J. Semicond. > 2017, Volume 38 > Issue 3 > 031004, doi: 10.1088/1674-4926/38/3/031004
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SPECIAL TOPIC ON 2D MATERIALS AND DEVICES

Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures

Huihui Yang1, 2, 3, Feng Gao1, 2, 3, Mingjin Dai1, 2, 3, Dechang Jia1, Yu Zhou1 and Ping'an Hu1, 2, 3

+ Author Affiliations

 Corresponding author: Pingan Hu,Email: hupa@hit.edu.cn

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Abstract: Two-dimensional (2D) layered materials, such as graphene, hexagonal boron nitride (h-BN), molybdenum disulfide (MoS2), have attracted tremendous interest due to their atom-thickness structures and excellent physical properties. h-BN has predominant advantages as the dielectric substrate in FET devices due to its outstanding properties such as chemically inert surface, being free of dangling bonds and surface charge traps, especially the large-band-gap insulativity. h-BN involved vertical heterostructures have been widely exploited during the past few years. Such heterostructures adopting h-BN as dielectric layers exhibit enhanced electronic performance, and provide further possibilities for device engineering. Besides, a series of intriguing physical phenomena are observed in certain vertical heterostructures, such as superlattice potential induced replication of Dirac points, band gap tuning, Hofstadter butterfly states, gate-dependent pseudospin mixing. Herein we focus on the rapid developments of h-BN synthesis and fabrication of vertical heterostructures devices based on h-BN, and review the novel properties as well as the potential applications of the heterostructures composed of h-BN.

Key words: h-BN, heterostructures, graphene, van der Waals epitaxy, FETs



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Fig. 1.  (Color online) (a) Schematic of the gas exfoliation of h-BN triggered by thermal expansion. (b) Characterization of exfoliated h-BN nanosheets: (i) SEM and (ii) TEM images after ten repeated cycles [28] .

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Fig. 2.  (Color online) (a) (i) The decomposition process of ammonia borane in the two heating zones. (ii) and (iii) SEM images of fully covered h-BN on Cu (larger images) and transferred onto SiO2/Si (images inside) (ii) without BN nanoparticles and (iii) with many BN particles, grown for 1 h, respectively. (iv) Schematic diagram of the filtering system [41] . (b) The schematic diagram of hexagonal boron nitride (h-BN) LPCVD synthesis setup [39] .

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Fig. 3.  (Color online) (a) Optical images of Cu foils prepared by (i) pristine, (ii) thermal annealing at 1020 ℃ for 2 h, and (iii) thermal annealing (1020 ℃ for 2 h)/chemical polishing. (iv) to (vi) are the corresponding optical images of transferred h-BN nanosheets transferred onto SiO2/Si substrates of (i) to (iii) [35] . (b) SEM image of triangular-shaped h-BN domains grown on Cu foil surface (i) without pre-annealing. (ii) Annealed for 3 h and (iii) 6 h, respectively [49] .

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Fig. 4.  (Color online) (a) (i) Schematic drawing of the self-aligned process of h-BN domains on liquid Cu. (ii) SEM image of multiple circular h-BN domains and (iii) h-BN self-aligned single-crystals array with circular h-BN domains on the edges [52] . (b) (i) A photograph of wafer-scale EM-h-BN on sapphire substrate, (b) Atomic resolution scheme for R30° orientation. Red, green, salmon-color, and blue spheres stand for oxygen, aluminum, boron, and nitrogen elements [54] . (c) (i) CVD system setup for the growth of h-BN on SiO2/Si substrates. (ii) Schematic for the proposed growth mechanism, and (iii) the h-BN film on SiO2/Si of 1.5 × 1.5 cm2 area [40] .

