Study of transport properties in graphene monolayer flakes on SiO[sub 2] substrates The MIT Faculty has made this article openly available. Please share how this access benefits you. Your story matters. Citation Tirado, J. M., D. Nezich, X. Zhao, J. W. Chung, J. Kong, and T. Palacios. “Study of Transport Properties in Graphene Monolayer Flakes on SiO[sub 2] Substrates.” J. Vac. Sci. Technol. B 28, no. 6 (2010): C6D11. As Published http://dx.doi.org/10.1116/1.3516649 Publisher American Institute of Physics/American Vacuum Society Version Final published version Accessed Wed May 25 22:08:49 EDT 2016 Citable Link http://hdl.handle.net/1721.1/87120 Terms of Use Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. Detailed Terms Study of transport properties in graphene monolayer flakes on SiO 2 substrates J. M. Tirado, D. Nezich, X. Zhao, J. W. Chung, J. Kong, and T. Palacios Citation: Journal of Vacuum Science & Technology B 28, C6D11 (2010); doi: 10.1116/1.3516649 View online: http://dx.doi.org/10.1116/1.3516649 View Table of Contents: http://scitation.aip.org/content/avs/journal/jvstb/28/6?ver=pdfcov Published by the AVS: Science & Technology of Materials, Interfaces, and Processing Articles you may be interested in Dielectric thickness dependence of carrier mobility in graphene with HfO 2 top dielectric Appl. Phys. Lett. 97, 123105 (2010); 10.1063/1.3492843 Theory and measurements of room temperature transport in graphene using Si O 2 backgate and electrochemical gate J. Vac. Sci. Technol. B 27, 2003 (2009); 10.1116/1.3156733 Origin of the ambipolar operation of a pentacene field-effect transistor fabricated on a poly(vinyl alcohol)-coated Ta 2 O 5 gate dielectric with Au source/drain electrodes Appl. Phys. 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Palacios Department of Electrical Engineering and Computer Science and Microsystems Technology Laboratories, Massachusetts Institute of Technology, 77 Massachusetts Ave., Massachusetts 02139 共Received 8 July 2010; accepted 18 October 2010; published 12 November 2010兲 This work studies the transport properties of field effect transistors fabricated on graphene single monolayer flakes. In particular, carrier mobilities in graphene for electrons and holes as a function of the vertical electric field are presented and compared with universal mobility curves in silicon. The graphene device shows excellent transport properties, especially at low electric fields due to the lack of Coulomb scattering. At higher electric fields, the phonon scattering dominates and makes the electron mobility similar to the one in silicon. The effect of defects and traps by charged impurities in the transport properties has also been studied, and it has been shown that an initial high temperature annealing significantly improves the transport properties and stability of these devices. © 2010 American Vacuum Society. 关DOI: 10.1116/1.3516649兴 I. INTRODUCTION Materials based on carbon nanostructures are quickly becoming a feasible alternative to silicon technology in future high speed electronics. Graphene, a single monolayer of sp2-bonded carbon atoms, turns out to be an ideal candidate for this application due to its excellent high mobility and Fermi velocity. In spite of these very promising properties,1 the development of graphene devices is still in a very preliminary stage and there are many unknowns about the reproducibility and transport properties of these devices.2 Extrinsic scattering sources, many of which arise from the surface morphology, chemistry, structural, and electronic properties of the widely used SiO2 substrate, limit the mobility of graphene devices by as much as several orders of magnitude with respect to theoretical calculations.3 Great effort is currently underway to increase the mobility beyond extrinsic limits. For example, the extrinsic mobility reported in graphene devices varies widely across the literature. Mobility values between 3000 and 40 000 cm2 V−1 s−1 have been reported.1,4–7 In addition, the gate voltage required for minimum conduction in this ambipolar material is not centered at 0 V as is typical in other ambipolar semiconductors, but it is shifted toward positive gate voltages.4,8 The origin of this shift is still under study, although impurity density7 and chemical doping4 are proposed to explain this phenomenon. In this work, the transport properties of a field effect transistor fabricated on a graphene flake have been studied. In particular, carrier mobilities in graphene for electrons and holes as a function of the vertical electric field are presented and compared with the universal mobility curves in silicon. The effect of temperature on the electrical response of the device and its influence on the mobility curves for electrons a兲 Electronic mail: josemaria.tirado@uclm.es C6D11 J. Vac. Sci. Technol. B 28„6…, Nov/Dec 2010 and holes have also been analyzed to understand the origin of the shift in the gate voltage required for minimum conduction. II. METHOD OF ANALYSIS AND DISCUSSION p-type silicon wafers 共100兲 with a boron doping concentration of NA = 1015 cm−3 have been thermally oxidized to a SiO2 thickness of tox = 300 nm. Then, graphene has been deposited onto the silicon dioxide by microcleaving according to Reina et al.9 and visually inspected to identify a suitable monolayer graphene flake. Optical lithography was used to define the contact pads and a titanium 共50 nm兲/chrome 