Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation

Li, Xufan; Lin, Ming -Wei; Basile, Leonardo; Hus, Saban M.; Puretzky, Alexander A.; Lee, Jaekwang; Kuo, Yen -Chien; Chang, Lo -Yueh; Wang, Kai; Idrobo, Juan C.; Li, An -Ping; Chen, Chia-Hao; Rouleau, Christopher M.; Geohegan, David B.; Xiao, Kai

doi:10.1002/adma.201601991

Title: Isoelectronic tungsten doping in monolayer MoSe₂ for carrier type modulation

Journal Article · Wed Jul 06 00:00:00 EDT 2016 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201601991· OSTI ID:1329120

Li, Xufan ^[1]; Lin, Ming -Wei ^[1]; Basile, Leonardo ^[2]; Hus, Saban M. ^[1]; Puretzky, Alexander A. ^[1]; Lee, Jaekwang ^[3]; Kuo, Yen -Chien ^[4]; Chang, Lo -Yueh ^[4]; Wang, Kai ^[1]; Idrobo, Juan C. ^[1]; Li, An -Ping ^[1]; Chen, Chia-Hao ^[4]; Rouleau, Christopher M. ^[1]; Geohegan, David B. ^[1]; Xiao, Kai ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Escuela Politecnica Nacional, Quito (Ecuador)
Pusan National Univ., Busan (South Korea)
National Synchrotron Radiation Research Center (NSRRC), Hsinchu (Taiwan)

Doping and alloying are effective ways to engineer the band structure and modulate the optoelectronic functionality of monolayer transition metal dichalcogenides (TMDs). In this work, we explore the synthesis and electronic properties of monolayer Mo_1-xW_xSe₂ (0 < x < 0.18) alloys with almost 100% alloying degree. The isoelectronic substitutional doping of tungsten for molybdenum in the monolayer MoSe₂ is shown to suppress its intrinsically n-type conduction behavior, with p-type conduction gradually emerging to become dominant with increasing W concentration in the alloys. Atomic resolution Z-contrast electron microscopy show that W is shown to substitute directly for Mo without the introduction of noticeable vacancy or interstitial defects, however with randomly-distributed W-rich regions ~2 nm in diameter. Scanning tunneling microscopy/spectroscopy measurements reveal that these W-rich regions exhibit a local band structure with the valence band maximum (VBM) closer to the Fermi level as compared with the Mo-rich regions in the monolayer Mo_1-xW_xSe₂ crystal. These localized upshifts of the VBM in the local band structure appear responsible for the overall p-type behavior observed for the monolayer Mo_1-xW_xSe₂ crystals. Stacked monolayers of n-type MoSe₂ and p-type Mo_1-xW_xSe₂ were demonstrated to form atomically thin, vertically stacked p n homojunctions with gate-tunable characteristics, which appear useful for future optoelectronic applications. Lastly, these results indicate that alloying with isoelectronic dopant atoms appears to be an effective and advantageous alternate strategy to doping or alloying with electron donors or acceptors in two-dimensional TMDs.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1329120

Journal Information:: Advanced Materials, Vol. 28, Issue 37; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 72 works

Citation information provided by
Web of Science

References (42)

