graphene doping thesis

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• Published: 22 October 2021

High carrier mobility in graphene doped using a monolayer of tungsten oxyselenide

• Min Sup Choi 1 , 2   na1 ,
• Ankur Nipane 3   na1 ,
• Brian S. Y. Kim 1   na1 ,
• Mark E. Ziffer 4 ,
• Ipshita Datta 3 ,
• Abhinandan Borah 3 ,
• Younghun Jung 1 ,
• Bumho Kim 1 ,
• Daniel Rhodes 1 ,
• Apoorv Jindal 5 ,
• Zachary A. Lamport 3 ,
• Myeongjin Lee 2 ,
• Amirali Zangiabadi   ORCID: orcid.org/0000-0003-3586-0687 6 ,
• Maya N. Nair   ORCID: orcid.org/0000-0001-6532-8208 7 ,
• Takashi Taniguchi   ORCID: orcid.org/0000-0002-1467-3105 8 ,
• Kenji Watanabe   ORCID: orcid.org/0000-0003-3701-8119 8 ,
• Ioannis Kymissis 3 ,
• Abhay N. Pasupathy   ORCID: orcid.org/0000-0002-2744-0634 5 ,
• Michal Lipson   ORCID: orcid.org/0000-0003-2903-3765 3 ,
• Xiaoyang Zhu 4 ,
• Won Jong Yoo   ORCID: orcid.org/0000-0002-3767-7969 2 ,
• James Hone   ORCID: orcid.org/0000-0002-8084-3301 1 &
• James T. Teherani   ORCID: orcid.org/0000-0002-7778-8073 3  

Nature Electronics volume  4 ,  pages 731–739 ( 2021 ) Cite this article

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An Author Correction to this article was published on 24 November 2021

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Doped graphene could be of use in next-generation electronic and photonic devices. However, chemical doping cannot be precisely controlled in the material and leads to external disorder that diminishes carrier mobility and conductivity. Here we show that graphene can be efficiently doped using a monolayer of tungsten oxyselenide (TOS) that is created by oxidizing a monolayer of tungsten diselenide. When the TOS monolayer is in direct contact with graphene, a room-temperature mobility of 2,000 cm 2  V −1  s −1 at a hole density of 3 × 10 13  cm −2 is achieved. Hole density and mobility can also be controlled by inserting tungsten diselenide interlayers between TOS and graphene, where increasing the layers reduces the disorder. With four layers, a mobility value of around 24,000 cm 2  V −1  s −1 is observed, approaching the limit set by acoustic phonon scattering, resulting in a sheet resistance below 50 Ω sq −1 . To illustrate the potential of our approach, we show that TOS-doped graphene can be used as a transparent conductor in a near-infrared (1,550 nm) silicon nitride photonic waveguide and ring resonator.

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24 november 2021.

A Correction to this paper has been published: https://doi.org/10.1038/s41928-021-00696-5

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Acknowledgements

We acknowledge fruitful discussions with S. Chae, X. Xu, K. Yao, J. Schuck and E. Hwang, as well as experimental support from L. D’Cruz. This work was primarily supported by the NSF MRSEC Program at Columbia in the Center for Precision-Assembled Quantum Materials (DMR-2011736 and DMR-1420634), in partnership with the National Research Foundation of Korea through the Global Research Laboratory (GRL) program (2016K1A1A2912707) and Research Fellow program (2018R1A6A3A11045864). Device characterization was supported by the National Science Foundation through the CAREER Award (ECCS-1752401). This work was performed in part at the Advanced Science Research Center NanoFabrication Facility at the Graduate Center of the City University of New York and in part at the Columbia Nano Initiative (CNI) Shared Lab Facilities at Columbia University. Synthesis of hBN (K.W. and T.T.) was supported by the MEXT Element Strategy Initiative to Form Core Research Center (grant number JPMXP0112101001) and the CREST(JPMJCR15F3), JST.

Author information

These authors contributed equally: Min Sup Choi, Ankur Nipane, Brian S. Y. Kim.

Authors and Affiliations

Department of Mechanical Engineering, Columbia University, New York, NY, USA

Min Sup Choi, Brian S. Y. Kim, Younghun Jung, Bumho Kim, Daniel Rhodes & James Hone

SKKU Advanced Institute of Nano Technology, Sungkyunkwan University, Suwon, Korea

Min Sup Choi, Myeongjin Lee & Won Jong Yoo

Department of Electrical Engineering, Columbia University, New York, NY, USA

Ankur Nipane, Ipshita Datta, Abhinandan Borah, Zachary A. Lamport, Ioannis Kymissis, Michal Lipson & James T. Teherani

Department of Chemistry, Columbia University, New York, NY, USA

Mark E. Ziffer & Xiaoyang Zhu

Department of Physics, Columbia University, New York, NY, USA

Apoorv Jindal & Abhay N. Pasupathy

Department of Applied Physics and Applied Mathematics, Columbia University, New York, NY, USA

