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Carbon nanotube quantum dots on hexagonal boron nitride Carbon nanotube quantum dots on hexagonal boron nitride A. Baumgartner,1 G. Abulizi,1 T. Taniguchi,2 and C. Schönenberger1 1 Institute of Physics, University of Basel, Klingelbergstrasse 82, 4056 Basel, Switzerland A. Baumgartner 1, G. Abulizi 1, T. Taniguchi 2, and C. Schönenberger 1 ⇤ 2 Advanced Materials Laboratory, National Institute for Material Science, 1-1 Namiki, Tsukuba, 305-0044, Japan (Dated: April 6, 2014) 1 Institute of Physics, University of Basel, Klingelbergstrasse 82, 4056 Basel, Switzerland Advanced Materials Laboratory, National Institute for Material Science, 1-1 Namiki, Tsukuba, 305-0044, Japan [email protected] We report the fabrication details and low-temperature characteristics of the first carbon nanotube 2 (CNT) quantum dots on flakes of hexagonal boron nitride (hBN) substrate. We demonstrate that CNTs can be grown on hBN by standard chemical vapor deposition and that standard scanning electron microscopy imaging and lithography can be employed to fabricate nanoelectronic structures when using optimized parameters. Our findings pave the way to more complex devices on hBN, with more predictable and reproducible characteristics and electronic stability. PACS numbers: 73.23.-b Carbon nanotubes (CNTs) are a versatile fundamental building block for classical small-scale Carbon nanotubes (CNTs) are aand versatile fundamenricate hBN-graphene multi-layer one electronics quantum electronics - in theory. In structures practice,(REF?), the ideal properties of CNTs are tal building block for classical small scale electronics and dimensional contacts14 and combinations with other layusually masked by Inelectrical fluctuations induced by the substrate. For graphene, a new ered materials. quantum electronics applications - in theory. practice, potential the ideal properties of CNTs are usually masked by elecThe nextnanostructures, step, however, namely the usethe of hBN approach has recently lead to 'clean' namely useasof thin layers of hexagonal trical potential fluctuations induced by the substrate. An substrate for independent, more complex nanostructures boron nitride (hBN) [1]. contrast to the standard Si/SiO2 intuitive solution to avoid the noise induced by theused sub- aslikeinsulating quantum dotssubstrates (QDs), has not beenIn demonstrated strate is to suspend the active device volume above the so far. Specifically, no experiments on CNTs grown on substrates, hBN exhibits significantly less charge traps and leads to larger charge puddles in substrate, which has lead fundamental experiments, both hBN substrates have been reported. The main reason 1,2,5,6 3 on suspended CNTs and on[2], suspended graphene whichgraphene results. in for a reduction noisetoinlocate transport experiments. this probablyofis the thatelectronic CNTs are difficult on hBN, because optical microscopy lacks the required Suspended devices, however, su↵er from limitations in resolution, the contrast in scanning electron microscopy the scalability, geometry and in the choice of the conThe next step, however, namely the use hBN as substrate for independent, more complex (SEM) images can beof poor (see below) and AFM imaging tact and gate materials. For example, it is difficult to isdots rather(QDs), demandinghas because largedemonstrated lateral and verfind a superconductor or a ferromagnet like suitable for the nanostructures quantum notof the been so far. Specifically, no tical scales involved, while retaining the nanometer resCVD growth of CNTs at temperatures around 1000 C. experiments on CNTs grownolution on tohBN been reported. Here, we report the image substrates the CNTs. Herehave we report the fabricaStamping techniques5? are more versatile, but strongly tion details andcharacteristics low-temperature characteristics of CNT depend on the interface characteristics of the contacts. In fabrication details and low-temperature of the first CNT QDs on flakes of hBN quantum dots (QDs) on top of hBN flakes. We demoncontrast, devices fabricated on a substrate o↵er a much substrate. We demonstrate that CNTs can be grown on hBN by strate that for a range of hBN thicknesses and SEM set- standard chemical vapor larger variety of design options and possible materials, tings rapid feed-back large scale SEM imagingimaging of but the stability and quality of the electronic structure scanning deposition and that standard electronandmicroscopy (SEM) and lithography can CNTs on hBN is possible, also shedding light on the is usually compromised. Standard cleaning