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Transient ultrafast and negative diffusion of charge carriers in suspended MoSe2 from multilayer to monolayer

Author

Listed:
  • Giulia Lo Gerfo Morganti

    (The Barcelona Institute of Science and Technology, Castelldefels)

  • Roberto Rosati

    (Philipps-Universität Marburg)

  • Guillermo D. Brinatti Vazquez

    (The Barcelona Institute of Science and Technology, Castelldefels)

  • Sebin Varghese

    (Catalan Institute of Nanoscience and Nanotechnology - ICN2 (BIST and CSIC)
    Department of Applied Physics)

  • David Saleta Reig

    (Catalan Institute of Nanoscience and Nanotechnology - ICN2 (BIST and CSIC))

  • Ermin Malic

    (Philipps-Universität Marburg)

  • Niek F. Hulst

    (The Barcelona Institute of Science and Technology, Castelldefels
    ICREA - Institució Catalana de Recerca i Estudis Avançats)

  • Klaas-Jan Tielrooij

    (Catalan Institute of Nanoscience and Nanotechnology - ICN2 (BIST and CSIC)
    Department of Applied Physics)

Abstract

Understanding the ultrafast transport properties of charge carriers in transition metal dichalcogenides is essential for advancing technologies based on these materials. Here, we study MoSe2 crystals with thicknesses down to the monolayer, combining ultrafast spatiotemporal microscopy and quantitative microscopic modelling. Crucially, we obtain the intrinsic ultrafast transport dynamics by studying suspended crystals that do not suffer from detrimental substrate effects. In mono- and bilayer crystals, we identify four sequential transport regimes. The first two regimes involve high-energy non-thermalized and quasi-thermalized carriers that propagate rapidly with diffusivities up to 1000 cm2/s. After ~1.5 ps, a remarkable third regime occurs with apparent negative diffusion, finally followed by exciton propagation limited by trapping into defect states. Interestingly, for trilayer and thicker crystals, only the first and last regimes occur. This work underscores the role of traps and dielectric environment in electron transport, offering valuable insights for the development of (flexible) (opto)electronic applications.

Suggested Citation

  • Giulia Lo Gerfo Morganti & Roberto Rosati & Guillermo D. Brinatti Vazquez & Sebin Varghese & David Saleta Reig & Ermin Malic & Niek F. Hulst & Klaas-Jan Tielrooij, 2025. "Transient ultrafast and negative diffusion of charge carriers in suspended MoSe2 from multilayer to monolayer," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60197-3
    DOI: 10.1038/s41467-025-60197-3
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    References listed on IDEAS

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    1. Chiara Trovatello & Florian Katsch & Nicholas J. Borys & Malte Selig & Kaiyuan Yao & Rocio Borrego-Varillas & Francesco Scotognella & Ilka Kriegel & Aiming Yan & Alex Zettl & P. James Schuck & Andreas, 2020. "The ultrafast onset of exciton formation in 2D semiconductors," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Ermin Malic & Raül Perea-Causin & Roberto Rosati & Daniel Erkensten & Samuel Brem, 2023. "Exciton transport in atomically thin semiconductors," Nature Communications, Nature, vol. 14(1), pages 1-4, December.
    3. Soonyoung Cha & Ji Ho Sung & Sangwan Sim & Jun Park & Hoseok Heo & Moon-Ho Jo & Hyunyong Choi, 2016. "1s-intraexcitonic dynamics in monolayer MoS2 probed by ultrafast mid-infrared spectroscopy," Nature Communications, Nature, vol. 7(1), pages 1-7, April.
    4. Dhinesh Babu Velusamy & Richard Hahnkee Kim & Soonyoung Cha & June Huh & Reza Khazaeinezhad & Sahar Hosseinzadeh Kassani & Giyoung Song & Suk Man Cho & Sung Hwan Cho & Ihn Hwang & Jinseong Lee & Kyung, 2015. "Flexible transition metal dichalcogenide nanosheets for band-selective photodetection," Nature Communications, Nature, vol. 6(1), pages 1-11, November.
    5. Roberto Rosati & Robert Schmidt & Samuel Brem & Raül Perea-Causín & Iris Niehues & Johannes Kern & Johann A. Preuß & Robert Schneider & Steffen Michaelis de Vasconcellos & Rudolf Bratschitsch & Ermin , 2021. "Dark exciton anti-funneling in atomically thin semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
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