DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Chemical vapor deposition of monolayer MoS2 directly on ultrathin Al2O3 for low-power electronics

Abstract

Monolayer MoS2 has recently been identified as a promising material for high-performance electronics. However, monolayer MoS2 must be integrated with ultrathin high-κ gate dielectrics in order to realize practical low-power devices. In this paper, we report the chemical vapor deposition (CVD) of monolayer MoS2 directly on 20 nm thick Al2O3 grown by atomic layer deposition (ALD). The quality of the resulting MoS2 is characterized by a comprehensive set of microscopic and spectroscopic techniques. Furthermore, a low-temperature (200 °C) Al2O3 ALD process is developed that maintains dielectric integrity following the high-temperature CVD of MoS2 (800 °C). Field-effect transistors (FETs) derived from these MoS2/Al2O3 stacks show minimal hysteresis with a sub-threshold swing as low as ~220 mV/decade, threshold voltages of ~2 V, and current ION/IOFF ratio as high as ~104, where IOFF is defined as the current at zero gate voltage as is customary for determining power consumption in complementary logic circuits. Finally, the system presented here concurrently optimizes multiple low-power electronics figures of merit while providing a transfer-free method of integrating monolayer MoS2 with ultrathin high-κ dielectrics, thus enabling a scalable pathway for enhancement-mode FETs for low-power applications.

Authors:
 [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  2. Northwestern Univ., Evanston, IL (United States). Applied Physics Graduate Program
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering. Applied Physics Graduate Program. Dept. of Physics and Astronomy
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering. Dept. of Chemistry
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering. Applied Physics Graduate Program. Dept. of Chemistry. Dept. of Electrical Engineering and Computer Science
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Inst. of Standards and Technology (NIST) (United States); National Science Foundation (NSF); National Aeronautics and Space Administration (NASA); Office of Naval Research (ONR) (United States)
OSTI Identifier:
1465963
Alternate Identifier(s):
OSTI ID: 1351027
Grant/Contract Number:  
SC0001059; 70NANB14H012; EFRI-1433510; DMR-1121262; NNCI-1542205; NNX12AM44H; N00014-14-1-0669
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 110; Journal Issue: 5; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; doping; metal insulator semiconductor structures; semiconductor growth; chemical vapor deposition; atomic layer deposition; dielectric materials; dielectric thin films; monolayers; field effect transistors

Citation Formats

Bergeron, Hadallia, Sangwan, Vinod K., McMorrow, Julian J., Campbell, Gavin P., Balla, Itamar, Liu, Xiaolong, Bedzyk, Michael J., Marks, Tobin J., and Hersam, Mark C. Chemical vapor deposition of monolayer MoS2 directly on ultrathin Al2O3 for low-power electronics. United States: N. p., 2017. Web. doi:10.1063/1.4975064.
Bergeron, Hadallia, Sangwan, Vinod K., McMorrow, Julian J., Campbell, Gavin P., Balla, Itamar, Liu, Xiaolong, Bedzyk, Michael J., Marks, Tobin J., & Hersam, Mark C. Chemical vapor deposition of monolayer MoS2 directly on ultrathin Al2O3 for low-power electronics. United States. https://doi.org/10.1063/1.4975064
Bergeron, Hadallia, Sangwan, Vinod K., McMorrow, Julian J., Campbell, Gavin P., Balla, Itamar, Liu, Xiaolong, Bedzyk, Michael J., Marks, Tobin J., and Hersam, Mark C. Mon . "Chemical vapor deposition of monolayer MoS2 directly on ultrathin Al2O3 for low-power electronics". United States. https://doi.org/10.1063/1.4975064. https://www.osti.gov/servlets/purl/1465963.
@article{osti_1465963,
title = {Chemical vapor deposition of monolayer MoS2 directly on ultrathin Al2O3 for low-power electronics},
author = {Bergeron, Hadallia and Sangwan, Vinod K. and McMorrow, Julian J. and Campbell, Gavin P. and Balla, Itamar and Liu, Xiaolong and Bedzyk, Michael J. and Marks, Tobin J. and Hersam, Mark C.},
abstractNote = {Monolayer MoS2 has recently been identified as a promising material for high-performance electronics. However, monolayer MoS2 must be integrated with ultrathin high-κ gate dielectrics in order to realize practical low-power devices. In this paper, we report the chemical vapor deposition (CVD) of monolayer MoS2 directly on 20 nm thick Al2O3 grown by atomic layer deposition (ALD). The quality of the resulting MoS2 is characterized by a comprehensive set of microscopic and spectroscopic techniques. Furthermore, a low-temperature (200 °C) Al2O3 ALD process is developed that maintains dielectric integrity following the high-temperature CVD of MoS2 (800 °C). Field-effect transistors (FETs) derived from these MoS2/Al2O3 stacks show minimal hysteresis with a sub-threshold swing as low as ~220 mV/decade, threshold voltages of ~2 V, and current ION/IOFF ratio as high as ~104, where IOFF is defined as the current at zero gate voltage as is customary for determining power consumption in complementary logic circuits. Finally, the system presented here concurrently optimizes multiple low-power electronics figures of merit while providing a transfer-free method of integrating monolayer MoS2 with ultrathin high-κ dielectrics, thus enabling a scalable pathway for enhancement-mode FETs for low-power applications.},
doi = {10.1063/1.4975064},
journal = {Applied Physics Letters},
number = 5,
volume = 110,
place = {United States},
year = {Mon Jan 30 00:00:00 EST 2017},
month = {Mon Jan 30 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 63 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