Origin of the $n$ -type and $p$ -type conductivity of MoS $_{2}$ monolayers on a SiO $_{2}$ substrate Dolui, Kapildeb; Rungger, Ivan; Sanvito, Stefano Physical Review B, Vol. 87, Issue 16 https://doi.org/10.1103/PhysRevB.87.165402	journal	April 2013
Spin-orbit engineering in transition metal dichalcogenide alloy monolayers Wang, Gang; Robert, Cedric; Suslu, Aslihan Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms10110	journal	December 2015
Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene Butler, Sheneve Z.; Hollen, Shawna M.; Cao, Linyou ACS Nano, Vol. 7, Issue 4, p. 2898-2926 https://doi.org/10.1021/nn400280c	journal	March 2013
Engineering electronic properties of layered transition-metal dichalcogenide compounds through alloying Kutana, Alex; Penev, Evgeni S.; Yakobson, Boris I. Nanoscale, Vol. 6, Issue 11 https://doi.org/10.1039/C4NR00177J	journal	January 2014
Controllable synthesis of molybdenum tungsten disulfide alloy for vertically composition-controlled multilayer Song, Jeong-Gyu; Ryu, Gyeong Hee; Lee, Su Jeong Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8817	journal	July 2015
Structural Models and Atomic Distribution of Bimetallic Nanoparticles as Investigated by X-ray Absorption Spectroscopy Hwang, Bing-Joe; Sarma, Loka Subramanyam; Chen, Jiun-Ming Journal of the American Chemical Society, Vol. 127, Issue 31 https://doi.org/10.1021/ja0526618	journal	August 2005
Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials Bernardi, Marco; Palummo, Maurizia; Grossman, Jeffrey C. Nano Letters, Vol. 13, Issue 8, p. 3664-3670 https://doi.org/10.1021/nl401544y	journal	July 2013
Two-dimensional semiconductor alloys: Monolayer Mo _1−x W _x Se ₂ Tongay, Sefaattin; Narang, Deepa S.; Kang, Jun Applied Physics Letters, Vol. 104, Issue 1 https://doi.org/10.1063/1.4834358	journal	January 2014
Electroluminescence and Photocurrent Generation from Atomically Sharp WSe ₂ /MoS ₂ Heterojunction p–n Diodes Cheng, Rui; Li, Dehui; Zhou, Hailong Nano Letters, Vol. 14, Issue 10 https://doi.org/10.1021/nl502075n	journal	September 2014
Large Area Growth and Electrical Properties of p-Type WSe ₂ Atomic Layers Zhou, Hailong; Wang, Chen; Shaw, Jonathan C. Nano Letters, Vol. 15, Issue 1 https://doi.org/10.1021/nl504256y	journal	December 2014
Graphene as tunable transparent electrode material on GaN: Layer-number-dependent optical and electrical properties Wei, Hung; Chang, Lo Yueh; Lee, Kai-Hsuan Applied Physics Letters, Vol. 103, Issue 8 https://doi.org/10.1063/1.4818787	journal	January 2013
Decrease of dislocations in GaAs by isoelectronic doping of liquid phase epitaxial layers Liu, Wenjie; Chen, Nuofu Journal of Crystal Growth, Vol. 154, Issue 1-2 https://doi.org/10.1016/0022-0248(95)00173-5	journal	September 1995
Lateral epitaxial growth of two-dimensional layered semiconductor heterojunctions Duan, Xidong; Wang, Chen; Shaw, Jonathan C. Nature Nanotechnology, Vol. 9, Issue 12, p. 1024-1030 https://doi.org/10.1038/nnano.2014.222	journal	September 2014
