High-Mobility Flexible Transistors with Low-Temperature Solution-Processed Tungsten Dichalcogenides

The investigation of high-mobility two-dimensional (2D) flakes beyond molybdenum disulfide (MoS2) will be necessary to create a library of high-mobility solution-processed networks that conform to substrates and remain functional over thousands of bending cycles. Here we report electrochemical exfoliation of large-aspect-ratio (>100) semiconducting flakes of tungsten diselenide (WSe2) and tungsten disulfide (WS2) as well as MoS2 as a comparison. We use Langmuir–Schaefer coating to achieve highly aligned and conformal flake networks, with minimal mesoporosity (∼2–5%), at low processing temperatures (120 °C) and without acid treatments. This allows us to fabricate electrochemical transistors in ambient air, achieving average mobilities of μMoS2 ≈ 11 cm2 V–1 s–1, μWS2 ≈ 9 cm2 V–1 s–1, and μWSe2 ≈ 2 cm2 V–1 s–1 with a current on/off ratios of Ion/Ioff ≈ 2.6 × 103, 3.4 × 103, and 4.2 × 104 for MoS2, WS2, and WSe2, respectively. Moreover, our transistors display threshold voltages near ∼0.4 V with subthreshold slopes as low as 182 mV/dec, which are essential factors in maintaining power efficiency and represent a 1 order of magnitude improvement in the state of the art. Furthermore, the performance of our WSe2 transistors is maintained on polyethylene terephthalate (PET) even after 1000 bending cycles at 1% strain.

[1]  D. Rhee,et al.  All inkjet-printed electronics based on electrochemically exfoliated two-dimensional metal, semiconductor, and dielectric , 2022, npj 2D Materials and Applications.

[2]  A. Radenović,et al.  High Performance Semiconducting Nanosheets via a Scalable Powder-Based Electrochemical Exfoliation Technique. , 2022, ACS nano.

[3]  J. Coleman,et al.  Highly Conductive Networks of Silver Nanosheets. , 2022, Small.

[4]  X. Duan,et al.  Highly stretchable van der Waals thin films for adaptable and breathable electronic membranes , 2022, Science.

[5]  J. Coleman,et al.  Cyclic production of biocompatible few-layer graphene ink with in-line shear-mixing for inkjet-printed electrodes and Li-ion energy storage , 2022, npj 2D Materials and Applications.

[6]  D. Rhee,et al.  All‐Solution‐Processed Van der Waals Heterostructures for Wafer‐Scale Electronics , 2021, Advanced materials.

[7]  V. Nicolosi,et al.  Charge transport mechanisms in inkjet-printed thin-film transistors based on two-dimensional materials , 2021, Nature Electronics.

[8]  R. Chung,et al.  Low Subthreshold Slope AlGaN/GaN MOS-HEMT with Spike-Annealed HfO2 Gate Dielectric , 2021, Micromachines.

[9]  Han‐Ki Kim,et al.  Area-Selective Chemical Doping on Solution-Processed MoS2 Thin-Film for Multi-Valued Logic Gates. , 2021, Nano letters.

[10]  J. Coleman,et al.  The electrical conductivity of solution-processed nanosheet networks , 2021, Nature Reviews Materials.

[11]  Young-Jin Kwack,et al.  Bottom-up water-based solution synthesis for a large MoS2 atomic layer for thin-film transistor applications , 2021, npj 2D Materials and Applications.

[12]  X. Duan,et al.  Two-dimensional van der Waals thin film transistors as active matrix for spatially resolved pressure sensing , 2021, Nano Research.

[13]  Shayan Seyedin,et al.  Fibre electronics: towards scaled-up manufacturing of integrated e-textile systems. , 2021, Nanoscale.

[14]  M. Lanza,et al.  Inkjet Printed Circuits with 2D Semiconductor Inks for High‐Performance Electronics , 2021, Advanced Electronic Materials.

[15]  M. Terrones,et al.  Quantification and Healing of Defects in Atomically Thin Molybdenum Disulfide: Beyond the Controlled Creation of Atomic Defects. , 2021, ACS nano.

[16]  J. Coleman,et al.  Covalently interconnected transition metal dichalcogenide networks via defect engineering for high-performance electronic devices , 2021, Nature Nanotechnology.

[17]  Qinghua Zhang,et al.  One-step synthesis of single-site vanadium substitution in 1T-WS2 monolayers for enhanced hydrogen evolution catalysis , 2021, Nature Communications.

[18]  J. Redwing,et al.  Benchmarking monolayer MoS2 and WS2 field-effect transistors , 2021, Nature communications.

[19]  H. Lv,et al.  Ion‐Gated Transistor: An Enabler for Sensing and Computing Integration , 2020, Adv. Intell. Syst..

[20]  Congli He,et al.  Large-scale flexible and transparent electronics based on monolayer molybdenum disulfide field-effect transistors , 2020, Nature Electronics.