High-Gain Phototransistors Based on a CVD MoS 2 Monolayer
journal, May 2013

  • Zhang, Wenjing; Huang, Jing-Kai; Chen, Chang-Hsiao
  • Advanced Materials, Vol. 25, Issue 25
  • DOI: 10.1002/adma.201301244

Controlled Scalable Synthesis of Uniform, High-Quality Monolayer and Few-layer MoS2 Films
journal, May 2013

  • Yu, Yifei; Li, Chun; Liu, Yi
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01866

Intrinsic carrier mobility of multi-layered MoS 2 field-effect transistors on SiO 2
journal, March 2013

  • Pradhan, N. R.; Rhodes, D.; Zhang, Q.
  • Applied Physics Letters, Vol. 102, Issue 12
  • DOI: 10.1063/1.4799172

High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity
journal, April 2015


Large-Area Vapor-Phase Growth and Characterization of MoS2 Atomic Layers on a SiO2 Substrate
journal, February 2012


Subnanowatt Carbon Nanotube Complementary Logic Enabled by Threshold Voltage Control
journal, September 2013

  • Geier, Michael L.; Prabhumirashi, Pradyumna L.; McMorrow, Julian J.
  • Nano Letters, Vol. 13, Issue 10
  • DOI: 10.1021/nl402478p

Scalable Growth of High-Quality Polycrystalline MoS 2 Monolayers on SiO 2 with Tunable Grain Sizes
journal, May 2014


High mobility ambipolar MoS 2 field-effect transistors: Substrate and dielectric effects
journal, January 2013

  • Bao, Wenzhong; Cai, Xinghan; Kim, Dohun
  • Applied Physics Letters, Vol. 102, Issue 4
  • DOI: 10.1063/1.4789365

Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Low-Temperature Al2O3 Atomic Layer Deposition
journal, February 2004

  • Groner, M. D.; Fabreguette, F. H.; Elam, J. W.
  • Chemistry of Materials, Vol. 16, Issue 4, p. 639-645
  • DOI: 10.1021/cm0304546

Synthesis and Transfer of Single-Layer Transition Metal Disulfides on Diverse Surfaces
journal, March 2013

  • Lee, Yi-Hsien; Yu, Lili; Wang, Han
  • Nano Letters, Vol. 13, Issue 4
  • DOI: 10.1021/nl400687n

How Good Can Monolayer MoS 2 Transistors Be?
journal, September 2011

  • Yoon, Youngki; Ganapathi, Kartik; Salahuddin, Sayeef
  • Nano Letters, Vol. 11, Issue 9
  • DOI: 10.1021/nl2018178

The effect of the substrate on the Raman and photoluminescence emission of single-layer MoS2
journal, April 2014


Electronic transport and device prospects of monolayer molybdenum disulphide grown by chemical vapour deposition
journal, January 2014

  • Zhu, Wenjuan; Low, Tony; Lee, Yi-Hsien
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4087

Transition Metal Dichalcogenide Growth via Close Proximity Precursor Supply
journal, December 2014

  • O'Brien, Maria; McEvoy, Niall; Hallam, Toby
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep07374

Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


Synthesis of Large-Area MoS2 Atomic Layers with Chemical Vapor Deposition
journal, March 2012

