Structural Studies of Alloyed and Nanoparticle Transition Metal Dichalcogenides by Selenium-77 Solid-State Nuclear Magnetic Resonance Spectroscopy

dc.contributor.author Carnahan, Scott L.
dc.contributor.author Gi, Eunbyeol
dc.contributor.author Wagner, Molly
dc.contributor.author Santhiran, Anuluxan
dc.contributor.author Amerongen, Elise
dc.contributor.author Yin, Hang
dc.contributor.author Geisenhoff, Jessica Q.
dc.contributor.author Rahman, Sharifur
dc.contributor.author Dolotko, Oleksander
dc.contributor.author Hlova, Ihor Z.
dc.contributor.author Balema, Viktor P.
dc.contributor.author Smith, Emily
dc.contributor.author Schimpf, Alina M.
dc.contributor.author Vela, Javier
dc.contributor.author Rossini, Aaron
dc.contributor.department Ames National Laboratory
dc.contributor.department Department of Chemistry
dc.date.accessioned 2024-04-22T14:54:41Z
dc.date.available 2024-04-22T14:54:41Z
dc.date.issued 2024-04-15
dc.description.abstract Layered transition metal dichalcogenides (TMDCs) such as MoS2, MoSe2 and WSe2 are under intense investigation because they are atomically thin semiconductors with photophysical properties can be tuned by changing their composition or morphology. Mechanochemical processing has been proposed as a method to obtain alloyed TMDCs in the series Mo1-xWxSySe2-y (x = 0, 1; y = 0, 1, 2). However, elucidating the chemical transformations occurring at the atomic scale following mechanochemical processing is challenging because the products are usually fine powders. To address this challenge, we probe TMDC mixing and alloying by using a combination of powder X-ray diffraction (PXRD), optical spectroscopy, 77Se solid-state nuclear magnetic resonance (SSNMR) spectroscopy and planewave density functional theory (DFT) calculations. The nature of the milling material and reaction atmosphere are shown to be essential factors in limiting the formation of undesired oxide byproducts. We demonstrate acquisition of 77Se SSNMR spectra using different combinations of Carr-Purcell Meiboom-Gill acquisition (CPMG) pulse sequences, magic angle spinning (MAS), and MAS dynamic nuclear polarization (DNP). The combination of SSNMR with the other characterization methods demonstrates that ball milling induces molecular level alloying of Mo, W and chalcogen atoms in the family Mo1-xWxSySe2-y. GIPAW DFT calculations yield accurate values of 77Se chemical shift tensor components. 77Se SSNMR spectroscopy was also applied to study the structure of WSe2 nanocrystals intercalated with ethylenediamine. The WSe2 nanocrystals exhibited a more positive isotropic 77Se chemical shift as compared to bulk WSe2, however, the 77Se chemical shift anisotropy was the same, confirming the WSe2 layers have a similar structure as in their bulk counterparts.
dc.description.comments This is a preprint from Carnahan, Scott, Eunbyeol Gi, Molly Wagner, Anuluxan Santhiran, Elise Amerongen, Hang Yin, Jessica Geisenhoff et al. "Structural Studies of Alloyed and Nanoparticle Transition Metal Dichalcogenides by Selenium-77 Solid-State Nuclear Magnetic Resonance Spectroscopy." (2024). doi: https://doi.org/10.26434/chemrxiv-2024-rgsrh-v2. </p><br>Published as Carnahan, Scott L., Eunbyeol Gi, Molly Wagner, Anuluxan Santhiran, Elise Amerongen, Hang Yin, Jessica Q. Geisenhoff et al. "Structural Studies of Alloyed and Nanoparticle Transition Metal Dichalcogenides by Selenium-77 Solid-State Nuclear Magnetic Resonance Spectroscopy." Chemistry of Materials 36, no. 22 (2024): 11264-11279. doi: https://doi.org/10.1021/acs.chemmater.4c02352.
dc.identifier.uri https://dr.lib.iastate.edu/handle/20.500.12876/RwyqJ9Jw
dc.language.iso en
dc.rights This preprint is licensed (https://creativecommons.org/licenses/by-nc-nd/4.0/).
dc.source.uri https://doi.org/10.26434/chemrxiv-2024-rgsrh *
dc.subject.disciplines DegreeDisciplines::Physical Sciences and Mathematics::Chemistry::Physical Chemistry
dc.title Structural Studies of Alloyed and Nanoparticle Transition Metal Dichalcogenides by Selenium-77 Solid-State Nuclear Magnetic Resonance Spectroscopy
dc.type preprint
dc.type.genre preprint
dspace.entity.type Publication
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