Amirali Zangiabadi

Nanoscience Initiative, Advanced Science Research Center, CUNY, New York, NY, USA

Maya N. Nair

National Institute for Materials Science, Tsukuba, Japan

Takashi Taniguchi & Kenji Watanabe

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Contributions

M.S.C., A.N. and Y.J. designed and conducted the initial experiments under the supervision of J.H. and J.T.T. M.S.C. and A.N. stacked, fabricated and conducted the electrical, optical and material characterizations of the samples with B.S.Y.K.’s contribution. B.S.Y.K. established a model for a work-function-mismatch-based doping mechanism. M.E.Z. and X.Z. contributed to the transmittance measurement of CVD samples. I.D. and M. Lipson contributed to the optical loss measurements of TOS-doped graphene integrated into the SiN waveguide. A.B. contributed to the doping study of DNTT. B.K. and D.R. provided flux-grown WSe 2 crystals. A.J. and A.N.P. provided the SWCNT grown on SiO 2 /Si. Z.A.L. and I.K. provided the grown DNTT on TOS. M. Lee contributed to the sample preparation. A.Z. contributed to the transmission electron microscopy, SAED and energy-dispersive X-ray spectroscopy measurements. M.N.N. contributed to the XPS measurements of CVD samples. T.T. and K.W. provided the hBN crystals. W.J.Y. contributed to discussions of the results. M.S.C., A.N. and B.S.Y.K. wrote the manuscript under the supervision of J.H. and J.T.T.

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Correspondence to James Hone or James T. Teherani .

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M.S.C., A.N., A.B., Y.J., J.H. and J.T.T. have filed for a US non-provisional patent application no. 17/236,404 regarding the technology reported in this article. The remaining authors declare no competing interests.

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Choi, M.S., Nipane, A., Kim, B.S.Y. et al. High carrier mobility in graphene doped using a monolayer of tungsten oxyselenide. Nat Electron 4 , 731–739 (2021). https://doi.org/10.1038/s41928-021-00657-y

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Published : 22 October 2021

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DOI : https://doi.org/10.1038/s41928-021-00657-y

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2014 Theses Doctoral

Towards inducing superconductivity into graphene

Efetov, Dmitri K.

Graphenes transport properties have been extensively studied in the 10 years since its discovery in 2004, with ground-breaking experimental observations such as Klein tunneling, fractional quantum Hall effect and Hofstadters butterfly. Though, so far, it turned out to be rather poor on complex correlated electronic ground states and phase transitions, despite various theoretical predictions. The purpose of this thesis is to help understanding the underlying theoretical and experimental reasons for the lack of strong electronic interactions in graphene, and, employing graphenes high tunability and versatility, to identify and alter experimental parameters that could help to induce stronger correlations. In particular graphene holds one last, not yet experimentally discovered prediction, namely exhibiting intrinsic superconductivity. With its vanishingly small Fermi surface at the Dirac point, graphene is a semi-metal with very weak electronic interactions. Though, if it is doped into the metallic regime, where the size of the Fermi surface becomes comparable to the size of the Brillouin zone, the density of states becomes sizeable and electronic interactions are predicted to be dramatically enhanced, resulting in competing correlated ground states such as superconductivity, magnetism and charge density wave formation. Following these predictions, this thesis first describes the creation of metallic graphene at high carrier doping via electrostatic doping techniques based on electrolytic gates. Due to graphenes surface only properties, we are able to induce carrier densities above n>10¹⁴cm⁻²(εF>1eV) into the chemically inert graphene. While at these record high carrier densities we yet do not observe superconductivity, we do observe fundamentally altered transport properties as compared to semi-metallic graphene. Here, detailed measurements of the low temperature resistivity reveal that the electron-phonon interactions are governed by a reduced, density dependent effective Debey temperature - the so-called Bloch-Grüneisen temperature ΘBG. We also probe the transport properties of the high energy sub-bands in bilayer graphene by electrolyte gating. Furthermore we demonstrate that electrolyte gates can be used to drive intercalation reactions in graphite and present an all optical study of the reaction kinetics during the creation of the graphene derived graphite intercalation compound LiC₆, and show the general applicability of the electrolyte gates to other 2-dimensional materials such as thin films of complex oxides, where we demonstrate gating dependent conductance changes in the spin-orbit Mott insulator Sr₂IrO₄. Another, entirely different approach to induce superconducting correlations into graphene is by bringing it into proximity to a superconductor. Although not intrinsic to graphene, Cooper pairs can leak in from the superconductor and exist in graphene in the form of phase-coherent electron-hole states, the so-called Andreev states. Here we demonstrate a new way of fabricating highly transparent graphene/superconductor junctions by vertical stacking of graphene and the type-II van der Waals superconductor NbSe₂. Due to NbSe₂'s high upper critical field of Hc₂= 4 T we are able to test a long proposed and yet not well understood regime, where proximity effect and quantum Hall effect coexist.

