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Time-domain observation of interlayer exciton formation and thermalization in a MoSe2/WSe2 heterostructure

Author

Listed:
  • Veronica R. Policht

    (Politecnico di Milano
    NRC Postdoc residing at U.S. Naval Research Laboratory)

  • Henry Mittenzwey

    (Technische Universität Berlin)

  • Oleg Dogadov

    (Politecnico di Milano)

  • Manuel Katzer

    (Technische Universität Berlin)

  • Andrea Villa

    (Politecnico di Milano)

  • Qiuyang Li

    (Columbia University)

  • Benjamin Kaiser

    (Zuse-Institut Berlin)

  • Aaron M. Ross

    (Politecnico di Milano)

  • Francesco Scotognella

    (Politecnico di Milano
    Department of Applied Science and Technology, Politecnico di Torino)

  • Xiaoyang Zhu

    (Columbia University)

  • Andreas Knorr

    (Technische Universität Berlin)

  • Malte Selig

    (Technische Universität Berlin)

  • Giulio Cerullo

    (Politecnico di Milano
    CNR-IFN)

  • Stefano Dal Conte

    (Politecnico di Milano)

Abstract

Vertical heterostructures of transition metal dichalcogenides (TMDs) host interlayer excitons with electrons and holes residing in different layers. With respect to their intralayer counterparts, interlayer excitons feature longer lifetimes and diffusion lengths, paving the way for room temperature excitonic optoelectronic devices. The interlayer exciton formation process and its underlying physical mechanisms are largely unexplored. Here we use ultrafast transient absorption spectroscopy with a broadband white-light probe to simultaneously resolve interlayer charge transfer and interlayer exciton formation dynamics in a MoSe2/WSe2 heterostructure. We observe an interlayer exciton formation timescale nearly an order of magnitude (~1 ps) longer than the interlayer charge transfer time (~100 fs). Microscopic calculations attribute this relative delay to an interplay of a phonon-assisted interlayer exciton cascade and thermalization, and excitonic wave-function overlap. Our results may explain the efficient photocurrent generation observed in optoelectronic devices based on TMD heterostructures, as the interlayer excitons are able to dissociate during thermalization.

Suggested Citation

  • Veronica R. Policht & Henry Mittenzwey & Oleg Dogadov & Manuel Katzer & Andrea Villa & Qiuyang Li & Benjamin Kaiser & Aaron M. Ross & Francesco Scotognella & Xiaoyang Zhu & Andreas Knorr & Malte Selig, 2023. "Time-domain observation of interlayer exciton formation and thermalization in a MoSe2/WSe2 heterostructure," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42915-x
    DOI: 10.1038/s41467-023-42915-x
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    as
    1. Pasqual Rivera & John R. Schaibley & Aaron M. Jones & Jason S. Ross & Sanfeng Wu & Grant Aivazian & Philip Klement & Kyle Seyler & Genevieve Clark & Nirmal J. Ghimire & Jiaqiang Yan & D. G. Mandrus & , 2015. "Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures," Nature Communications, Nature, vol. 6(1), pages 1-6, May.
    2. Kyle L. Seyler & Pasqual Rivera & Hongyi Yu & Nathan P. Wilson & Essance L. Ray & David G. Mandrus & Jiaqiang Yan & Wang Yao & Xiaodong Xu, 2019. "Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers," Nature, Nature, vol. 567(7746), pages 66-70, March.
    3. Evgeny M. Alexeev & David A. Ruiz-Tijerina & Mark Danovich & Matthew J. Hamer & Daniel J. Terry & Pramoda K. Nayak & Seongjoon Ahn & Sangyeon Pak & Juwon Lee & Jung Inn Sohn & Maciej R. Molas & Maciej, 2019. "Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures," Nature, Nature, vol. 567(7746), pages 81-86, March.
    4. Chenhao Jin & Emma C. Regan & Aiming Yan & M. Iqbal Bakti Utama & Danqing Wang & Sihan Zhao & Ying Qin & Sijie Yang & Zhiren Zheng & Shenyang Shi & Kenji Watanabe & Takashi Taniguchi & Sefaattin Tonga, 2019. "Observation of moiré excitons in WSe2/WS2 heterostructure superlattices," Nature, Nature, vol. 567(7746), pages 76-80, March.
    5. A. K. Geim & I. V. Grigorieva, 2013. "Van der Waals heterostructures," Nature, Nature, vol. 499(7459), pages 419-425, July.
    6. David Schmitt & Jan Philipp Bange & Wiebke Bennecke & AbdulAziz AlMutairi & Giuseppe Meneghini & Kenji Watanabe & Takashi Taniguchi & Daniel Steil & D. Russell Luke & R. Thomas Weitz & Sabine Steil & , 2022. "Formation of moiré interlayer excitons in space and time," Nature, Nature, vol. 608(7923), pages 499-503, August.
    7. Philipp Nagler & Mariana V. Ballottin & Anatolie A. Mitioglu & Fabian Mooshammer & Nicola Paradiso & Christoph Strunk & Rupert Huber & Alexey Chernikov & Peter C. M. Christianen & Christian Schüller &, 2017. "Giant magnetic splitting inducing near-unity valley polarization in van der Waals heterostructures," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    8. Kha Tran & Galan Moody & Fengcheng Wu & Xiaobo Lu & Junho Choi & Kyounghwan Kim & Amritesh Rai & Daniel A. Sanchez & Jiamin Quan & Akshay Singh & Jacob Embley & André Zepeda & Marshall Campbell & Trav, 2019. "Evidence for moiré excitons in van der Waals heterostructures," Nature, Nature, vol. 567(7746), pages 71-75, March.
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