Abstract
The ability to tune material properties using gating by electric fields is at the heart of modern electronic technology. It is also a driving force behind recent advances in two-dimensional systems, such as the observation of gate electric-field-induced superconductivity and metal–insulator transitions. Here, we describe an ionic field-effect transistor (termed an iFET), in which gate-controlled Li ion intercalation modulates the material properties of layered crystals of 1T-TaS2. The strong charge doping induced by the tunable ion intercalation alters the energetics of various charge-ordered states in 1T-TaS2 and produces a series of phase transitions in thin-flake samples with reduced dimensionality. We find that the charge-density wave states in 1T-TaS2 collapse in the two-dimensional limit at critical thicknesses. Meanwhile, at low temperatures, the ionic gating induces multiple phase transitions from Mott-insulator to metal in 1T-TaS2 thin flakes, with five orders of magnitude modulation in resistance, and superconductivity emerges in a textured charge-density wave state induced by ionic gating. Our method of gate-controlled intercalation opens up possibilities in searching for novel states of matter in the extreme charge-carrier-concentration limit.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 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
References
Imada, M., Fujimori, A. & Tokura, Y. Metal–insulator transitions. Rev. Mod. Phys. 70, 1039 (1998).
Ahn, C. H., Triscone, J-M. & Mannhart, J. Electric field effect in correlated oxide systems. Nature 424, 1015–1018 (2003).
Ahn, C. H. et al. Electrostatic modification of novel materials. Rev. Mod. Phys. 78, 1185–1212 (2006).
Glover, R. E. & Sherrill, M. D. Changes in superconducting critical temperature produced by electrostatic charging. Phys. Rev. Lett. 5, 248–250 (1960).
Mannhart, J., Bednorz, J. G., Müller, K. A. & Schlom, D. G. Electric field effect on superconducting YBa2Cu3O7−δ films. Z. Für Phys. B Condens. Matter 83, 307–311 (1991).
Ahn, C. H. et al. Electrostatic modulation of superconductivity in ultrathin GdBa2Cu3O7–x films. Science 284, 1152–1155 (1999).
Parendo, K. A. et al. Electrostatic tuning of the superconductor–insulator transition in two dimensions. Phys. Rev. Lett. 94, 197004 (2005).
Fazekas, P. & Tosatti, E. Electrical, structural and magnetic properties of pure and doped 1T-TaS2 . Phil. Mag. B 39, 229–244 (1979).
Kim, J-J., Yamaguchi, W., Hasegawa, T. & Kitazawa, K. Observation of Mott localization gap using low temperature scanning tunneling spectroscopy in commensurate 1T-TaS2 . Phys. Rev. Lett. 73, 2103–2106 (1994).
Zwick, F. et al. Spectral consequences of broken phase coherence in 1T-TaS2 . Phys. Rev. Lett. 81, 1058–1061 (1998).
Wilson, J. A., Di Salvo, F. J. & Mahajan, S. Charge-density waves and superlattices in the metallic layered transition metal dichalcogenides. Adv. Phys. 24, 117–201 (1975).
Scruby, C. B., Williams, P. M. & Parry, G. S. The role of charge density waves in structural transformations of 1T TaS2 . Philos. Mag. 31, 255–274 (1975).
Thomson, R. E., Burk, B., Zettl, A. & Clarke, J. Scanning tunneling microscopy of the charge-density-wave structure in 1T-TaS2 . Phys. Rev. B 49, 16899–16916 (1994).
Sipos, B. et al. From Mott state to superconductivity in 1T-TaS2 . Nature Mater. 7, 960–965 (2008).
Ritschel, T. et al. Pressure dependence of the charge density wave in 1T-TaS2 and its relation to superconductivity. Phys. Rev. B 87, 125135 (2013).
Ang, R. et al. Real-space coexistence of the melted Mott state and superconductivity in Fe-substituted 1T-TaS2 . Phys. Rev. Lett. 109, 176403 (2012).