• Nanoscience
• Superconductivity
• Fermi surfaces
• Dirac equation
• Quantum Hall effect

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Alkali Metal Doped Graphene: Superconductivity, Structural, Magnetic and Optical Properties

• James Chapman
• Department of Physics & Astronomy

Student thesis : Phd

• Superconductivity

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Type : Thesis

Surface transfer hole doping of epitaxial graphene using MoO 3 thin film

Author to whom correspondence should be addressed. Electronic mail: [email protected] .

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Zhenyu Chen , Iman Santoso , Rui Wang , Lan Fei Xie , Hong Ying Mao , Han Huang , Yu Zhan Wang , Xing Yu Gao , Zhi Kuan Chen , Dongge Ma , Andrew Thye Shen Wee , Wei Chen; Surface transfer hole doping of epitaxial graphene using MoO 3 thin film. Appl. Phys. Lett. 24 May 2010; 96 (21): 213104. https://doi.org/10.1063/1.3441263

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Synchrotron-based in situ photoelectron spectroscopy investigations demonstrate effective surface transfer p-type doping of epitaxial graphene (EG) thermally grown on 4H–SiC(0001) via the deposition of MoO 3 thin film on top. The large work function difference between EG and MoO 3 facilitates electron transfer from EG to the MoO 3 thin film. This leads to hole accumulation in the EG layer with an areal hole density of about 1.0 × 10 13   cm − 2 ⁠ , and places the Fermi level 0.38 eV below the graphene Dirac point.

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Nitrogen-Doped Graphene Quantum Dots for Efficient Detection of Toxic Gas

• Topical Collection: Low-Energy Digital Devices and Computing 2023
• Published: 07 May 2024

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• Modhurima Bhuiya 1 ,
• Saurav Kumar 1 ,
• Aman Kumar 1 &
• Neha Agnihotri   ORCID: orcid.org/0000-0003-0500-2905 1  

Owing to their adjustable optoelectronic and adsorption characteristics, graphene quantum dots (GQDs) have become a potential material to manufacture effective gas sensors. Our present work deals with the study of interaction of a pristine graphene quantum dot (GQD) and a pyridinic nitrogen-doped defective graphene quantum dot (4N-GQD) with various toxic gases such as sulfur dioxide (SO 2 ), hydrogen fluoride (HF), hydrogen chloride (HCl), methane (CH 4 ), and carbon monoxide (CO). The 4N-GQD system has revealed strong interaction with these toxic gases in comparison to their pristine counterpart, which is because of the formation of an active region due to charge accumulation at the nitrogen-doped site. The adsorbate–adsorbent interaction in these systems has been studied at the molecular level employing density functional theory (DFT). Our findings suggest that the 4N-GQD system would be an effective adsorbent for a variety of toxic gases. These findings will help to steer the development of gas sensors with desirable features.

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The authors would like to express their gratitude to the Science and Engineering Research Board (SERB), New Delhi, India for providing the financial support.

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Modhurima Bhuiya, Saurav Kumar, Aman Kumar & Neha Agnihotri

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Bhuiya, M., Kumar, S., Kumar, A. et al. Nitrogen-Doped Graphene Quantum Dots for Efficient Detection of Toxic Gas. J. Electron. Mater. (2024). https://doi.org/10.1007/s11664-024-11123-8

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DOI : https://doi.org/10.1007/s11664-024-11123-8

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Green Chemistry

Boosting the catalytic performance of ru nanoparticles in the cleavage of β-o-4 linkages in lignin by doping mo †.

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a Department of Electronic Engineering, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China E-mail: [email protected]

In this work, Ru nanoparticles doped with Mo on reduced graphene oxide (RuMo/rGO) are prepared through synchronous reduction of RuCl 3 , MoCl 5 , and graphene oxide. The compositions, morphologies, and structures of the as-prepared RuMo/rGO composites are fully characterized. Their catalytic properties in oxidative cleavage of β-O-4 linkages in lignin model compounds and lignin are explored. It is illustrated that with O 2 as the oxidant RuMo/rGO shows overall better catalytic performance in the oxidative cleavage of β-O-4 linkages than the catalysts, such as Ru/rGO and RuCo/rGO, reported in our previous work. The catalytic mechanism is elaborated through experiments and density functional theory (DFT) calculation. Pronouncedly, we show that the as-doped Mo can effectively boost the molecular oxygen activation process and the adsorption of β-O-4 model compounds on the Ru nanoparticle surface on rGO, and thus enhance the catalytic activity. It is demonstrated meanwhile that RuMo/rGO can catalyze the depolymerization of organosolv birch lignin yielding 17.1% aromatic compounds under relatively mild conditions (100 °C, 0.3 MPa O 2 , 12 h, pH = 12).

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Boosting the catalytic performance of Ru nanoparticles in the cleavage of β-O-4 linkages in lignin by doping Mo

P. Lei, J. Zhang, W. Shen, M. Zhong and S. Guo, Green Chem. , 2024, Advance Article , DOI: 10.1039/D4GC00294F

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