Alloy Engineering of Defect Properties in Semiconductors: Suppression of Deep Levels in Transition-Metal Dichalcogenides Huang, Bing; Yoon, Mina; Sumpter, Bobby G. Physical Review Letters, Vol. 115, Issue 12 https://doi.org/10.1103/PhysRevLett.115.126806	journal	September 2015
Doping against the Native Propensity of MoS ₂ : Degenerate Hole Doping by Cation Substitution Suh, Joonki; Park, Tae-Eon; Lin, Der-Yuh Nano Letters, Vol. 14, Issue 12 https://doi.org/10.1021/nl503251h	journal	November 2014
Chemical Vapor Deposition Growth of Crystalline Monolayer MoSe₂ Wang, Xingli; Gong, Yongji; Shi, Gang ACS Nano, Vol. 8, Issue 5, p. 5125-5131 https://doi.org/10.1021/nn501175k	journal	April 2014
Twisted MoSe ₂ Bilayers with Variable Local Stacking and Interlayer Coupling Revealed by Low-Frequency Raman Spectroscopy Puretzky, Alexander A.; Liang, Liangbo; Li, Xufan ACS Nano, Vol. 10, Issue 2 https://doi.org/10.1021/acsnano.5b07807	journal	January 2016
Tunable Photoluminescence of Monolayer MoS ₂ via Chemical Doping Mouri, Shinichiro; Miyauchi, Yuhei; Matsuda, Kazunari Nano Letters, Vol. 13, Issue 12 https://doi.org/10.1021/nl403036h	journal	November 2013
Growth of Alloy MoS_2xSe_2(1–x) Nanosheets with Fully Tunable Chemical Compositions and Optical Properties Li, Honglai; Duan, Xidong; Wu, Xueping Journal of the American Chemical Society, Vol. 136, Issue 10, p. 3756-3759 https://doi.org/10.1021/ja500069b	journal	February 2014
Functionalization of Single-Layer MoS ₂ Honeycomb Structures Ataca, C.; Ciraci, S. The Journal of Physical Chemistry C, Vol. 115, Issue 27 https://doi.org/10.1021/jp2000442	journal	June 2011
Degenerate n-Doping of Few-Layer Transition Metal Dichalcogenides by Potassium Fang, Hui; Tosun, Mahmut; Seol, Gyungseon Nano Letters, Vol. 13, Issue 5, p. 1991-1995 https://doi.org/10.1021/nl400044m	journal	April 2013
Ultrasensitive photodetectors based on monolayer MoS2 Lopez-Sanchez, Oriol; Lembke, Dominik; Kayci, Metin Nature Nanotechnology, Vol. 8, Issue 7 https://doi.org/10.1038/nnano.2013.100	journal	June 2013
Tunable Electronic Properties of Two-Dimensional Transition Metal Dichalcogenide Alloys: A First-Principles Prediction Xi, Jinyang; Zhao, Tianqi; Wang, Dong The Journal of Physical Chemistry Letters, Vol. 5, Issue 2 https://doi.org/10.1021/jz402375s	journal	December 2013
Single-Layer Group-III Monochalcogenide Photocatalysts for Water Splitting Zhuang, Houlong L.; Hennig, Richard G. Chemistry of Materials, Vol. 25, Issue 15 https://doi.org/10.1021/cm401661x	journal	July 2013
A Van Der Waals Homojunction: Ideal p-n Diode Behavior in MoSe ₂ Jin, Youngjo; Keum, Dong Hoon; An, Sung-Jin Advanced Materials, Vol. 27, Issue 37 https://doi.org/10.1002/adma.201502278	journal	August 2015
Symmetry-dependent phonon renormalization in monolayer MoS $_{2}$ transistor Chakraborty, Biswanath; Bera, Achintya; Muthu, D. V. S. Physical Review B, Vol. 85, Issue 16 https://doi.org/10.1103/PhysRevB.85.161403	journal	April 2012
Stress, structural and electrical properties of Si-doped GaN film grown by MOCVD Zhihao, Xu; Jincheng, Zhang; Huantao, Duan Journal of Semiconductors, Vol. 30, Issue 12 https://doi.org/10.1088/1674-4926/30/12/123003	journal	December 2009
