Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS
Recent advances in the field of two-dimensional (2D) transition metal dichalcogenide (TMD) materials have indicated that atomic layer deposition (ALD) of the metal oxide and subsequent sulfidation could offer a method for the synthesis of large area two-dimensional materials such as MoS 2 with excel...
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| Format: | Article |
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American Chemical Society (ACS)
2018
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| Online Access: | http://hdl.handle.net/1721.1/114819 https://orcid.org/0000-0003-4148-2424 https://orcid.org/0000-0003-1281-2359 https://orcid.org/0000-0001-8975-6434 |
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| author | Bertuch, Adam Provine, J. Sundaram, Ganesh Ferralis, Nicola Grossman, Jeffrey C. Keller, Brent D. |
| author2 | Massachusetts Institute of Technology. Center for Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Center for Materials Science and Engineering Bertuch, Adam Provine, J. Sundaram, Ganesh Ferralis, Nicola Grossman, Jeffrey C. Keller, Brent D. |
| author_sort | Bertuch, Adam |
| collection | MIT |
| description | Recent advances in the field of two-dimensional (2D) transition metal dichalcogenide (TMD) materials have indicated that atomic layer deposition (ALD) of the metal oxide and subsequent sulfidation could offer a method for the synthesis of large area two-dimensional materials such as MoS 2 with excellent layer control over the entire substrate. However, growing large area oxide films by ALD with sub 1 nm nucleation coalescence remains a significant challenge, and the necessary steps are unexplored. In this work, we demonstrate the necessary process improvements required to achieve sub 1 nm nucleation control by characterization of nucleation domains formed by oxide deposition. Synthesis of the TMD MoS 2 from sulfidation of oxide deposited by both thermal ALD from (tBuN) 2 (NMe 2 ) 2 Mo and O 3 and plasma enhanced ALD (PEALD) from (tBuN) 2 (NMe 2 ) 2 Mo and remote O 2 plasma was performed. Large uniform MoS 2 areas were achieved by optimizing the effects of various growth process conditions and surface treatments on the ALD nucleation and growth of Mo-oxide and the postsulfidation of MoS 2 . In addition to insights into the control of the oxide deposition, film chemistry analysis during a multistep sulfidation based on less toxic sulfur as compared to H 2 S was performed for several temperature profiles revealing sulfur incorporation and molybdenum reduction at low temperatures but higher temperatures required for 2H crystal structure formation. The knowledge gained of the ALD, PEALD, and postsulfidation was leveraged to demonstrate tunable film thickness and centimeter-scale monolayer growth. Material quality can be studied independently of the MoS 2 layer count as demonstrated by the control of the monolayer photoluminescence intensity by the temperature ramp rate during sulfidation. |
| first_indexed | 2024-09-23T16:49:40Z |
| format | Article |
| id | mit-1721.1/114819 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2024-09-23T16:49:40Z |
| publishDate | 2018 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1148192022-09-29T21:47:41Z Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS Bertuch, Adam Provine, J. Sundaram, Ganesh Ferralis, Nicola Grossman, Jeffrey C. Keller, Brent D. Massachusetts Institute of Technology. Center for Materials Science and Engineering Ferralis, Nicola Grossman, Jeffrey C. Keller, Brent D. Recent advances in the field of two-dimensional (2D) transition metal dichalcogenide (TMD) materials have indicated that atomic layer deposition (ALD) of the metal oxide and subsequent sulfidation could offer a method for the synthesis of large area two-dimensional materials such as MoS 2 with excellent layer control over the entire substrate. However, growing large area oxide films by ALD with sub 1 nm nucleation coalescence remains a significant challenge, and the necessary steps are unexplored. In this work, we demonstrate the necessary process improvements required to achieve sub 1 nm nucleation control by characterization of nucleation domains formed by oxide deposition. Synthesis of the TMD MoS 2 from sulfidation of oxide deposited by both thermal ALD from (tBuN) 2 (NMe 2 ) 2 Mo and O 3 and plasma enhanced ALD (PEALD) from (tBuN) 2 (NMe 2 ) 2 Mo and remote O 2 plasma was performed. Large uniform MoS 2 areas were achieved by optimizing the effects of various growth process conditions and surface treatments on the ALD nucleation and growth of Mo-oxide and the postsulfidation of MoS 2 . In addition to insights into the control of the oxide deposition, film chemistry analysis during a multistep sulfidation based on less toxic sulfur as compared to H 2 S was performed for several temperature profiles revealing sulfur incorporation and molybdenum reduction at low temperatures but higher temperatures required for 2H crystal structure formation. The knowledge gained of the ALD, PEALD, and postsulfidation was leveraged to demonstrate tunable film thickness and centimeter-scale monolayer growth. Material quality can be studied independently of the MoS 2 layer count as demonstrated by the control of the monolayer photoluminescence intensity by the temperature ramp rate during sulfidation. 2018-04-20T18:25:02Z 2018-04-20T18:25:02Z 2017-03 2016-09 2018-04-19T14:10:36Z Article http://purl.org/eprint/type/JournalArticle 0897-4756 1520-5002 http://hdl.handle.net/1721.1/114819 Keller, Brent D. et al. “Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS2 Monolayers.” Chemistry of Materials 29, 5 (February 2017): 2024–2032 © 2017 American Chemical Society https://orcid.org/0000-0003-4148-2424 https://orcid.org/0000-0003-1281-2359 https://orcid.org/0000-0001-8975-6434 http://dx.doi.org/10.1021/ACS.CHEMMATER.6B03951 Chemistry of Materials 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. application/pdf American Chemical Society (ACS) MIT Web Domain |
| spellingShingle | Bertuch, Adam Provine, J. Sundaram, Ganesh Ferralis, Nicola Grossman, Jeffrey C. Keller, Brent D. Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title | Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title_full | Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title_fullStr | Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title_full_unstemmed | Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title_short | Process Control of Atomic Layer Deposition Molybdenum Oxide Nucleation and Sulfidation to Large-Area MoS |
| title_sort | process control of atomic layer deposition molybdenum oxide nucleation and sulfidation to large area mos |
| url | http://hdl.handle.net/1721.1/114819 https://orcid.org/0000-0003-4148-2424 https://orcid.org/0000-0003-1281-2359 https://orcid.org/0000-0001-8975-6434 |
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