Ang, R. et al. Superconductivity and bandwidth-controlled Mott metal–insulator transition in 1T-TaS2−xSex . Phys. Rev. B 88, 115145 (2013).
Misra, R., McCarthy, M. & Hebard, A. F. Electric field gating with ionic liquids. Appl. Phys. Lett. 90, 052905 (2007).
Ueno, K. et al. Electric-field-induced superconductivity in an insulator. Nature Mater. 7, 855–858 (2008).
Ye, J. T. et al. Liquid-gated interface superconductivity on an atomically flat film. Nature Mater. 9, 125–128 (2010).
Pillo, T. et al. Remnant Fermi surface in the presence of an underlying instability in layered 1T–TaS2 . Phys. Rev. Lett. 83, 3494–3497 (1999).
Spijkerman, A., de Boer, J. L., Meetsma, A., Wiegers, G. A. & van Smaalen, S. X-ray crystal-structure refinement of the nearly commensurate phase of 1T-TaS2 in (3+2)-dimensional superspace. Phys. Rev. B 56, 13757–13767 (1997).
Tidman, J. P. & Frindt, R. F. Resistivity of thin TaS2 crystals. Can. J. Phys. 54, 2306–2309 (1976).
Williams, P. M., Scruby, C. B., Clark, W. B. & Parry, G. S. Charge density waves in the layered transition metal dichalcogenides. J. Phys. Colloq. 37, C4-139–C4-150 (1976).
Moncton, D. E., DiSalvo, F. J., Axe, J. D., Sham, L. J. & Patton, B. R. Charge-density wave stacking order in 1T-Ta1–xZrxSe2: interlayer interactions and impurity (Zr) effects. Phys. Rev. B 14, 3432–3437 (1976).
Bulaevskii, L. N. & Khomskii, D. I. Three-dimensional ordering of charge-density waves in quasi-one-dimensional and layered crystals. J. Exp. Theor. Phys. 46, 608–615 (1977).
Walker, M. B. & Withers, R. L. Stacking of charge-density waves in 1T transition-metal dichalcogenides. Phys. Rev. B 28, 2766–2774 (1983).
Bovet, M. et al. Interplane coupling in the quasi-two-dimensional 1T-TaS2 . Phys. Rev. B 67, 125105 (2003).
Nakanishi, K. & Shiba, H. Theory of three-dimensional orderings of charge-density waves in 1T-TaX2 (X: S, Se). J. Phys. Soc. Jpn 53, 1103–1113 (1984).
Tanda, S., Sambongi, T., Tani, T. & Tanaka, S. X-ray study of charge density wave structure in 1T-TaS2 . J. Phys. Soc. Jpn 53, 476–479 (1984).
Whittingham, M. S. Lithium batteries and cathode materials. Chem. Rev. 104, 4271–4302 (2004).
Thompson, A. H. Electrochemical studies of lithium intercalation in titanium and tantalum dichalcogenides. Physica B+C 99, 100–106 (1980).
Li, Z. J., Gao, B. F., Zhao, J. L., Xie, X. M. & Jiang, M. H. Effect of electrolyte gating on the superconducting properties of thin 2H-NbSe2 platelets. Supercond. Sci. Technol. 27, 015004 (2014).
Bao, W. et al. Approaching the limits of transparency and conductivity in graphitic materials through lithium intercalation. Nature Commun. 5, 4224 (2014).
Perfetti, L. et al. Time evolution of the electronic structure of 1T-TaS2 through the insulator–metal transition. Phys. Rev. Lett. 97, 067402 (2006).
Hellmann, S. et al. Ultrafast melting of a charge-density wave in the Mott insulator 1T-TaS2 . Phys. Rev. Lett. 105, 187401 (2010).
Eichberger, M. et al. Snapshots of cooperative atomic motions in the optical suppression of charge density waves. Nature 468, 799–802 (2010).