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Fig. 5.  (Color online) (a) Schematics of the catalyst system and SEM images of the surface after growth for 1 min (a, d, g, j) for Fe/SiO2(x)/Si substrates, where x = native, 200, 500, and 2000 nm, respectively. (b)(i) Schematic illustrating the salient stages of the CVD process. (ii) Schematic of the growth model for h-BN CVD on Fe/SiO2/Si substrates. (iii) Detail of the Ferich corner of the Fe-B-N ternary phase diagram in the isothermal section at 950 ℃ [55] . (c) (i)SEM images of h-BN grains grown on Cu foil for 10 min at 1050 ℃. (ii) to (iv) are SEM images of h-BN grains grown for 60 min on Cu-Ni alloy foils with (ii) 10 atom %, (iii) 20 atom % and (iv) 30 atom % Ni at 1050 ℃. The scale bars are 20 μm [56] .

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Fig. 6.  (a) (i) Triangular structure with all sides with N-terminated edges and (ii) hexagonal structure with alternating N- and B-terminated edges [48] . (b) SEM images of the hBN crystals grown at different conditions. (i) APCVD experimental setup for hBN growth. (ii) SEM images of the hBN domains grown at 1065 ℃ using argon as a buffer gas. Sketch of the resulting hBN crystal shapes and corresponding termination-nitrogen (blue) and boron (red) [61] .

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Fig. 7.  (Color online) (a) Atomic structure of monolayer h-BN on different orientations of copper surfaces (i) Cu(111), (ii) Cu(110), and (iii) Cu(100) [65] . (b) SEM images of h-BN triangles grown on (i) Cu(111), (ii) Cu(102), and( iii) Cu(103). Scalar bars in (i-iii) are 20 μm. (iv) Orientation statistics of the h-BN triangles grown on these three Cu facets. (c) Orientation-dependent stacking energies and the optimized structures based on DFT simulation. (i, iv, vii) Energy corrugations of h-BN rotating on Cu(102), Cu(103), and Cu(111), respectively. The optimized 60° stacking structures are shown for h-BN on (ii, iii) Cu(102), (v, vi) Cu(103), and 30° stacking structures for h-BN on (viii, ix) Cu(111). Nitrogen in blue, boron in pink, and copper in yellow. Top and second atom layers of Cu facets are highlighted by red and orange colors [66] .

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Fig. 8.  (Color online) (a) Etching of h-BN crystals with formation of triangular etched holes on (i) grain boundary and (ii) crystal edge. (b) (i) Optical microscope image of a triangular shaped h-BN crystal with well-defined edge structure of etched triangular hole at the center. (ii) Schematic representation of atomic structure of a triangular h-BN crystal with zigzag N-terminated edges [69] .

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Fig. 9.  (Color online) (a) (i) Illustration of epitaxial growth of BN onto graphene edges. (ii) SEM image of a hydrogen-etched graphene (Gr) island with equiangular hexagon etch holes. (iii) Nucleation of BN at graphene edges during initial growth. (iv) Formation of BN epistrips at graphene edges. (v) Continuous BN epistrips enclosing graphene islands. (vi) Full coverage of the etch holes in a graphene island by BN. (vii) Atomic-resolution STM image (3.5 nm by 2.5 nm) of a graphene-BN boundary [75]. (b) Graphene growth starts from seeds on the Cu foil (i) and hexagonal-BN grows continuously from the graphene template (left to right). Low (ii) and high (iii) magnification image for G-BN heterostructure on the Cu growth substrate that was oxidized. (iv) False color black, white, and brown regions indicate graphene, BN, and bare Cu regions in panel (iii), respectively. Scale bar in panel (ii) is 50 μm, and the scale bar in panel (iii) is 10 μm [76].

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Fig. 10.  (Color online) (a) (i) Friction image of a graphene/h-BN heterostructure, (ii) zoomed in view in the black box in (i) with the scan angle 15° [84]. (b) Schematic of growth progress and AFM image of graphene showing aligned hexagonal grains [10] (the scale bars are 200 nm). (c) Schematic diagram of different types of orientation alignment [87]. (d) (i) Illustration of time-triggered selective growth of lateral and vertical epitaxy. SEM images of in-plane h-BN/graphene (ii) and stacked graphene/h-BN (iii). The scale bars in (ii) and (iii) are 2 μm. (iv, v) and (vi, vii) are AFM height images of h-BN/graphene and graphene/h-BN and extracted height histograms of the corresponding section. The scale bars in (iv) and (v) are 1 and 0.5 μm, separately. (viii, ix) SEM images of h-BN/graphene and graphene/h-BN structures. The scale bars are 10 and 5 μm, separately [79].