  • Lee, Yi-Hsien; Zhang, Xin-Quan; Zhang, Wenjing
  • Advanced Materials, Vol. 24, Issue 17, p. 2320-2325
  • DOI: 10.1002/adma.201104798

Design, Modeling, and Fabrication of Chemical Vapor Deposition Grown MoS 2 Circuits with E-Mode FETs for Large-Area Electronics
journal, September 2016


$\hbox{MoS}_{2}$ Dual-Gate MOSFET With Atomic-Layer-Deposited $\hbox{Al}_{2}\hbox{O}_{3}$ as Top-Gate Dielectric
journal, April 2012


High mobility and high on/off ratio field-effect transistors based on chemical vapor deposited single-crystal MoS 2 grains
journal, April 2013

  • Wu, Wei; De, Debtanu; Chang, Su-Chi
  • Applied Physics Letters, Vol. 102, Issue 14
  • DOI: 10.1063/1.4801861

High-mobility and low-power thin-film transistors based on multilayer MoS2 crystals
journal, January 2012

  • Kim, Sunkook; Konar, Aniruddha; Hwang, Wan-Sik
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2018

Solution-processed carbon nanotube thin-film complementary static random access memory
journal, September 2015

  • Geier, Michael L.; McMorrow, Julian J.; Xu, Weichao
  • Nature Nanotechnology, Vol. 10, Issue 11
  • DOI: 10.1038/nnano.2015.197

Band-like transport in high mobility unencapsulated single-layer MoS 2 transistors
journal, April 2013

  • Jariwala, Deep; Sangwan, Vinod K.; Late, Dattatray J.
  • Applied Physics Letters, Vol. 102, Issue 17
  • DOI: 10.1063/1.4803920

Flexible MoS 2 Field-Effect Transistors for Gate-Tunable Piezoresistive Strain Sensors
journal, March 2015

  • Tsai, Meng-Yen; Tarasov, Alexey; Hesabi, Zohreh R.
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 23
  • DOI: 10.1021/acsami.5b02336

Electrical transport and low-frequency noise in chemical vapor deposited single-layer MoS 2 devices
journal, March 2014


From Bulk to Monolayer MoS2: Evolution of Raman Scattering
journal, January 2012

  • Li, Hong; Zhang, Qing; Yap, Chin Chong Ray
  • Advanced Functional Materials, Vol. 22, Issue 7
  • DOI: 10.1002/adfm.201102111

Fundamental Performance Limits of Carbon Nanotube Thin-Film Transistors Achieved Using Hybrid Molecular Dielectrics
journal, July 2012

  • Sangwan, Vinod K.; Ortiz, Rocio Ponce; Alaboson, Justice M. P.
  • ACS Nano, Vol. 6, Issue 8
  • DOI: 10.1021/nn302768h

Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide
journal, May 2013

  • van der Zande, Arend M.; Huang, Pinshane Y.; Chenet, Daniel A.
  • Nature Materials, Vol. 12, Issue 6, p. 554-561
  • DOI: 10.1038/nmat3633

Highly Uniform Trilayer Molybdenum Disulfide for Wafer-Scale Device Fabrication
journal, August 2014

  • Tarasov, Alexey; Campbell, Philip M.; Tsai, Meng-Yen
  • Advanced Functional Materials, Vol. 24, Issue 40
  • DOI: 10.1002/adfm.201401389

Scalable synthesis of layer-controlled WS 2 and MoS 2 sheets by sulfurization of thin metal films
journal, August 2014

  • Orofeo, Carlo M.; Suzuki, Satoru; Sekine, Yoshiaki
  • Applied Physics Letters, Vol. 105, Issue 8
  • DOI: 10.1063/1.4893978

Hysteresis in Single-Layer MoS 2 Field Effect Transistors
journal, May 2012

  • Late, Dattatray J.; Liu, Bin; Matte, H. S. S. Ramakrishna
  • ACS Nano, Vol. 6, Issue 6
  • DOI: 10.1021/nn301572c

Channel Length Scaling of MoS 2 MOSFETs
journal, September 2012

  • Liu, Han; Neal, Adam T.; Ye, Peide D.
  • ACS Nano, Vol. 6, Issue 10
  • DOI: 10.1021/nn303513c

Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers
journal, June 2013

  • Najmaei, Sina; Liu, Zheng; Zhou, Wu
  • Nature Materials, Vol. 12, Issue 8, p. 754-759
  • DOI: 10.1038/nmat3673

Seeding Atomic Layer Deposition of High- k Dielectrics on Epitaxial Graphene with Organic Self-Assembled Monolayers
journal, May 2011

  • Alaboson, Justice M. P.; Wang, Qing Hua; Emery, Jonathan D.
  • ACS Nano, Vol. 5, Issue 6
  • DOI: 10.1021/nn201414d

Synchrotron X-ray reflectivity study of high dielectric constant alumina thin films prepared by atomic layer deposition
journal, July 2006


Integrated Circuits Based on Bilayer MoS2 Transistors
journal, January 2012

  • Wang, Han; Yu, Lili; Lee, Yi-Hsien
  • Nano Letters, Vol. 12, Issue 9, p. 4674-4680
  • DOI: 10.1021/nl302015v

Chemical Vapor Deposition of High-Quality Large-Sized MoS 2 Crystals on Silicon Dioxide Substrates
journal, March 2016


Growth-substrate induced performance degradation in chemically synthesized monolayer MoS 2 field effect transistors
journal, May 2014

  • Amani, Matin; Chin, Matthew L.; Mazzoni, Alexander L.
  • Applied Physics Letters, Vol. 104, Issue 20
  • DOI: 10.1063/1.4873680

XPS investigation of preferential sputtering of S from MoS2 and determination of MoSx stoichiometry from Mo and S peak positions
journal, August 1999


Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

  • Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
  • Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
  • DOI: 10.1038/nnano.2012.193

Large-scale chemical assembly of atomically thin transistors and circuits
journal, July 2016


Electrical Transport Properties of Polycrystalline Monolayer Molybdenum Disulfide
journal, July 2014

  • Najmaei, Sina; Amani, Matin; Chin, Matthew L.
  • ACS Nano, Vol. 8, Issue 8
  • DOI: 10.1021/nn501701a

MoS2 and WS2 Analogues of Graphene
journal, April 2010

  • Ramakrishna Matte, H. S. S.; Gomathi, A.; Manna, Arun K.
  • Angewandte Chemie, Vol. 122, Issue 24
  • DOI: 10.1002/ange.201000009

Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides
journal, January 2014

  • Jariwala, Deep; Sangwan, Vinod K.; Lauhon, Lincoln J.
  • ACS Nano, Vol. 8, Issue 2
  • DOI: 10.1021/nn500064s

Post deposition annealing of aluminum oxide deposited by atomic layer deposition using tris(diethylamino)aluminum and water vapor on Si(100)
journal, June 2007


An XPS study of the surface modification of natural MoS2 following treatment in an RF-oxygen plasma
journal, September 1998


Growth of Large-Scale and Thickness-Modulated MoS 2 Nanosheets
journal, November 2014

  • Choudhary, Nitin; Park, Juhong; Hwang, Jun Yeon
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 23
  • DOI: 10.1021/am506198b

Exploring atomic defects in molybdenum disulphide monolayers
journal, February 2015

  • Hong, Jinhua; Hu, Zhixin; Probert, Matt
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7293

Transport Properties of Monolayer MoS 2 Grown by Chemical Vapor Deposition
journal, March 2014

  • Schmidt, Hennrik; Wang, Shunfeng; Chu, Leiqiang
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl4046922

Electronics based on two-dimensional materials
journal, October 2014

  • Fiori, Gianluca; Bonaccorso, Francesco; Iannaccone, Giuseppe
  • Nature Nanotechnology, Vol. 9, Issue 10
  • DOI: 10.1038/nnano.2014.207

Synthesis of wafer-scale uniform molybdenum disulfide films with control over the layer number using a gas phase sulfur precursor
journal, January 2014

  • Lee, Youngbin; Lee, Jinhwan; Bark, Hunyoung
  • Nanoscale, Vol. 6, Issue 5
  • DOI: 10.1039/c3nr05993f

A roadmap for graphene
journal, October 2012

  • Novoselov, K. S.; Fal′ko, V. I.; Colombo, L.
  • Nature, Vol. 490, Issue 7419
  • DOI: 10.1038/nature11458

Influence of Stoichiometry on the Optical and Electrical Properties of Chemical Vapor Deposition Derived MoS 2
journal, September 2014

  • Kim, In Soo; Sangwan, Vinod K.; Jariwala, Deep
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn503988x

