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Charge carrier dynamics in colloidally synthesized monolayer MoX2 nanosheets

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Abstract
Transition metal dichalcogenides (TMDs) are nanostructured semiconductors with prospects in optoelectronics and photocatalysis. Several bottom-up procedures to synthesize such materials have been developed yielding colloidal transition metal dichalcogenides (c-TMDs). Where such methods initially yielded multilayered sheets with indirect band gaps, recently, also the formation of monolayered c-TMDs became possible. Despite these advances, no clear picture on the charge carrier dynamics in monolayer c-TMDs exists to date. Here, we show through broadband and multiresonant pump-probe spectroscopy, that the carrier dynamics in monolayer c-TMDs are dominated by a fast electron trapping mechanism, universal to both MoS2 and MoSe2, contrasting hole-dominated trapping in their multilayered counterparts. Through a detailed hyperspectral fitting procedure, sizable exciton red shifts are found and assigned to static shifts originating from both interactions with the trapped electron population and lattice heating. Our results pave the way to optimizing monolayer c-TMDs via passivation of predominantly the electron-trap sites.
Keywords
General Materials Science, Physical and Theoretical Chemistry, PHOTOINDUCED BANDGAP RENORMALIZATION, MOS2, WS2

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Citation

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MLA
Mutyala, Chandra Sekhar, et al. “Charge Carrier Dynamics in Colloidally Synthesized Monolayer MoX2 Nanosheets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 14, no. 10, 2023, pp. 2620–26, doi:10.1021/acs.jpclett.3c00278.
APA
Mutyala, C. S., Pippia, G., Tanghe, I., Martín-García, B., Rousaki, A., Vandenabeele, P., … Geiregat, P. (2023). Charge carrier dynamics in colloidally synthesized monolayer MoX2 nanosheets. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 14(10), 2620–2626. https://doi.org/10.1021/acs.jpclett.3c00278
Chicago author-date
Mutyala, Chandra Sekhar, Gabriele Pippia, Ivo Tanghe, Beatriz Martín-García, Anastasia Rousaki, Peter Vandenabeele, Pieter Schiettecatte, Iwan Moreels, and Pieter Geiregat. 2023. “Charge Carrier Dynamics in Colloidally Synthesized Monolayer MoX2 Nanosheets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 14 (10): 2620–26. https://doi.org/10.1021/acs.jpclett.3c00278.
Chicago author-date (all authors)
Mutyala, Chandra Sekhar, Gabriele Pippia, Ivo Tanghe, Beatriz Martín-García, Anastasia Rousaki, Peter Vandenabeele, Pieter Schiettecatte, Iwan Moreels, and Pieter Geiregat. 2023. “Charge Carrier Dynamics in Colloidally Synthesized Monolayer MoX2 Nanosheets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 14 (10): 2620–2626. doi:10.1021/acs.jpclett.3c00278.
Vancouver
1.
Mutyala CS, Pippia G, Tanghe I, Martín-García B, Rousaki A, Vandenabeele P, et al. Charge carrier dynamics in colloidally synthesized monolayer MoX2 nanosheets. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 2023;14(10):2620–6.
IEEE
[1]
C. S. Mutyala et al., “Charge carrier dynamics in colloidally synthesized monolayer MoX2 nanosheets,” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 14, no. 10, pp. 2620–2626, 2023.
@article{01GVQAWERGHJWSHNEQJ8JN1MVS,
  abstract     = {{Transition metal dichalcogenides (TMDs) are nanostructured semiconductors with prospects in optoelectronics and photocatalysis. Several bottom-up procedures to synthesize such materials have been developed yielding colloidal transition metal dichalcogenides (c-TMDs). Where such methods initially yielded multilayered sheets with indirect band gaps, recently, also the formation of monolayered c-TMDs became possible. Despite these advances, no clear picture on the charge carrier dynamics in monolayer c-TMDs exists to date. Here, we show through broadband and multiresonant pump-probe spectroscopy, that the carrier dynamics in monolayer c-TMDs are dominated by a fast electron trapping mechanism, universal to both MoS2 and MoSe2, contrasting hole-dominated trapping in their multilayered counterparts. Through a detailed hyperspectral fitting procedure, sizable exciton red shifts are found and assigned to static shifts originating from both interactions with the trapped electron population and lattice heating. Our results pave the way to optimizing monolayer c-TMDs via passivation of predominantly the electron-trap sites.}},
  author       = {{Mutyala, Chandra Sekhar and Pippia, Gabriele and Tanghe, Ivo and Martín-García, Beatriz and Rousaki, Anastasia and Vandenabeele, Peter and Schiettecatte, Pieter and Moreels, Iwan and Geiregat, Pieter}},
  issn         = {{1948-7185}},
  journal      = {{JOURNAL OF PHYSICAL CHEMISTRY LETTERS}},
  keywords     = {{General Materials Science,Physical and Theoretical Chemistry,PHOTOINDUCED BANDGAP RENORMALIZATION,MOS2,WS2}},
  language     = {{eng}},
  number       = {{10}},
  pages        = {{2620--2626}},
  title        = {{Charge carrier dynamics in colloidally synthesized monolayer MoX2 nanosheets}},
  url          = {{http://doi.org/10.1021/acs.jpclett.3c00278}},
  volume       = {{14}},
  year         = {{2023}},
}

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