[21]  J. Coleman,et al.  Effect of the Gate Volume on the Performance of Printed Nanosheet Network-Based Transistors , 2020 .

[22]  Zhaoqian Xie,et al.  Flexible and stretchable metal oxide nanofiber networks for multimodal and monolithically integrated wearable electronics , 2020, Nature Communications.

[23]  B. Derby,et al.  Tiled Monolayer Films of 2D Molybdenum Disulfide Nanoflakes Assembled at Liquid/Liquid Interfaces , 2020, ACS applied materials & interfaces.

[24]  Hiroki Sugiura,et al.  Robust, high-performance n-type organic semiconductors , 2020, Science Advances.

[25]  G. Malliaras.  Organic electrochemical transistors , 2020 .

[26]  J. Coleman,et al.  Length- and Thickness-Dependent Optical Response of Liquid-Exfoliated Transition Metal Dichalcogenides , 2019, Chemistry of Materials.

[27]  M. Prato,et al.  High-Yield Preparation of Exfoliated 1T-MoS2 with SERS Activity , 2019, Chemistry of Materials.

[28]  P. Šiffalovič,et al.  Tailored Langmuir-Schaefer Deposition of Few-Layer MoS2 Nanosheet Films for Electronic Applications. , 2019, Langmuir : the ACS journal of surfaces and colloids.

[29]  J. Coleman,et al.  Equipartition of Energy Defines the Size-Thickness Relationship in Liquid-Exfoliated Nanosheets. , 2019, ACS nano.

[30]  Z. Cui,et al.  High-performance metal-oxide thin-film transistors based on inkjet-printed self-confined bilayer heterojunction channels , 2019, Journal of Materials Chemistry C.

[31]  C. Mattevi,et al.  Direct solution-phase synthesis of 1T’ WSe2 nanosheets , 2019, Nature Communications.

[32]  C. Mattevi,et al.  Direct solution-phase synthesis of 1T’ WSe2 nanosheets , 2019, Nature Communications.

[33]  Shibo Wang,et al.  High-performance p-type MoS2 field-effect transistor by toroidal-magnetic-field controlled oxygen plasma doping , 2019, 2D Materials.

[34]  Thomas M. Higgins,et al.  Electrolyte‐Gated n‐Type Transistors Produced from Aqueous Inks of WS2 Nanosheets , 2018, Advanced Functional Materials.

[35]  F. Torrisi,et al.  Graphene, related two-dimensional crystals and hybrid systems for printed and wearable electronics , 2018, Nano Today.

[36]  S. Pennycook,et al.  The origin of single photon emission in 2 D WSe 2 , 2018 .

[37]  B. Lüssem,et al.  Organic Electrochemical Transistors Based on Room Temperature Ionic Liquids: Performance and Stability , 2018, physica status solidi (a).

[38]  Yu Huang,et al.  Solution-processable 2D semiconductors for high-performance large-area electronics , 2018, Nature.

[39]  E. Fortunato,et al.  Papertronics: Multigate paper transistor for multifunction applications , 2018, Applied Materials Today.

[40]  Yang Han,et al.  Recent Progress in High‐Mobility Organic Transistors: A Reality Check , 2018, Advanced materials.

[41]  Matthew J. Catenacci,et al.  In-Place Printing of Carbon Nanotube Transistors at Low Temperature , 2018 .

[42]  V. Nicolosi,et al.  Solution processed thin film transistor from liquid phase exfoliated MoS 2 flakes , 2017 .

[43]  R. Sordan,et al.  Fully inkjet-printed two-dimensional material field-effect heterojunctions for wearable and textile electronics , 2017, Nature Communications.

[44]  Vasileios Koutsos,et al.  Controlled Layer Thinning and p‐Type Doping of WSe2 by Vapor XeF2 , 2017 .

[45]  H. Sebastian Seung,et al.  Trainable Weka Segmentation: a machine learning tool for microscopy pixel classification , 2017, Bioinform..

[46]  J. Coleman.  All-printed electrochemical thin-film transistors from networks of liquid-exfoliated nanosheets , 2017 .

[47]  J. Coleman,et al.  All-printed thin-film transistors from networks of liquid-exfoliated nanosheets , 2017, Science.

[48]  Duncan N. Johnstone,et al.  Microfluidization of Graphite and Formulation of Graphene-Based Conductive Inks , 2016, ACS nano.

[49]  Daniel Wolverson,et al.  Strain-induced phonon shifts in tungsten disulfide nanoplatelets and nanotubes , 2016 .

[50]  Xuan Cao,et al.  Fully Screen-Printed, Large-Area, and Flexible Active-Matrix Electrochromic Displays Using Carbon Nanotube Thin-Film Transistors. , 2016, ACS nano.

[51]  Jie Zhu,et al.  Improving Charge Mobility of Polymer Transistors by Judicious Choice of the Molecular Weight of Insulating Polymer Additive , 2016 .