共5 nm兲 bilayer was used as the contact metal. The typical dimensions of the graphene flakes used in this work are 615 nm in length and 1450 nm in width. The current-voltage 共I-V兲 characteristics of this device were measured with an Agilent 4155A semiconductor parameter analyzer. In these measurements, the source-drain bias was set to a very low value of 0.1 V to prevent device selfheating, while a back-gate step voltage was applied to the conductive Si substrate with a bias sweep ranging from ⫺40 to 40 V and back again in steps of 0.5 V. No significant hysteresis was found in the device. The same experiment was repeated again with a negative source-drain voltage of ⫺0.1 V; similar results were found in both cases showing a clear bidirectional behavior of the device. All the measurements were performed under vacuum 共chamber pressure below 5 ⫻ 10−6 Torr兲 to avoid the oxidation of the graphene layer. The device temperature was varied from 300 to 425 K through the use of a thermal chuck. Figure 1 shows the drain current of the device as a function of the back-gate voltage at different chuck temperatures. Initially, the starting temperature is 300 K, then the temperature is increased in steps of 25 K until it reaches a maximum value of 425 K. Finally, the temperature is decreased again in 1071-1023/2010/28„6…/C6D11/4/$30.00 ©2010 American Vacuum Society C6D11 Redistribution subject to AVS license or copyright; see http://scitation.aip.org/termsconditions. Download to IP: 18.51.1.88 On: Thu, 22 May 2014 16:13:48 C6D12 Tirado et al.: Study of transport properties in graphene monolayer flakes C6D12 FIG. 2. Effect of a temperature annealing cycle in the position of the minimum conductivity valley in Fig. 1. The cycle initially starts at a temperature of 300 K. Then, the temperature is increased until it reaches 425 K, in steps of 25 K, and then the temperature is decreased again to finally achieve 325 K. FIG. 1. 共Color online兲 Drain current of a back-gated graphene field effect transistor. The back-gate voltage is swept from VGS = −40 to 40 V in steps of 0.5 V. Drain-source voltage is set to 0.1 V to minimize self-heating. The curves when the temperature is increased from 300 to 425 K are plotted in solid lines, while dashed lines show the behavior of the device when the temperature is decreased from 425 to 325 K. steps of 25 K. The ambipolar nature of the graphene is clearly revealed in Fig. 1. For negative gate voltages, the conduction is mainly due to holes, and the current decreases as the voltage becomes more positive. For a positive enough gate voltage, the current reaches a minimum, where the conduction due to electrons and holes is equally important. For even more positive voltages, the electron current dominates as the Fermi level moves deeper into the conduction band. Finally, for high enough gate voltages, the current decreases again. The origin of this decrease in the conduction is still under study but may be due to the effect of traps by charged impurities in the graphene layer being the dominant scattering mechanism or carrier injection in low electron velocity valleys of the band diagram. Figure 1 also shows a shift in the gate bias required for minimum conduction toward positive voltages. Some authors attribute this behavior to unintentional chemical doping, impurity densities, or trapping by absorbed gas molecules or defects during processing and handling of the sample.4,6,7 In addition, the possible existence of zigzag edges in graphene ribbons could lead to localized edge states at the Fermi level.8 Other authors proposed that the band diagram of graphene is better represented by a conduction model with an overlap between conductance and valence bands,6 where a mixed state of both electrons and holes would be present. To clarify the main mechanism behind this shift in the minimum current, in this article, we have studied the position of this minimum as a function of temperature. Figure 2 shows the gate voltage required to get minimum current in the graphene device as a function of device temperature. Initially, at 300 K, the valley of minimum current is located at a gate bias voltage near 29 V. As the temperature increases, the minimum current valley shifts toward lower voltages. This effect is more pronounced for temperatures above 350 K. At a temperature of 425 K, the maximum temperature allowed by our measurement setup, the valley has shifted to 13.6 V. When the sample temperature is reduced, the voltage finally stabilizes at 8 V. For repeated temperature cycles, the voltage minimum remains constant at 8 V. This behavior supports the theory of unintentional acceptorlike doping of the graphene layer by adsorbed gas molecules by explaining 72% of the shift. At high enough temperatures 共i.e., 350 ° C兲, the gas molecules 共possibly hydrogen or oxygen兲 are desorbed and the conductivity of the graphene layer becomes more intrinsic. The origin of the remaining shift in the gate bias required for minimum conductivity could be due to undesorbed gas molecules or an overlap between conduction and valence bands. Further experiments at higher temperatures are needed to understand this phenomenon. Absorption/desorption of gas molecules changes the local carrier concentration, which leads to changes in resistance and conductivity. Carrier mobilities in this device have been calculated as a function of temperature using the following relation: = 1 L I W QG共VG兲 VD 共cm2 V−1 s−1兲, 共1兲 where W and L are the width and length of the graphene flake, respectively, and VD is the applied drain bias. QG共VG兲 is the accumulated charge in the graphene layer induced by the voltage directly applied to the graphene layer 共VG兲, QG共VG兲 = CG共VG兲 · VG , 共2兲 where CG is the quantum capacitance of graphene; this value has been extracted from Fang et al.10 CG共VG兲 = 25 ⫻ 10−6 · 兩VG兩 共F cm−2兲. Using these expressions in Eq. 