & editing (equal).NotesThe authors declare no competing financial interest.Table 2. Location-Dependent Values of G and k0 for Electrochemical Responses of FcMeOH and Ru(NH3)63+/2+ at TrilayerMoS2G (nS) G (nS) G (nS)VBG (V) (mV/nm) k0 (cm/s) at L = 1.4 μm at L = 9.4 μm at L = 17 μm0.5 12.5 ≥0.1 ≥2.5 ≥2.5 ≥2.50 0 ≥0.1 ≥2.5 ≥2.5 ≥2.5−0.5 −12.5 ≥0.1 ≥2.5 ≥2.5 ≥2.5−1.0 −25.0 0.085 ± 0.005 ≥2.5 0.55 ± 0.06 0.290 ± 0.003−1.5 −37.5 0.055 ± 0.002 ≥2.5 0.083 ± 0.003 0.047 ± 0.004ACS Nanoscience Au pubs.acs.org/nanoau Letterhttps://doi.org/10.1021/acsnanoscienceau.2c00064ACS Nanosci. Au 2023, 3, 204−210208https://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?goto=supporting-infohttps://pubs.acs.org/doi/suppl/10.1021/acsnanoscienceau.2c00064/suppl_file/ng2c00064_si_001.pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="D.+Kwabena+Bediako"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://orcid.org/0000-0003-0064-9814https://orcid.org/0000-0003-0064-9814mailto:bediako@berkeley.edumailto:bediako@berkeley.eduhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Sonal+Maroo"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://pubs.acs.org/action/doSearch?field1=Contrib&text1="Yun+Yu"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://orcid.org/0000-0002-0204-1012https://orcid.org/0000-0002-0204-1012https://pubs.acs.org/action/doSearch?field1=Contrib&text1="Takashi+Taniguchi"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://orcid.org/0000-0002-1467-3105https://orcid.org/0000-0002-1467-3105https://pubs.acs.org/action/doSearch?field1=Contrib&text1="Kenji+Watanabe"&field2=AllField&text2=&publication=&accessType=allContent&Earliest=&ref=pdfhttps://orcid.org/0000-0003-3701-8119https://pubs.acs.org/doi/10.1021/acsnanoscienceau.2c00064?ref=pdfpubs.acs.org/nanoau?ref=pdfhttps://doi.org/10.1021/acsnanoscienceau.2c00064?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-as■ ACKNOWLEDGMENTSWe thank K. Zhang for helpful discussions. This material isbased upon work supported by the U.S. Department of Energy,Office of Science, Office of Basic Energy Sciences under awardno. DE-SC0021049. Confocal Raman spectroscopy wassupported by a Defense University Research InstrumentationProgram grant through the Office of Naval Research underaward no. N00014-20-1-2599 (D.K.B.). Other instrumentationused in this work was supported by grants from the CanadianInstitute for Advanced Research (CIFAR−Azrieli GlobalScholar, award no. GS21-011), the Gordon and Betty MooreFoundation EPiQS Initiative (award no. 10637), the W. M.Keck Foundation (award no. 993922), and the 3M Foundationthrough the 3M Non-Tenured Faculty Award (no. 67507585).K.W. and T.T. acknowledge support from the Japan Society forthe Promotion of Science, Grants-in-Aid for ScientificResearch (KAKENHI; grant nos. 19H05790, 20H00354, and21H05233).■ REFERENCES(1) Ding, Q. 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