[52]  J. Coleman,et al.  Electrochemical Applications of Two-Dimensional Nanosheets: The Effect of Nanosheet Length and Thickness , 2016 .

[53]  Vivek Subramanian,et al.  Fully High‐Speed Gravure Printed, Low‐Variability, High‐Performance Organic Polymer Transistors with Sub‐5 V Operation , 2016 .

[54]  Christoph Gadermaier,et al.  Production of Highly Monolayer Enriched Dispersions of Liquid-Exfoliated Nanosheets by Liquid Cascade Centrifugation. , 2016, ACS nano.

[55]  E. Yablonovitch,et al.  Near-unity photoluminescence quantum yield in MoS2 , 2015, Science.

[56]  Thomas M. Higgins,et al.  Avoiding Resistance Limitations in High-Performance Transparent Supercapacitor Electrodes Based on Large-Area, High-Conductivity PEDOT:PSS Films. , 2015, ACS applied materials & interfaces.

[57]  M. Minary‐Jolandan,et al.  Fabrication of MoS2 thin film transistors via selective-area solution deposition methods , 2015 .

[58]  Ankit Mahajan,et al.  Aerosol jet printed p- and n-type electrolyte-gated transistors with a variety of electrode materials: exploring practical routes to printed electronics. , 2014, ACS applied materials & interfaces.

[59]  Jiantong Li,et al.  Inkjet Printing of MoS2 , 2014 .

[60]  K. Sivula,et al.  Multiflake Thin Film Electronic Devices of Solution Processed 2D MoS2 Enabled by Sonopolymer Assisted Exfoliation and Surface Modification , 2014 .

[61]  Niall McEvoy,et al.  Edge and confinement effects allow in situ measurement of size and thickness of liquid-exfoliated nanosheets , 2014, Nature Communications.

[62]  Lei Zhang,et al.  Inkjet Printing Short‐Channel Polymer Transistors with High‐Performance and Ultrahigh Photoresponsivity , 2014, Advanced materials.

[63]  Tatsuya Shimoda,et al.  Rheology printing for metal-oxide patterns and devices , 2014 .

[64]  M. Calandra.  Chemically exfoliated single-layer MoS 2 : Stability, lattice dynamics, and catalytic adsorption from first principles , 2013, 1312.1702.

[65]  A. Yamano,et al.  V‐Shaped Organic Semiconductors With Solution Processability, High Mobility, and High Thermal Durability , 2013, Advanced materials.

[66]  P. H. Lau,et al.  Fully printed, high performance carbon nanotube thin-film transistors on flexible substrates. , 2013, Nano letters.

[67]  G. Eda,et al.  Lattice dynamics in mono- and few-layer sheets of WS2 and WSe2. , 2013, Nanoscale.

[68]  Shinhyuk Yang,et al.  An ‘aqueous route’ for the fabrication of low-temperature-processable oxide flexible transparent thin-film transistors on plastic substrates , 2013 .

[69]  L. Chu,et al.  Evolution of electronic structure in atomically thin sheets of WS2 and WSe2. , 2012, ACS nano.

[70]  Yong‐Young Noh,et al.  Flexible Complementary Logic Gates Using Inkjet-Printed Polymer Field-Effect Transistors , 2013, IEEE Electron Device Letters.

[71]  Qiyuan He,et al.  Fabrication of flexible MoS2 thin-film transistor arrays for practical gas-sensing applications. , 2012, Small.

[72]  Schuller,et al.  Raman spectroscopy of the interlayer shear mode in few-layer MoS2 flakes , 2012, 1205.1916.

[73]  T. Saito,et al.  Highly Uniform Thin-Film Transistors Printed on Flexible Plastic Films with Morphology-Controlled Carbon Nanotube Network Channels , 2012 .

[74]  Yoshihiro Iwasa,et al.  Ambipolar MoS2 thin flake transistors. , 2012, Nano letters.

[75]  A. Ferrari,et al.  Inkjet-printed graphene electronics. , 2011, ACS nano.

[76]  E. Fortunato,et al.  Complementary Metal Oxide Semiconductor Technology With and On Paper , 2011, Advanced materials.

[77]  A. Radenović,et al.  Single-layer MoS2 transistors. , 2011, Nature nanotechnology.

[78]  J. Coleman,et al.  Two-Dimensional Nanosheets Produced by Liquid Exfoliation of Layered Materials , 2011, Science.

[79]  Seth R. Marder,et al.  n‐Type Organic Semiconductors in Organic Electronics , 2010, Advanced materials.

[80]  Wei Zhang,et al.  Printed, sub-3V digital circuits on plastic from aqueous carbon nanotube inks. , 2010, ACS nano.

[81]  H. Ohta,et al.  Room-temperature fabrication of transparent flexible thin-film transistors using amorphous oxide semiconductors , 2004, Nature.

[82]  J. Wilson,et al.  The transition metal dichalcogenides discussion and interpretation of the observed optical, electrical and structural properties , 1969 .