Visualization and quantification of transition metal atomic mixing in Mo_1−xW_xS₂ single layers Dumcenco, Dumitru O.; Kobayashi, Haruka; Liu, Zheng Nature Communications, Vol. 4, Article No. 1351 https://doi.org/10.1038/ncomms2351	journal	January 2013
Single-layer MoS₂ transistors Radisavljevic, B.; Radenovic, A.; Brivio, J. Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150 https://doi.org/10.1038/nnano.2010.279	journal	January 2011
Monolayer semiconductor nanocavity lasers with ultralow thresholds Wu, Sanfeng; Buckley, Sonia; Schaibley, John R. Nature, Vol. 520, Issue 7545 https://doi.org/10.1038/nature14290	journal	March 2015
2-Dimensional Transition Metal Dichalcogenides with Tunable Direct Band Gaps: MoS _2(1-x) Se _2x Monolayers Mann, John; Ma, Quan; Odenthal, Patrick M. Advanced Materials, Vol. 26, Issue 9 https://doi.org/10.1002/adma.201304389	journal	December 2013
Ultimate thin vertical p–n junction composed of two-dimensional layered molybdenum disulfide Li, Hua-Min; Lee, Daeyeong; Qu, Deshun Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7564	journal	March 2015
Manganese Doping of Monolayer MoS ₂ : The Substrate Is Critical Zhang, Kehao; Feng, Simin; Wang, Junjie Nano Letters, Vol. 15, Issue 10 https://doi.org/10.1021/acs.nanolett.5b02315	journal	September 2015
Microscopic basis for the band engineering of Mo1−xWxS2-based heterojunction Yoshida, Shoji; Kobayashi, Yu; Sakurada, Ryuji Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep14808	journal	October 2015
Role of Metal Contacts in Designing High-Performance Monolayer n-Type WSe ₂ Field Effect Transistors Liu, Wei; Kang, Jiahao; Sarkar, Deblina Nano Letters, Vol. 13, Issue 5 https://doi.org/10.1021/nl304777e	journal	April 2013
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4061	journal	August 2014
Band Gap Engineering and Layer-by-Layer Mapping of Selenium-Doped Molybdenum Disulfide Gong, Yongji; Liu, Zheng; Lupini, Andrew R. Nano Letters, Vol. 14, Issue 2 https://doi.org/10.1021/nl4032296	journal	December 2013
Zeeman-type spin splitting controlled by an electric field Yuan, Hongtao; Bahramy, Mohammad Saeed; Morimoto, Kazuhiro Nature Physics, Vol. 9, Issue 9 https://doi.org/10.1038/nphys2691	journal	July 2013
Broad-Range Modulation of Light Emission in Two-Dimensional Semiconductors by Molecular Physisorption Gating Tongay, Sefaattin; Zhou, Jian; Ataca, Can Nano Letters, Vol. 13, Issue 6 https://doi.org/10.1021/nl4011172	journal	May 2013
Possible doping strategies for MoS $_{2}$ monolayers: An ab initio study Dolui, Kapildeb; Rungger, Ivan; Das Pemmaraju, Chaitanya Physical Review B, Vol. 88, Issue 7 https://doi.org/10.1103/PhysRevB.88.075420	journal	August 2013
Monolayers of W _x Mo _1−x S ₂ alloy heterostructure with in-plane composition variations Zheng, Shoujun; Sun, Linfeng; Yin, Tingting Applied Physics Letters, Vol. 106, Issue 6 https://doi.org/10.1063/1.4908256	journal	February 2015
Electroluminescence and photocurrent generation from atomically sharp WSe2/MoS2 heterojunction p-n diodes Cheng, Rui; Li, Dehui; Zhou, Hailong arXiv https://doi.org/10.48550/arxiv.1403.3447	text	January 2014

