Abstract
Two-dimensional semiconductors, such as molybdenum disulfide (MoS2), exhibit a variety of properties that could be useful in the development of novel electronic devices. However, nanopatterning metal electrodes on such atomic layers, which is typically achieved using electron beam lithography, is currently problematic, leading to non-ohmic contacts and high Schottky barriers. Here, we show that thermal scanning probe lithography can be used to pattern metal electrodes with high reproducibility, sub-10-nm resolution, and high throughput (105 μm2 h−1 per single probe). The approach, which offers simultaneous in situ imaging and patterning, does not require a vacuum, high energy, or charged beams, in contrast to electron beam lithography. Using this technique, we pattern metal electrodes in direct contact with monolayer MoS2 for top-gate and back-gate field-effect transistors. These devices exhibit vanishing Schottky barrier heights (around 0 meV), on/off ratios of 1010, no hysteresis, and subthreshold swings as low as 64 mV per decade without using negative capacitors or hetero-stacks.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
- Purchase on SpringerLink
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
Data availability
The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.
References
Allain, A., Kang, J., Banerjee, K. & Kis, A. Electrical contacts to two-dimensional semiconductors. Nat. Mater. 14, 1195–1205 (2015).
Garcia, R., Knoll, A. W. & Riedo, E. Advanced scanning probe lithography. Nat. Nanotech. 9, 577–587 (2014).
Desai, S. B. et al. MoS2 transistors with 1-nanometer gate lengths. Science 354, 99–102 (2016).
Radisavljevic, B., Radenovic, A., Brivio, J., Giacometti, V. & Kis, A. Single-layer MoS2 transistors. Nat. Nanotech. 6, 147–150 (2011).
Chhowalla, M., Jena, D. & Zhang, H. Two-dimensional semiconductors for transistors. Nat. Rev. Mater. 1, 1–15 (2016).
Lembke, D., Bertolazzi, S. & Kis, A. Single-layer MoS2 electronics. Acc. Chem. Res. 48, 100–110 (2015).
Xu, Y. et al. Contacts between two- and three-dimensional materials: ohmic, Schottky, and p–n heterojunctions. ACS Nano 10, 4895–4919 (2016).
Zhao, Y. et al. Doping, contact and interface engineering of two-dimensional layered transition metal dichalcogenides transistors. Adv. Funct. Mater. 27, 1603484 (2017).
Wang, W. et al. Controllable Schottky barriers between MoS2 and Permalloy. Sci. Rep. 4, 6928 (2014).
Yang, L. et al. Chloride molecular doping technique on 2D materials: WS2 and MoS2. Nano Lett. 14, 6275–6280 (2014).
Kappera, R. et al. Phase-engineered low-resistance contacts for ultrathin MoS2 transistors. Nat. Mater. 13, 1128–1134 (2014).
Farmanbar, M. & Brocks, G. Controlling the Schottky barrier at MoS2/metal contacts by inserting a BN monolayer. Phys. Rev. B 91, 161304 (2015).
Cui, X. et al. Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform. Nat. Nanotech. 10, 534–540 (2015).
Guimarães, M. H. et al. Atomically thin ohmic edge contacts between two-dimensional materials. ACS Nano 10, 6392–6399 (2016).
Leong et al. Low resistance metal contacts to MoS2 devices with nickel etched graphene electrodes. ACS Nano 9, 869–877 (2015).
Zan, R. et al. Control of radiation damage in MoS2 by graphene encapsulation. ACS Nano 7, 10167–10174 (2013).
Meyer, J. C. et al. Accurate measurement of electron beam induced displacement cross sections for single-layer graphene. Phys. Rev. Lett. 108, 196102 (2012).
Lehnert, T., Lehtinen, O., Algara–Siller, G. & Kaiser, U. Electron radiation damage mechanisms in 2D MoSe2. Appl. Phys. Lett. 110, 033106 (2017).
Imamura, G. & Saiki, K. Modification of graphene/SiO2 interface by UV-irradiation: effect on electrical characteristics. ACS Appl. Mater. Interfaces 7, 2439–2443 (2015).
Zhang, R., Chen, T., Bunting, A. & Cheung, R. Optical lithography technique for the fabrication of devices from mechanically exfoliated two-dimensional materials. Microelectron. Eng. 154, 62–68 (2016).
Ishigami, M., Chen, J. H., Cullen, W. G., Fuhrer, M. S. & Williams, E. D. Atomic structure of graphene on SiO2. Nano Lett. 7, 1643–1648 (2007).
Robinson, J. A. et al. Contacting graphene. Appl. Phys. Lett. 98, 053103 (2011).
Macintyre, D. S., Ignatova, O., Thoms, S. & Thayne, I. G. Resist residues and transistor gate fabrication. J. Vac. Sci. Technol. B 27, 2597–2601 (2009).
Kang, S., Movva, H. C. P., Sanne, A., Rai, A. & Banerjee, S. K. Influence of electron-beam lithography exposure current level on the transport characteristics of graphene field effect transistors. J. Appl. Phys. 119, 124502 (2016).