Petersen, J. C. et al. Clocking the melting transition of charge and lattice order in 1T-TaS2 with ultrafast extreme-ultraviolet angle-resolved photoemission spectroscopy. Phys. Rev. Lett. 107, 177402 (2011).
Efetov, D. K. & Kim, P. Controlling electron–phonon interactions in graphene at ultrahigh carrier densities. Phys. Rev. Lett. 105, 256805 (2010).
Dagotto, E. Complexity in strongly correlated electronic systems. Science 309, 257–262 (2005).
Joe, Y. I. et al. Emergence of charge density wave domain walls above the superconducting dome in 1T-TiSe2 . Nature Phys. 10, 421–425 (2014).
Yoshida, M. et al. Controlling charge-density-wave states in nano-thick crystals of 1T-TaS2 . Sci. Rep. 4, 7302 (2014).
Fullerton-Shirey, S. K. & Maranas, J. K. Effect of LiClO4 on the structure and mobility of PEO-based solid polymer electrolytes. Macromolecules 42, 2142–2156 (2009).
Acknowledgements
The authors thank D-H. Lee for critical reading of the manuscript, Z-X. Shen, P. Kim, F. Wang, L. Zhou, J. Zhao, Y. Wang, W. Wu, P. Darancet and J. Liu for helpful discussions, and X. Hong, L. He, K. Yu and L. Sun for assistance with measurements. Part of the sample fabrication was conducted at Fudan Nano-fabrication Laboratory. Y.Y., F.Y., L.M. and Y.Z. acknowledge financial support from the National Basic Research Program of China (973 Program) under grants nos. 2011CB921802 and 2013CB921902, and from the NSF of China under grant no. 11034001. X.F.L., Y.J.Y. and X.H.C. are supported by the ‘Strategic Priority Research Program (B)’ of the Chinese Academy of Sciences (grant no. XDB04040100) and the NSF of China (grant no. 11190021). Y-W.S. is supported by the NRF of Korea grant funded by MEST (QMMRC, no. R11-2008-053-01002-0). The work at Rutgers is funded by the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant GBMF4413 to the Rutgers Center for Emergent Materials, and the work at Postech is supported by the Max Planck POSTECH/KOREA Research Initiative Program (grant no. 2011-0031558) through the NRF of Korea funded by MEST.
Author information
Authors and Affiliations
Contributions
Y.Z. conceived the project. X.F.L., Y.J.Y., Y.H.C., S.W.C. and X.H.C. grew bulk 1T-TaS2 crystal. Y.Y. fabricated 1T-TaS2 thin-film devices, performed electric measurements and analysed the data. F.Y. made the solid electrolyte. L.M. carried out scanning tunnelling microscopy measurement on 1T-TaS2 thin films. Y.Y. and Y.Z. analysed the data. X.N. and D.F. performed angle-resolved photoemission spectroscopy measurement on bulk 1T-TaS2 crystal. S.K. and Y.W.S. carried out ab initio calculations. S.L. helped with low-temperature measurements. Y.Y. and Y.Z. wrote the paper and all authors commented on it.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Supplementary information
Supplementary information
Supplementary Information (PDF 3192 kb)
Rights and permissions
About this article
Cite this article
Yu, Y., Yang, F., Lu, X. et al. Gate-tunable phase transitions in thin flakes of 1T-TaS2. Nature Nanotech 10, 270–276 (2015). https://doi.org/10.1038/nnano.2014.323
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nnano.2014.323
This article is cited by
-
Intercalation in 2D materials and in situ studies
Nature Reviews Chemistry (2024)
-
Controllable van der Waals gaps by water adsorption
Nature Nanotechnology (2024)
-
Endotaxial stabilization of 2D charge density waves with long-range order
Nature Communications (2024)
-
Dualistic insulator states in 1T-TaS2 crystals
Nature Communications (2024)
-
Tantalum Disulfide (TaS2)–Based Symmetrical Long-Range Surface Plasmon Resonance Biosensor with Ultrahigh Imaging Sensitivity and Figure of Merit
Plasmonics (2024)