Cited By (16)

Tuning the Electronic and Photonic Properties of Monolayer MoS ₂ via In Situ Rhenium Substitutional Doping Zhang, Kehao; Bersch, Brian M.; Joshi, Jaydeep Advanced Functional Materials, Vol. 28, Issue 16 https://doi.org/10.1002/adfm.201706950	journal	February 2018
Atomic Defects in Two-Dimensional Materials: From Single-Atom Spectroscopy to Functionalities in Opto-/Electronics, Nanomagnetism, and Catalysis Hong, Jinhua; Jin, Chuanhong; Yuan, Jun Advanced Materials, Vol. 29, Issue 14 https://doi.org/10.1002/adma.201606434	journal	March 2017
Synthesis of Large‐Size 1T′ ReS ₂ _x Se ₂₍₁₋ _x ₎ Alloy Monolayer with Tunable Bandgap and Carrier Type Cui, Fangfang; Feng, Qingliang; Hong, Jinhua Advanced Materials, Vol. 29, Issue 46 https://doi.org/10.1002/adma.201705015	journal	October 2017
Controlled Growth and Thickness‐Dependent Conduction‐Type Transition of 2D Ferrimagnetic Cr ₂ S ₃ Semiconductors Cui, Fangfang; Zhao, Xiaoxu; Xu, Junjie Advanced Materials, Vol. 32, Issue 4 https://doi.org/10.1002/adma.201905896	journal	December 2019
Recent advances in low‐dimensional semiconductor nanomaterials and their applications in high‐performance photodetectors Fang, Jingzhi; Zhou, Ziqi; Xiao, Mengqi InfoMat, Vol. 2, Issue 2 https://doi.org/10.1002/inf2.12067	journal	December 2019
Various Structures of 2D Transition-Metal Dichalcogenides and Their Applications Wei, Zhongming; Li, Bo; Xia, Congxin Small Methods, Vol. 2, Issue 11 https://doi.org/10.1002/smtd.201800094	journal	July 2018
In situ edge engineering in two-dimensional transition metal dichalcogenides Sang, Xiahan; Li, Xufan; Zhao, Wen Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04435-x	journal	May 2018
Tuning electrochemical catalytic activity of defective 2D terrace MoSe ₂ heterogeneous catalyst via cobalt doping Chen, Xiaoshuang; Qiu, Yunfeng; Liu, Guangbo Journal of Materials Chemistry A, Vol. 5, Issue 22 https://doi.org/10.1039/c7ta02327h	journal	January 2017
XPS experimental and DFT investigations on solid solutions of Mo _1−x Re _x S ₂ (0 < x < 0.20) Dalmatova, Svetlana A.; Fedorenko, Anastasiya D.; Mazalov, Lev N. Nanoscale, Vol. 10, Issue 21 https://doi.org/10.1039/c8nr01661e	journal	January 2018
Hydrogen-assisted post-growth substitution of tellurium into molybdenum disulfide monolayers with tunable compositions Yin, Guoli; Zhu, Dancheng; Lv, Danhui Nanotechnology, Vol. 29, Issue 14 https://doi.org/10.1088/1361-6528/aaabe8	journal	February 2018
2D materials advances: from large scale synthesis and controlled heterostructures to improved characterization techniques, defects and applications Lin, Zhong; McCreary, Amber; Briggs, Natalie 2D Materials, Vol. 3, Issue 4 https://doi.org/10.1088/2053-1583/3/4/042001	journal	December 2016
Influence of defects and doping on phonon transport properties of monolayer MoSe ₂ Yan, Zhequan; Yoon, Mina; Kumar, Satish 2D Materials, Vol. 5, Issue 3 https://doi.org/10.1088/2053-1583/aabd54	journal	April 2018
A roadmap for electronic grade 2D materials Briggs, Natalie; Subramanian, Shruti; Lin, Zhong 2D Materials, Vol. 6, Issue 2 https://doi.org/10.1088/2053-1583/aaf836	journal	January 2019
Giant enhancement of solid solubility in monolayer alloys by selective orbital coupling Du, Shiqiao; Wang, Jianfeng; Kang, Lei Physical Review B, Vol. 101, Issue 5 https://doi.org/10.1103/physrevb.101.054201	journal	February 2020
Doping of Two-Dimensional Semiconductors: A Rapid Review and Outlook Zhang, Kehao; Robinson, Joshua MRS Advances, Vol. 4, Issue 51-52 https://doi.org/10.1557/adv.2019.391	journal	January 2019
Giant Enhancement of Solid Solubility in Monolayer BNC Alloys by Selective Orbital Coupling Du, Shiqiao; Wang, Jianfeng; Kang, Lei arXiv https://doi.org/10.48550/arxiv.1907.12847	text	January 2019

Similar Records

Suppression of Defects and Deep Levels Using Isoelectronic Tungsten Substitution in Monolayer MoSe₂

Journal Article · Thu May 18 00:00:00 EDT 2017 · Advanced Functional Materials (Online) · OSTI ID:1329120

Li, Xufan; Puretzky, Alexander A.; Sang, Xiahan; +12 more

Persistent photoconductivity in two-dimensional Mo_1-xW _xSe₂–MoSe₂ van der Waals heterojunctions

Journal Article · Tue Feb 16 00:00:00 EST 2016 · Journal of Materials Research · OSTI ID:1329120

Puretzky, Alexander A.; Basile, Leonardo; Idrobo, Juan Carlos; +6 more

The role of Anderson’s rule in determining electronic, optical and transport properties of transition metal dichalcogenide heterostructures

Journal Article · Fri Dec 28 00:00:00 EST 2018 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:1329120

Xu, Ke; Xu, Yuanfeng; Zhang, Hao; +8 more

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY

Title: Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation

Citation Formats

References (42)

Cited By (16)

Similar Records

Related Subjects

Title: Isoelectronic tungsten doping in monolayer MoSe₂ for carrier type modulation