Lin, Y. C. et al. Graphene annealing: how clean can it be? Nano Lett. 12, 414–419 (2012).
Van Ngoc, H., Qian, Y., Han, S. K. & Kang, D. J. PMMA-etching-free transfer of wafer-scale chemical vapor deposition two-dimensional atomic crystal by a water soluble polyvinyl alcohol polymer method. Sci. Rep. 6, 33096 (2016).
Lin, Z. et al. Controllable growth of large-size crystalline MoS2 and resist-free transfer assisted with a Cu thin film. Sci. Rep. 5, 18596 (2015).
Albisetti, E. et al. Nanopatterning reconfigurable magnetic landscapes via thermally assisted scanning probe lithography. Nat. Nanotech. 11, 545–551 (2016).
Pires, D. et al. Nanoscale three-dimensional patterning of molecular resists by scanning probes. Science 328, 732–735 (2010).
Carroll, K. M. et al. Parallelization of thermochemical nanolithography. Nanoscale 6, 1299–1304 (2014).
Szoszkiewicz, R. et al. High-speed, sub-15 nm feature size thermochemical nanolithography. Nano Lett. 7, 1064–1069 (2007).
Wu, W. et al. High mobility and high on/off ratio field-effect transistors based on chemical vapor deposited single-crystal MoS2 grains. Appl. Phys. Lett. 102, 142106 (2013).
Kim, C. et al. Fermi level pinning at electrical metal contacts of monolayer molybdenum dichalcogenides. ACS Nano 11, 1588–1596 (2017).
Chen, J. R. et al. Control of Schottky barriers in single layer MoS2 transistors with ferromagnetic contacts. Nano Lett. 13, 3106–3110 (2013).
Kwon, J. et al. Thickness-dependent Schottky barrier height of MoS2 field-effect transistors. Nanoscale 9, 6151–6157 (2017).
Cui, X. et al. Low-temperature ohmic contact to monolayer MoS2by van der Waals bonded Co/h-BN electrodes. Nano Lett. 17, 4781–4786 (2017).
Ryu Cho, Y. K. et al. Sub-10 nanometer feature size in silicon using thermal scanning probe lithography. ACS Nano 11, 11890–11897 (2017).
Gottlieb, S. et al. Thermal scanning probe lithography for the directed self-assembly of block copolymers. Nanotechnology 28, 175301 (2017).
Lee, C. et al. Anomalous lattice vibrations of single and few-layer MoS2. ACS Nano 4, 2695–2700 (2010).
Castellanos-Gomez, A. et al. Laser-thinning of MoS2: on demand generation of a single-layer semiconductor. Nano Lett. 12, 3187–3192 (2012).
Li, H. et al. From bulk to monolayer MoS2: evolution of Raman scattering. Adv. Funct. Mater. 22, 1385–1390 (2012).
Liu, W., Sarkar, D., Kang, J., Cao, W. & Banerjee, K. Impact of contact on the operation and performance of back-gated monolayer MoS2 field-effect-transistors. ACS Nano 9, 7904–7912 (2015).
Childres, I. et al. Effect of electron-beam irradiation on graphene field effect devices. Appl. Phys. Lett. 97, 173109 (2010).
Parkin, W. M. et al. Raman shifts in electron-irradiated monolayer MoS2. ACS Nano 10, 4134–4142 (2016).
Ji, H. et al. Thickness-dependent carrier mobility of ambipolar MoTe2: Interplay between interface trap and Coulomb scattering. App. Phys. Lett. 110, 183501 (2017).
Das, S., Chen, H. Y., Penumatcha, A. V. & Appenzeller, J. High performance multilayer MoS2 transistors with scandium contacts. Nano Lett. 13, 100–105 (2013).
Popov, I., Seifert, G. & Tomanek, D. Designing electrical contacts to MoS2 monolayers: a computational study. Phys. Rev. Lett. 108, 156802 (2012).
Su, J., Feng, L., Zhang, Y. & Liu, Z. Defect induced gap states in monolayer MoS2 control the Schottky barriers of Pt-mMoS2 interfaces. Appl. Phys. Lett. 110, 161604 (2017).
Liu, Y., Stradins, P. & Wei, S.-H. Van der Waals metal–semiconductor junction: weak Fermi level pinning enables effective tuning of Schottky barrier. Sci. Adv. 2, 1–6 (2016).
Mott, N. F. Metal–insulator transition. Rev Mod Phys 40, 677–683 (1968).
Radisavljevic, B. & Kis, A. Mobility engineering and a metal–insulator transition in monolayer MoS2. Nat. Mater. 12, 815–820 (2013).
Schmidt, H. et al. Transport properties of monolayer MoS2 grown by chemical vapor deposition. Nano Lett. 14, 1909–1913 (2014).
Wang, J. et al. High mobility MoS2 transistor with low Schottky barrier contact by using atomic thick h-BN as a tunneling layer. Adv. Mater. 28, 8302–8308 (2016).