techniques be employed to fabricate nanoelectronic structures when using optimized parameters. Our imaging contrast for CNTs on dielectrics. Based on these cannot be deployed because they also remove the carbon results, we fabricate CNT QDs on hBN, the most fundastructures4 and thefindings thermal coupling to the substrate is pave the way to more complex devices on hBN, with more predictable and reproducible mental non-trivial electronic nanostructure, and report too large for in-situ current annealing. characteristics and electronic stability. For graphene, a new approach has recently lead to ’clean’ nanostructures, namely the use of thin layers (flakes) of hexagonal boron nitride (hBN) used as insu(a) metal hBN lating substrates. This approach allows the implemencontacts Pd tation of substrate supported graphene in high-mobility CNT CNT (QD) hBN transistors7 and the observation of fundamental physiPd SiO SiO cal phenomena like the formation of a superlattice band ++ Si p 9 10 structure or the cloning of Dirac Fermions . Using hBN as a substrate has also enabled the fabrication of (b) optical (c) SEM (d) AFM highly efficient monolayer WSe2 light emitting diodes11 . In contrast to the standard Si/SiO2 substrates, hBN exhibits significantly less charge traps and leads to larger charge puddles in graphene8 , which results in a reduction 2 m 4 m 4 m of the electronic noise in transport experiments, e.g. in graphene quantum dots12 and double layer graphene13 . FIG. 1: (a) Schematic of the quantum dot structure on a hBN hBN can be cleaved (mechanically exfoliated) with sim(a) Schematic quantum a hBN flake. The inset shows a device with Pd contacts. (b) flake. dot The structure inset showson a device with Pd contacts. (b) optical ple methods7 with Figure resulting1:thicknesses down of to the single (c) SEM and (d) AFM image of a CNT (⇠ 8 nm radius) on a(~ 28 nm thickness) on SiO2. Optical, (c) SEM, and (d) AFM image of a CNT (~ 8 nm radius) on a hBN flake atomic layers. To date, only few graphene-based devices hBN flake (⇠ 28 nm thickness) on a SiO2 substrate. have been demonstrated, but big e↵orts are made to fab2 2 40 20 height (nm) 60 0 The structure of our devices is shown schematically in figure 1a. Figure 1b shows the optical microscopy image of a ~ 28 nm thick hBN flake after CNT growth. The contrast and color allow for an initial screening for suitable flakes on a marker field before the device fabrication [3]. The CNTs are not visible using an optical microscope and can only be found by SEM or atomic force microscopy (AFM) imaging, as shown for the same hBN flake in figure 1c and 1d, respectively. Figure 2 shows a series of SEM images of a ~ 1 nm radius CNT on a hBN flake with several steps in the thickness for different SEM acceleration voltages Uacc. The apparent CNT diameter is considerably larger on hBN than on SiO2 and wider for lower voltages. The CNT contrast is 1 G (G0) VSD (mV) a recipe optimized to obtain clean CNTs and reliable number of secondary electrons in the contacts4 and thermal evaporation of Pd to fabricate gies lower than in the primary beam, electrical contacts for two-terminal devices on CNTs han the material’s energy gap. These on top of hBN flakes. The contacts are separated by ns can leave the substrate through the ⇠ 300 nm so that we expect the formation of quantum orbed in the material. The total charge dots (QDs) at cryogenic temperatures. The conductance nds on the balance between the number of a device at 4.2 K is plotted in Fig. 4 as a function of ry and back-scattered secondary elec(a) (dark) around U (b) ≈ 1.5 kV, then (c) bestthe andprimary positive for the voltages and turns negative acc thelowest backgate voltage V BG and the source-drain bias VSD . cceleration voltages, elecpositive again Uacc >The 2 kV. Weexhibits find anclear optical Uacc for imaging both, the hBN flakes and the device Coulomb blockade diamonds trate deep into the substrate andfor more a series of resonances due to excited states. The images of CNTs on CNTs, between 0.4 kVand and 1.1 kV. The contrast mechanism for SEM ns are scattered back through the surdashed lines in the figure trace the edges of the Coulomb to a positive charging of the substrate insulating substrates can be understood qualitatively in a simple picture [4]: the primary beam blockade diamonds and suggest a four-fold symmetry as . At higher voltages, the freea electrons generates large number of secondary electrons in the dielectric at energies lower than in the found in clean CNT quantum dots due to the spin and into the substrate and the secondary primary beam, but