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SCIENCE CHINA Information Sciences, Volume 62, Issue 12: 220407(2019) https://doi.org/10.1007/s11432-019-2653-9

Chemical vapor deposition synthesis of two-dimensional freestanding transition metal oxychloride for electronic applications

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  • ReceivedAug 17, 2019
  • AcceptedSep 16, 2019
  • PublishedNov 12, 2019

Abstract

Two-dimensional transition metal oxychlorides (MOCl, $M$ = Fe, Cr, V, Ti, Sc) with the metal-oxygen plane sandwiched by two layers of chloride ions possess many exotic physical properties. Nevertheless, it is of great challenge to grow two-dimensional single-crystal MOCl because polyvalent nature of transition metal elements usually gives rise to mixed oxyhalides compounds with distinct physical properties. Here, we take VOCl as an example to present a solution for synthesizing 2D freestanding MOCl with various thicknesses through chemical vapor deposition (CVD) method. The single crystal and elementary composition as well as elements ratio of as-grown samples have been characterized through measurements of X-ray diffraction, X-ray photoelectron spectroscopy and energy-dispersive spectroscopy, respectively. Furthermore, we demonstrate that 2D VOCl-based memristive devices show low power consumption and excellent device reliability due to the layered-structure and electrically insulating properties of 2D VOCl flakes. Besides, we utilize the feature of multilevel resistive switching that memristive devices exhibit to emulate depression and potentiation of synaptic plasticity. This method developed in this study may open up a new avenue for the growth of 2D MOCl with single crystal and pave the way for high-performance electronic applications.


Acknowledgment

This work was supported in part by National Key Basic Research Program of China (Grant No. 2015CB921600), National Natural Science Foundation of China (Grant Nos. 61974176, 61574076), Collaborative Innovation Center of Advanced Microstructures, Natural Science Foundation of Jiangsu Province (Grant Nos. BK20180330, BK20150055), and Fundamental Research Funds for the Central Universities (Grant Nos. 020414380122, 020414380084).


Supplement

Figures S1–S4.


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  • Figure 1

    (Color online) Chemical vapor deposition of two-dimension single crystal VOCl and their optical images.protectłinebreak (a) Cross-section for atomic configurations of the VOCl lattice; (b) a schematic of VOCl synthesis setup; (c) and (d) optical images of as-grown VOCl on Si/SiO$~_2~$ substrate; (c) optical image of freestanding VOCl transferred to target substrate; protectłinebreak (d) inset, height profiles of VOCl nanosheet, scale bar is 10 $\mu~$m.

  • Figure 2

    (Color online) Characterization of VOCl. (a) X-ray diffraction (XRD) pattern; (b) X-ray photoelectron spectroscopy with full spectrum shown in the inset.

  • Figure 3

    (Color online) (a) Low resolution TEM images of VOCl flakes (scale bar: 0.5 $\mu$m); (b) energy dispersive X-ray spectroscopy (EDS) mapping of the sample area marked in the red box appearing in (a); (c) high resolution TEM image; (d) selected area electron diffraction (SAED) pattern (scale bar: 21 nm$^~{-1}$).

  • Figure 4

    (Color online) Electrical characterizations of VOCl based memristive devices. (a) Top: schematic of the VOCl devices. Bottom: optical image of a simple array of 2 $\mu$m $\times$ 2 $\mu$m VOCl based memristive devices. The top (TE) and bottom (BE) electrodes are Ag/Au and Au, respectively. (b) Typical IV switching curves of the VOCl based devices. The blue line represents the reset process after electroforming step and the red line is the 1st set process. The arrows indicate the switching direction. (c) Measured endurance of the device under DC sweep mode with compliance current of 250 $\mu$A and reset voltage of $-$1.4 V. (d) Measured retention data of on/off resistance states at room temperature with read voltage of 0.1 V. (e) Multilevel resistive switching characteristics of VOCl based memristive device via increasing compliance current (right red lines) and increasing RESET voltage (left blue lines). The arrows indicate the directions of adjusting resistance. (f) Variation of device resistance with consecutive depressing and potentiating pulses. The resistance is measured at 0.1 V after each pulse. Depression ($-$1.15 V, 500 $\mu$s); potentiation (1.6 V, 50 $\mu$s).

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