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Gate-Tuned Insulator-Metal Transition in Electrolyte-Gated Transistors Based on Tellurene Xinglong Ren, Yan Wang, Zuoti Xie, Feng Xue, Chris Leighton, and C. Daniel Frisbie Nano Lett., Just Accepted Manuscript • DOI: 10.1021/acs.nanolett.9b01827 • Publication Date (Web): 10 Jun 2019 Downloaded from http://pubs.acs.org on June 11, 2019

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Gate-Tuned Insulator-Metal Transition in Electrolyte-Gated Transistors Based on Tellurene Xinglong Ren1, Yan Wang2, Zuoti Xie1, Feng Xue1, Chris Leighton1, and C. Daniel Frisbie1* 1Department 2Department

of Chemical Engineering and Materials Science,

of Chemistry, University of Minnesota, Minneapolis, MN 55455, USA *Corresponding Author: [email protected]

Abstract Tellurene is a recently discovered 2D material with high hole mobility and air stability, rendering it a good candidate for future applications in electronics, optoelectronics, and energy devices. However, the physical properties of tellurene remain poorly understood. In this paper, we report on the fabrication and characterization of high-performance electrolyte-gated transistors (EGTs) based on solution-grown tellurene flakes 1  1013

cm-2, as confirmed by the temperature dependence of resistance, and magnetoresistance measurements. Wide-range tuning of the electronic ground state of tellurene is thus achievable in EGTs, opening up new opportunities to realize electrical control of its physical properties.

Keywords: insulator-metal transition, electrolyte gating, 2D tellurene, charge transport

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Electrolyte gating, which enables accumulation of high charge densities (>1013 cm-2) at targeted surfaces, has been widely applied in field-effect transport experiments based on a variety of materials.1–4 Due to the existence of strong electric fields and thus high charge densities, electrical control of materials properties can be realized both electrostatically and electrochemically in the electrolyte-gated transistor (EGT) geometry, simply by varying the gate voltage (VG).3,4 The effectiveness and ease of electrolyte gating make it a powerful tool to tune transitions among different electronics phases. Since the first observation of a gate-induced insulator–metal transition in epitaxial ZnO films in 2007,5 for example, the electrolyte gating approach has been applied to trigger electronic phase transitions in a broad range of materials, including organic semiconductors,6–8 transition metal and complex oxides,9–14 1D nanowires and nanotubes,15–18 and 2D van der Waals layered materials.19–25

Upon the discovery of graphene in 2004,26 2D materials (e.g., transition metal dichalcogenides,27 black phosphorus28, etc.) have attracted significant attention due to their attractive electronic and optical properties. Recently, a new elemental 2D material, tellurene (i.e., nm-thick tellurium (Te) flakes), was discovered, showing promising properties.29 Te has a trigonal crystal structure, in which individual atoms are covalently bonded into 1D helical chains, with van der Waals interactions bonding the neighboring chains together.30 Under appropriate conditions, 2D flakes of Te with thicknesses 1013 cm-2, mobilities >400 cm2V-1s-1 and operating voltages -0.2 V strongly-localized insulating behavior occurs. Around -0.5 V this gives way to weak localization, the resistance upturn at -0.5 V occurring around 100 K (see Figure S6). Increasing the magnitude of VG to -1 V then leads to the onset of truly metallic conduction, with dR/dT ≥ 0 down to the lowest temperatures probed. The upturn temperature marked by the dashed line thus decreases to below 2 K. Finally, further increase of the magnitude of VG leads to reentrance of a state with a measurable upturn temperature for the resistance (dashed line), which grows from 20 to 60 K from -1.5 to -2.0 V (see Figure S6). As discussed above, MR measurements in this regime suggest both weak localization and weak antilocalization, consistent with the high atomic number of Te. One possibility here is that weak antilocalization effects are more prevalent at higher bias magnitudes due to confinement of the hole gas closer to the interface, where spin-orbit effects may be stronger. More work is clearly needed to fully understand the evolution of weak localization/antilocalization with gate voltage, however. Clearly related to this, the exact origins of the saturation of Hall carrier density and decrease of mobility at high |VG| remain open questions for further work on electrolyte gated tellurene. In particular,

better

understanding

of

ion-hole

and

hole-hole

interactions

at

the

electrolyte/semiconductor interface are required.

In summary, we have presented a systematic study of tellurene EGTs and their low temperature charge transport behavior. Fabricated EGTs based on solution-grown tellurene exhibit unipolar


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p-type behavior with good on-off current ratios. Charge densities over 1013 cm-2 and mobilities as high as 500 cm-2V-1s-1 were revealed by Hall effect measurements on such devices. VGdependent R-T measurements were then applied to investigate charge transport mechanisms, and a gate-tuned 2D insulator-metal transition was thus established at VG = -1 V (corresponding to 1.6  10-13 cm-2). Higher VG magnitudes result in reentrance of a weakly-localized state, however, evidencing a non-trivial interplay between insulating, truly metallic, and weaklylocalized/antilocalized transport. Overall, our results demonstrate that electrolyte gating is a powerful tool to tune the charge-density-dependent properties of tellurene, potentially of utility for controlling other properties (optical, thermoelectric, and even structural) in future work.

Supporting Information The Supporting Information is available free of charge on the ACS Publications website. Synthesis of tellurene flakes and device fabrication; characterization of back-gated tellurene devices; additional results on tellurene EGTs; additional information on fitting of magnetoresistance data.

Acknowledgements This work was primarily supported by the MRSEC program of the National Science Foundation at the University of Minnesota under Award Number DMR-1420013. Parts of this work were carried out in the Characterization Facility, University of Minnesota, which receives partial support from NSF through the MRSEC program (DMR-1420013), and in the Minnesota Nano Center, which receives partial support from NSF through the NINN program (NNCI-1542202). X.R. thanks Rui Ma and Jiayi He for helpful discussions and experimental assistance.


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