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Fig. 11.  (Color online) (a) SEM image of triangular-shaped WS2 crystals grown onto an h-BN flake. (ii) Proposed structure model of WS2/h-BN, the bottom and top layers correspond to h-BN and WS2 [98]. (b) (i) Schematic of the synthesis process for heterostructures. (ii) SEM image of the directly grown single-crystal MoS2 on h-BN. Inset: MoS2 crystal with grain size up to 200 μm2; the scale bar is 5 μm. (iii) TEM characterizations of MoS2/h-BN heterostructures. SAED patterns corresponding to the heterostructures (inset); the scale bar is 0.2 nm. The spots in the green dashed hexagons indicate the (110) plane of MoS2, and the spots in the blue dashed hexagons indicate the (1010) plane of BN [101] .

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Fig. 12.  (Color online) (a) A schematic illustration of the moiré pattern generated by lattice mismatch with zero rotation angle [10] . (b) Band structure along the ΓK and KM directions in reciprocal space, and total and projected densities of states DOSs for the relaxed structure of graphene on h-BN [9] . (c) Local resistance measured by conductive AFM for one of our graphene-on-h-BN samples with an 8 nm moiré pattern (i) and with a 14 nm moiré periodicity (ii). Young's modulus distribution, measured in the Peak Force mode, for structures with 8 (iii) and 14 nm (iv) moiré patterns, respectively. (v) and（vi）are cross-sections of the Young's modulus distribution taken along the dashed lines in (iii) and (iv), respectively. (vii) Ratio between FWHM of the peak in the Young's modulus distributionand the period of the moiré structure L. (viii) Young's modulus distribution across an unaligned sample. Scale bars for (i), (ii), (iii), (iv) and (viii) are 10 nm [103] .

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Fig. 13.  (Color online) (a) (i) Theoretical local density of states curves for three different rotation angles between graphene and h-BN, red is $\phi$ =0.5° (12.5 nm), blue is $\phi $ =1° (10.0 nm) and green is $\phi $ =2° (6.3 nm). The curves have been vertically offset for clarity. (ii) Experimental dI/dV curves for two different moiré wavelengths, 9.0 nm (black) and 13.4 nm (red). The dips in the dI/dV curves are marked by arrows [12] . (b) (i) Resistance versus applied Vg at various T for monolayer graphene. (ii) Temperature dependence of the resistance at the DP and satellite peaks. Inset shows resistance versus natural logarithm of T [10] .

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Fig. 14.  (Color online) (a) (i) Schematic drawing of the band structure in the graphene/h-BN heterostructures. (ii) Stacking of constant-energy maps of EDC curvature to show the conical dispersion at the two $\kappa $ points. (b) (i) to (iii) are ARPES data through the SDPs along different directions. The graphene and superlattice Brillouin zones are indicated by black dashed and red solid lines, respectively. The red dots represent the $\kappa $ points of the SBZ. (iv) to (vi) are EDCs between the momenta indicated in (i) to (iii). The EDCs across the SDPs are highlighted by red lines. (vii) to (ix) are fitting results of the EDCs across the SDPs in (i) to (iii) with two (vii, viii) or three (ix) Lorentzian peaks [11] .

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Fig. 15.  (Color online) (a) Nontopological and topological Hall currents. (Left) Drifting cyclotron orbits give rise to Hall currents of the same sign for valleys K and $K'$ . (Right) Skewed motion induced by Berry curvature. (b) Nonlocal resistance in graphene superlattices (red curve) and longitudinal resistance (black curve) measured in G/hBN superlattices. (Top right inset) Optical micrograph of our typical G/hBN device and the nonlocal measurement geometry. Shown schematically are valley K and $K' $ currents and the long-range response mechanism. (Left inset) Schematic band structure of graphene superlattices, with Berry curvature hot spots arising near the gap opening and avoided band crossing regions. (Bottom right inset) Valley Hall conductivity modeled for gapped Dirac fermions as a function of carrier density [14] .