Layer-controlled CVD growth of large-area two-dimensional MoS 2 films
journal, January 2015

  • Jeon, Jaeho; Jang, Sung Kyu; Jeon, Su Min
  • Nanoscale, Vol. 7, Issue 5
  • DOI: 10.1039/C4NR04532G

Rotationally Commensurate Growth of MoS 2 on Epitaxial Graphene
journal, November 2015


Seeded growth of highly crystalline molybdenum disulphide monolayers at controlled locations
journal, January 2015

  • Han, Gang Hee; Kybert, Nicholas J.; Naylor, Carl H.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7128

Single-layer MoS2 transistors
journal, January 2011

  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Top-gated chemical vapor deposited MoS 2 field-effect transistors on Si 3 N 4 substrates
journal, February 2015

  • Sanne, A.; Ghosh, R.; Rai, A.
  • Applied Physics Letters, Vol. 106, Issue 6
  • DOI: 10.1063/1.4907885

Integrated Flexible and High-Quality Thin Film Transistors Based on Monolayer MoS 2
journal, January 2016

  • Zhao, Jing; Chen, Wei; Meng, Jianling
  • Advanced Electronic Materials, Vol. 2, Issue 3
  • DOI: 10.1002/aelm.201500379

Nature of Electronic States in Atomically Thin MoS2 Field-Effect Transistors
journal, October 2011

  • Ghatak, Subhamoy; Pal, Atindra Nath; Ghosh, Arindam
  • ACS Nano, Vol. 5, Issue 10, p. 7707-7712
  • DOI: 10.1021/nn202852j

Air Stable Doping and Intrinsic Mobility Enhancement in Monolayer Molybdenum Disulfide by Amorphous Titanium Suboxide Encapsulation
journal, June 2015


Works referencing / citing this record:

Large-Area Chemical Vapor Deposited MoS 2 with Transparent Conducting Oxide Contacts toward Fully Transparent 2D Electronics
journal, September 2017

  • Dai, Zhenyu; Wang, Zhenwei; He, Xin
  • Advanced Functional Materials, Vol. 27, Issue 41
  • DOI: 10.1002/adfm.201703119

Recent advances in two‐dimensional transition metal dichalcogenides as photoelectrocatalyst for hydrogen evolution reaction
journal, January 2020

  • Nguyen, Van‐Huy; Nguyen, Thang P.; Le, Thu‐Ha
  • Journal of Chemical Technology & Biotechnology
  • DOI: 10.1002/jctb.6335

Photoluminescence Study of B-Trions in MoS 2 Monolayers with High Density of Defects
journal, October 2018

  • Kaupmees, Reelika; Komsa, Hannu-Pekka; Krustok, Jüri
  • physica status solidi (b), Vol. 256, Issue 3
  • DOI: 10.1002/pssb.201800384

A review on chemiresistive room temperature gas sensors based on metal oxide nanostructures, graphene and 2D transition metal dichalcogenides
journal, March 2018


Mixed-dimensional 2D/3D heterojunctions between MoS 2 and Si(100)
journal, January 2018

  • Choi, Hyunsoo; Min, Kyung-Ah; Cha, Janghwan
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 39
  • DOI: 10.1039/c8cp05201h

Role of oxygen adsorption in modification of optical and surface electronic properties of MoS 2
journal, April 2018

  • Shakya, Jyoti; Kumar, Sanjeev; Mohanty, Tanuja
  • Journal of Applied Physics, Vol. 123, Issue 16
  • DOI: 10.1063/1.5023022

2D group 6 transition metal dichalcogenides toward wearable electronics and optoelectronics
journal, January 2020

  • Yao, Jiandong; Yang, Guowei
  • Journal of Applied Physics, Vol. 127, Issue 3
  • DOI: 10.1063/1.5140795

Near-ideal subthreshold swing MoS 2 back-gate transistors with an optimized ultrathin HfO 2 dielectric layer
journal, January 2019


A modified wrinkle-free MoS 2 film transfer method for large area high mobility field-effect transistor
journal, November 2019


Mask-free patterning and selective CVD-growth of 2D-TMDCs semiconductors
journal, July 2019

  • Alameri, Dheyaa; Nasr, Joseph R.; Karbach, Devon
  • Semiconductor Science and Technology, Vol. 34, Issue 8
  • DOI: 10.1088/1361-6641/ab28db