still larger than the material’s energy gap.Uacc = 0.3energy valley degeneracies in CNTs. The charging and KV Uacc = 0.5 KV Uacc = 0.9 KV 1µm 1µm 1µ e layers with reduced probability, which the energy of the first excited state are ⇠ 7 meV and o a negative charging of the structure (d) (e) (a) (b) (c) ⇠ 2 meV, respectively, and the lever arm is 0.1, comlectrons. Only when the penetration parable to bare SiO2 dielectrics, in accordance with the e oxide layer thickness, the secondary Schematic of contrast mecha similar dielectric constants. absorbed by the conducting backgate rge of the structure can again become We observe up to 6 excited states and negative di↵erential conductance between excited states resonances, as indicated in Fig. 4 by arrows (...). The excited states ation voltages the electrons interact 1µm 1µm = 1.5the KV Uacc = 20 KV Uacc = 0.3 KV Uaccenergies = 0.5 KV = 0.9 all). KV 1µm are 1µm ..., ... Uacc (list We 1µm note Uacc that ground CNTs and the image contrast stems state transitions are weaker in some Coulomb blockade hanges in the electron density near the (e) images of CNTs (~ 1 nm radius) on a hBN flake (first step ~ 35 nm thickness, second (d) Figure 2: Seriers of SEM can be seen as charge reservoirs (or~ 80 nm thickness) on a SiO substrate obtainedFIG. 2: (a)Schematic a CNT quantum dot fabricated second step for different accelerationofvoltages. 2 ot connected to an electrical contact) Schematic of contrast mechanism hBN flake as substrate. (b) optical, (c) SEM and (d) A −3 rons to the substrate if it is positively image of x 10CNTs on a hBN flake on a SiO2 surface. 4 pts electrons if the substrate is negaFor positive substrates electrons move 10 3 c and this additional electron density 1µm = 1.5 KV tering rates and theUaccgeneration of1µm sec- Uacc = 20 KV 2 5 leading to a positive contrast in the 1 Ts. This explains FIG. qualitatively the two of a CNT quantum dot fabricated on a 2: (a)Schematic 0 he CNT contrast hBN in SEM images and flake as substrate. (b) optical, (c) SEM and (d) AFM 0 is almost identical on the two rather image of CNTs on a hBN flake on a SiO2 surface. −5 es. −1 the contrast depends less on the di−2 −10 of the substrate (✏hBN ⇡ 4 (depends tation) and ✏SiO2 ⇡ 4), but rather on −3 ility to supply electrons, i.e. on its to−15.1 −15 −14.9 −14.8 −14.7 VBG (V) which scales with the length of the tube the logarithm of its diameter. This is h our findings of about the contrast beFigure 3: Coulomb blockade and excited states resonances on a CNT QD fabricated on top a hBN flake. FIG. 4: Coulomb blockade and excited states resonances on bstrates. The apparent width depends QD fabricated on top an hBN flake (temperature T = s electron di↵usion length for the quasi The conductance of a4.2 aCNT device (figure 1a) at 4.2 K is plotted in figure 3 as a function of the K). ove the energy gap, and on voltage the elec-V back-gate and the source-drain bias V . The device exhibits clear Coulomb BG SD blockade diamonds and a series of resonances due to excited states. The dashed lines in the figure trace the edges of the Coulomb blockade diamonds and suggest a four-fold symmetry as found in clean CNT QDs due to the spin and valley degeneracies in CNTs. The charging energy and the energy of the first excited state are ~ 7 meV and ~ 2 meV, respectively, and the lever arm (a) (b) (c) is 0.1, comparable to bare SiO2 dielectrics, in accordance with the similar dielectric constants. Height (nm) [1] C.R. Dean, A.F. Young, I. Meric, C. Lee, L. Wang, S. Sorgenfrei, K. Watanabe, T. Taniguchi, P. Kim, K.L. Shepard, and J. Hone, “Boron nitride substrates for high-quality graphene electronics”, Nature Nanotech. 5, 722 (2010). [2] J. Xue, J. Sanchez-Yamagishi, D. Bulmash, P. Jacquod, A. Deshpande, K. Watanabe, T. Taniguchi, P. Jarillo2µm 2µm Herero, and B.J. LeRoy, “Scanning tunneling microscopy and spectroscopy ofKVultra-flat2µm graphene onKVhexagonal Uacc = 0.6 Uacc = 0.6 boron nitride”, Nature Mater. 10, 282 (2011). 50 [3] (a)D. Golla, K. Chattrakun, B.J. LeRoy, and A. 3: Sandhu, “Optical thickness (b) K. Watanabe, T. Taniguchi, (c) FIG. (a)Schematic of a CNT quantum dot fabricated determination of hexagonal boron nitride flakes”, Appl. Phys. Lett. 102, 161906 (2013). hBN flake as substrate. (b) SEM image of a CNT quan [4] R.Y. Zhang, Y. Wei, L.A. Nagahara, I. Amlani, and R.K. Tsui, “The contrast mechanism in low voltage dot device. scanning electron microscopy of single-walled carbon nanotubes”, Nanotechnology 17, 272 (2006). Uacc = 0.6 KV 2µm Uacc = 0.6 KV 2µm 2µm 0 FIG. 3: (a)Schematic of a CNT quantum dot fabricated on a 2