Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides
Abstract
To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS2), here we report studies of the reactions of molybdenum hexafluoride (MoF6) and hydrogen sulfide (H2S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 °C revealed temperature-dependent nucleation behavior of the MoF6 precursor, which is attributed to variations in surface hydroxyl concentration with temperature. In situ Fourier transform infrared spectroscopy coupled with ex situ x-ray photoelectron spectroscopy (XPS) indicated the presence of molybdenum oxide and molybdenum oxyfluoride species during nucleation. Density functional theory calculations additionally support the formation of these species as well as predicted metal oxide to fluoride conversion. Residual gas analysis revealed reaction by-products, and the combined experimental and computational results provided insights into proposed nucleation surface reactions. With additional ALD cycles, Fourier transform infrared spectroscopy indicated steady film growth after ∼13 cycles at 200 °C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 °C and below, while layered films with vertical platelets were observed at 250 °C. These resultsmore »
- Publication Date:
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1899376
- Grant/Contract Number:
- AC02-06CH11357; SC0014664; No. DE-AC07-05ID14517; DOI: 10.18122/B2S41H
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Journal of Vacuum Science and Technology A
- Additional Journal Information:
- Journal Name: Journal of Vacuum Science and Technology A Journal Volume: 40 Journal Issue: 6; Journal ID: ISSN 0734-2101
- Publisher:
- American Vacuum Society
- Country of Publication:
- United States
- Language:
- English
Citation Formats
Soares, Jake, Letourneau, Steven, Lawson, Matthew, Mane, Anil U., Lu, Yu, Wu, Yaqiao, Hues, Steven M., Li, Lan, Elam, Jeffrey W., and Graugnard, Elton. Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides. United States: N. p., 2022.
Web. doi:10.1116/6.0002024.
Soares, Jake, Letourneau, Steven, Lawson, Matthew, Mane, Anil U., Lu, Yu, Wu, Yaqiao, Hues, Steven M., Li, Lan, Elam, Jeffrey W., & Graugnard, Elton. Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides. United States. https://doi.org/10.1116/6.0002024
Soares, Jake, Letourneau, Steven, Lawson, Matthew, Mane, Anil U., Lu, Yu, Wu, Yaqiao, Hues, Steven M., Li, Lan, Elam, Jeffrey W., and Graugnard, Elton. Mon .
"Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides". United States. https://doi.org/10.1116/6.0002024.
@article{osti_1899376,
title = {Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides},
author = {Soares, Jake and Letourneau, Steven and Lawson, Matthew and Mane, Anil U. and Lu, Yu and Wu, Yaqiao and Hues, Steven M. and Li, Lan and Elam, Jeffrey W. and Graugnard, Elton},
abstractNote = {To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS2), here we report studies of the reactions of molybdenum hexafluoride (MoF6) and hydrogen sulfide (H2S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 °C revealed temperature-dependent nucleation behavior of the MoF6 precursor, which is attributed to variations in surface hydroxyl concentration with temperature. In situ Fourier transform infrared spectroscopy coupled with ex situ x-ray photoelectron spectroscopy (XPS) indicated the presence of molybdenum oxide and molybdenum oxyfluoride species during nucleation. Density functional theory calculations additionally support the formation of these species as well as predicted metal oxide to fluoride conversion. Residual gas analysis revealed reaction by-products, and the combined experimental and computational results provided insights into proposed nucleation surface reactions. With additional ALD cycles, Fourier transform infrared spectroscopy indicated steady film growth after ∼13 cycles at 200 °C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 °C and below, while layered films with vertical platelets were observed at 250 °C. These results provide an improved understanding of MoS2 nucleation, which can guide surface preparation for the deposition of few-layer films and advance MoS2 toward integration into device manufacturing.},
doi = {10.1116/6.0002024},
journal = {Journal of Vacuum Science and Technology A},
number = 6,
volume = 40,
place = {United States},
year = {Mon Nov 21 00:00:00 EST 2022},
month = {Mon Nov 21 00:00:00 EST 2022}
}
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