共1兲, we obtain = 1 L I . −6 2 W 25 ⫻ 10 · 共VG兲 VD 共3兲 To determine the relation between the back-gated voltage 共VBG兲 and graphene voltage 共VG兲, we set the stored charge in J. Vac. Sci. Technol. B, Vol. 28, No. 6, Nov/Dec 2010 Redistribution subject to AVS license or copyright; see http://scitation.aip.org/termsconditions. Download to IP: 18.51.1.88 On: Thu, 22 May 2014 16:13:48 C6D13 Tirado et al.: Study of transport properties in graphene monolayer flakes C6D13 FIG. 3. 共Color online兲 Electron universal mobility curves for graphene and silicon. FIG. 4. 共Color online兲 Hole universal mobility curves for graphene and silicon. the graphene quantum capacitance 共CG兲 equal to that in the silicon dioxide capacitance 共Cox兲 as they are both connected in series, function of transversal electric field. In this figure, the electron mobility in graphene is also compared with the universal mobility curve of electrons in silicon.11 Graphene shows electron mobilities much higher than silicon at low electric fields. For example, the mobility reaches values close to 6600 cm2 / V s for electric fields of 50 000 kV/cm. These high mobilities are probably due to the reduced effect of Coulomb scattering in graphene when compared with silicon.12 However, at higher electric fields, phonon scattering significantly reduces the electron mobility, making it very similar to the mobility in Si devices. The important effect of the transversal electric field in the carrier mobility emphasizes the need of knowing the transversal electric field when studying graphene mobilities. The change in mobility with temperature has also been measured. As expected in a semimetal, the mobility increases when temperature increases 共not shown in the figure兲. Hole mobility curves versus electric field are shown in Fig. 4 for both the graphene flake reported in this article and for silicon transistors as reported by Liang et al.13 The hole mobility behaves in a very similar fashion to the electron mobility: very high values at low electric fields due to the lack of Coulomb scattering and a decrease at high electric fields due to the effect of phonon scattering. A hole mobility in excess of 6700 cm2 / V s is calculated in graphene at low electric fields. As in the case of electrons, the hole mobility increases when temperature increases. 共4兲 Cox · Vox = CG · VG . In this expression, given an oxide thickness of 300 nm, Cox is equal to Cox = ox 3.45 ⫻ 10−13 = = 11.5 ⫻ 10−9 F cm−2 300 ⫻ 10−7 tox 共5兲 and 共6兲 Vox = VBG − VG . By substituting Eqs. 共5兲 and 共6兲 in Eq. 共4兲 and using the expression of the quantum capacitance, we can solve for the voltage applied to the graphene layer, VG, as follows: VG ⬵ ⫾ 21.4 ⫻ 10−3冑VBG , 共7兲 where VBG is the applied back-gate voltage assuming that VBG = 0 V happens at the point of minimum conductivity. The mobility at each value of the gate voltage can be expressed as = 1 L I . −6 −3 2 W 25 ⫻ 10 共⫾21.447 ⫻ 10 冑VBG兲 VD 共8兲 To plot the universal mobility curves, an expression for the transversal electric field in the graphene flake is needed. This relation is obtained from the following expression: QG = CG · VG = EG · r,G · 0 , 共9兲 where the value of relative permittivity for graphene is r,G = 2.4.4 Finally, using again the expression for the quantum capacitance in graphene and substituting it in the expression 关Eq. 共9兲兴, we have EG = 2 25VG 2 = 1.18 ⫻ 108 · VG 2.13 ⫻ 10−7 共V/cm兲. 共10兲 Figure 3 shows the electron mobility in graphene as a III. CONCLUSIONS In conclusion, in this article, we have studied the transport properties of a field effect transistor based on a monolayer graphene flake. Universal carrier mobilities for electrons and holes have been extracted and compared with universal mobility curves for silicon. At low electric fields, the graphene mobilities are much higher than in silicon due in part to the lack of Coulomb scattering. At high electric fields, the effect of phonon scattering significantly reduces the mobilities. JVST B - Microelectronics and Nanometer Structures Redistribution subject to AVS license or copyright; see http://scitation.aip.org/termsconditions. Download to IP: 18.51.1.88 On: Thu, 22 May 2014 16:13:48 C6D14 Tirado et al.: Study of transport properties in graphene monolayer flakes Temperature annealing effects have also been studied, revealing a clear influence on the transport properties of the material, shifting the valley of minimum conductivity to gate voltages closer to 0 V. The effect of temperature on the carrier mobilities has also been investigated, concluding that mobilities are not very dependent on temperature, although a light improvement with temperature has been observed. ACKNOWLEDGMENTS This work has been partially supported by Consejeria de Educacion y Ciencia de la Junta de Comunidades de Castilla-La Mancha and the European Social Fund. The MIT team acknowledges the support of the Microsystems Technology Laboratories. A. K. Geim and K. S. 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