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Fig. 16.  (Color online) (a) (i) Optical microscope image of the mechanically exfoliated monolayer graphene flake with h-BN underneath and gold electrodes contacting it above. The wiring of the STM tip and back gate voltage is indicated. STM topographic image of monolayer graphene (ii) on h-BN and (iii) on SiO2. (iv) Histogram of the height distributions for graphene on SiO2 (blue squares) and graphene on h-BN (red triangles) along with Gaussian fits [109] . (b) (i) Schematic of the h-BN-encapsulated MoS2 multi-terminal device. (ii) Optical microscope image of a fabricated device. Graphene contact regions are outlined by dashed lines. (iii) Cross-sectional STEM image of the fabricated device [95] . (c) (i) Schematic structure of graphene field-effect tunneling transistor. (ii) The corresponding band structure with finite Vg and Vb. (iii) Tunneling I-V's characteristics for a graphene-hBN device for different Vg (in 10-V steps) [6] . (d) Energy band diagrams of vertical n-graphene/h-BN/p-graphene device under zero, reverse and forward bias conditions [117] .

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Fig. 17.  (Color online) (a) (i) J-V characteristics of the graphene/Si solar cells with (red) and without (black) an h-BN interlayer. (ii)(iii) Energy band diagrams of the Gr/SiSchottky junction solar cells (ii) without and (iii) with an h-BN electron blocking layer [120] . (b) (i) Schematic of a graphene/h-BN/graphene device under optical excitation. (ii) Schematic of intralayer thermalization and interlayer transport of the optically excited carriers. (iii) Band alignment between graphene and BN. (iv) Interlayer photocurrent as a function of $V_{\mathrm{b}}$ with and without light illumination [122].

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    Received: 19 October 2016 Revised: 09 November 2016 Online: Published: 01 March 2017

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      Article Navigation >  Journal of Semiconductors  > 2017  >  38(3): 031004
      Huihui Yang, Feng Gao, Mingjin Dai, Dechang Jia, Yu Zhou, Ping'an Hu. Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures[J]. Journal of Semiconductors, 2017, 38(3): 031004. doi: 10.1088/1674-4926/38/3/031004 ****H H Yang, F Gao, M J Dai, D C Jia, Y Zhou, P A Hu. Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures[J]. J. Semicond., 2017, 38(3): 031004. doi:  10.1088/1674-4926/38/3/031004.
      Citation:
      Huihui Yang, Feng Gao, Mingjin Dai, Dechang Jia, Yu Zhou, Ping'an Hu. Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures[J]. Journal of Semiconductors, 2017, 38(3): 031004. doi: 10.1088/1674-4926/38/3/031004 ****
      H H Yang, F Gao, M J Dai, D C Jia, Y Zhou, P A Hu. Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures[J]. J. Semicond., 2017, 38(3): 031004. doi:  10.1088/1674-4926/38/3/031004.
      shu

      Recent advances in preparation,properties and device applications of two-dimensional h-BN and its vertical heterostructures

      doi: 10.1088/1674-4926/38/3/031004
      • 1.

        Institute for Advanced Ceramics, Harbin Institute of Technology, Harbin 150001, China

      • 2.

        Key Lab of Microsystem and Microstructure, Harbin Institute of Technology, Harbin 150080, China

      • 3.

        School of Materials and Science Engineering, Harbin Institute of Technology, Harbin 150080, China

      Funds:

      Project supported by the National Natural Science Foundation of China Nos.61390502,21373068

      Project supported by the National Natural Science Foundation of China (Nos.61390502,21373068),the National Basic Research Program of China (No.2013CB632900),the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (No.51521003),and the Self-Planned Task of State Key Laboratory of Robotics and System (No.SKLRS201607B)

      the National Basic Research Program of China No.2013CB632900

      and the Self-Planned Task of State Key Laboratory of Robotics and System No.SKLRS201607B

      the Foundation for Innovative Research Groups of the National Natural Science Foundation of China No.51521003

      More Information
      • Corresponding author: Pingan Hu,Email: hupa@hit.edu.cn
      • Received Date: 2016-10-19
      • Revised Date: 2016-11-09
      • Published Date: 2017-03-01

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