Li, S.-L. et al. Thickness scaling effect on interfacial barrier and electrical contact to two-dimensional MoS2 layers. ACS Nano 8, 12836–12842 (2014).
Tung, R. T. The physics and chemistry of the Schottky barrier height. Appl. Phys. Rev. 1, 011304 (2014).
Liu, H. et al. Switching mechanism in single-layer molybdenum disulfide transistors: an insight into current flow across Schottky barriers. ACS Nano 8, 1031–1038 (2014).
Baugher, B. W., Churchill, H. O., Yang, Y. & Jarillo-Herrero, P. Intrinsic electronic transport properties of high-quality monolayer and bilayer MoS2. Nano Lett. 13, 4212–4216 (2013).
English, C. D., Shine, G., Dorgan, V. E., Saraswat, K. C. & Pop, E. Improved contacts to MoS2 transistors by ultra-high vacuum metal deposition. Nano Lett. 16, 3824–3830 (2016).
Dai, Z., Wang, Z., He, X., Zhang, X.-X. & Alshareef, H. N. Large-area chemical vapor deposited MoS2 with transparent conducting oxide contacts toward fully transparent 2D electronics. Adv. Funct. Mater. 27, 1703119 (2017).
Si, M. et al. Steep-slope hysteresis-free negative capacitance MoS2 transistors. Nat. Nanotech. 13, 24–28 (2018).
Radisavljevic, B., Whitwick, M. B. & Kis, A. Integrated circuits and logic operations based on single-layer MoS2. ACS Nano 5, 9934–9938 (2011).
Zhu, Y. et al. Monolayer molybdenum disulfide transistors with single-atom-thick gates. Nano Lett. 18, 3807–3813 (2018).
Xie, L. et al. Graphene-contacted ultrashort channel monolayer MoS2 transistors. Adv. Mater. 29, 1702522 (2017).
Lembke, D. & Kis, A. Breakdown of high-performance monolayer MoS2 transistors. ACS Nano 6, 10070–10075 (2012).
Kang, K. et al. High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity. Nature 520, 656–660 (2015).
Rawlings, C., Duerig, U., Hedrick, J., Coady, D. & Knoll, A. Nanometer control of the markerless overlay process using thermal scanning probe lithography. In IEEE/ASME International Conference on Advanced Intelligent Mechatronics (AIM) 1670–1675 (IEEE, 2014).
Acknowledgements
The authors acknowledge support from the US Army Research Office (proposal number 69180-CH), the Office of Basic Energy Sciences of the US Department of Energy, the National Science Foundation, SwissLitho, and the European Union’s Horizon 2020 research and innovation programme under grant agreement number 705326 (project SWING). A.S.M.A. and D.S. acknowledge financial support from NSF-ECCS (grant number 1638598).
Author information
Authors and Affiliations
Contributions
X.Z., A.C., E.A. and X.L. patterned the metal electrodes by t-SPL. A.S.M.A. performed the electronic measurements on the t-SPL FETs. X.Z., E.A., X.L., A.S.M.A., D.S. and E.R. designed the electronic experiments and analysed the data on the t-SPL FETs. G.A. and X.L. fabricated and measured the EBL FETs. X.Z., M.S. and E.R. developed the two-polymer stack t-SPL method. W.J.Y. and J.H. designed and analysed the EBL data. T.T. and K.W. provided the h-BN samples. C.A. analysed the XPS data. A.C. and A.K. provided the WSe2 samples and contributed to the corresponding data analysis. B.S.L. and M.L. deposited Pd electrodes on t-SPL FETs. E.R. conceived and analysed all the experiments on t-SPL FETs. X.Z., A.C., E.A., G.A., J.H., D.S. and E.R. contributed to writing the article.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Sections 1–15, Supplementary Figures 1–24, and Supplementary Tables 1–3.
Supplementary Video 1
Real-time screenshot recording acquired during the patterning process on PPA, from the writing of the large pads (10 × 10 µm2 squares) to the small fingers (1.5 µm wide) lying on top of a monolayer CVD MoS2 flake. The number of frames is 81,258 (29 frames per second).
Rights and permissions
About this article
Cite this article
Zheng, X., Calò, A., Albisetti, E. et al. Patterning metal contacts on monolayer MoS2 with vanishing Schottky barriers using thermal nanolithography. Nat Electron 2, 17–25 (2019). https://doi.org/10.1038/s41928-018-0191-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41928-018-0191-0
This article is cited by
-
Deterministic grayscale nanotopography to engineer mobilities in strained MoS2 FETs
Nature Communications (2024)
-
Combining thermal scanning probe lithography and dry etching for grayscale nanopattern amplification
Microsystems & Nanoengineering (2024)
-
Highly reproducible van der Waals integration of two-dimensional electronics on the wafer scale
Nature Nanotechnology (2023)
-
Two-dimensional diamonds from sp2-to-sp3 phase transitions
Nature Reviews Materials (2022)
-
Bridging the gap between atomically thin semiconductors and metal leads
Nature Communications (2022)