IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-42915-x.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-42915-x
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-42915-x?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. A. K. Geim & I. V. Grigorieva, 2013. "Van der Waals heterostructures," Nature, Nature, vol. 499(7459), pages 419-425, July.
    2. 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.
    3. 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.
    4. 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.
    5. 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.
    6. 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.
    7. 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.
    8. 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.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Jinjae Kim & Jiwon Park & Hyojin Choi & Taeho Kim & Soonyoung Cha & Yewon Lee & Kenji Watanabe & Takashi Taniguchi & Jonghwan Kim & Moon-Ho Jo & Hyunyong Choi, 2024. "Correlation-driven nonequilibrium exciton site transition in a WSe2/WS2 moiré supercell," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Hongbing Cai & Abdullah Rasmita & Qinghai Tan & Jia-Min Lai & Ruihua He & Xiangbin Cai & Yan Zhao & Disheng Chen & Naizhou Wang & Zhao Mu & Zumeng Huang & Zhaowei Zhang & John J. H. Eng & Yuanda Liu &, 2023. "Interlayer donor-acceptor pair excitons in MoSe2/WSe2 moiré heterobilayer," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    2. Qiaoling Lin & Hanlin Fang & Alexei Kalaboukhov & Yuanda Liu & Yi Zhang & Moritz Fischer & Juntao Li & Joakim Hagel & Samuel Brem & Ermin Malic & Nicolas Stenger & Zhipei Sun & Martijn Wubs & Sanshui , 2024. "Moiré-engineered light-matter interactions in MoS2/WSe2 heterobilayers at room temperature," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Suman Chatterjee & Medha Dandu & Pushkar Dasika & Rabindra Biswas & Sarthak Das & Kenji Watanabe & Takashi Taniguchi & Varun Raghunathan & Kausik Majumdar, 2023. "Harmonic to anharmonic tuning of moiré potential leading to unconventional Stark effect and giant dipolar repulsion in WS2/WSe2 heterobilayer," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    4. Ruoming Peng & Adina Ripin & Yusen Ye & Jiayi Zhu & Changming Wu & Seokhyeong Lee & Huan Li & Takashi Taniguchi & Kenji Watanabe & Ting Cao & Xiaodong Xu & Mo Li, 2022. "Long-range transport of 2D excitons with acoustic waves," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    5. Zhen Lian & Dongxue Chen & Yuze Meng & Xiaotong Chen & Ying Su & Rounak Banerjee & Takashi Taniguchi & Kenji Watanabe & Sefaattin Tongay & Chuanwei Zhang & Yong-Tao Cui & Su-Fei Shi, 2023. "Exciton Superposition across Moiré States in a Semiconducting Moiré Superlattice," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    6. Hanlin Fang & Qiaoling Lin & Yi Zhang & Joshua Thompson & Sanshui Xiao & Zhipei Sun & Ermin Malic & Saroj P. Dash & Witlef Wieczorek, 2023. "Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    7. Fateme Mahdikhanysarvejahany & Daniel N. Shanks & Matthew Klein & Qian Wang & Michael R. Koehler & David G. Mandrus & Takashi Taniguchi & Kenji Watanabe & Oliver L. A. Monti & Brian J. LeRoy & John R., 2022. "Localized interlayer excitons in MoSe2–WSe2 heterostructures without a moiré potential," Nature Communications, Nature, vol. 13(1), pages 1-6, December.
    8. Zhen Lian & Dongxue Chen & Lei Ma & Yuze Meng & Ying Su & Li Yan & Xiong Huang & Qiran Wu & Xinyue Chen & Mark Blei & Takashi Taniguchi & Kenji Watanabe & Sefaattin Tongay & Chuanwei Zhang & Yong-Tao , 2023. "Quadrupolar excitons and hybridized interlayer Mott insulator in a trilayer moiré superlattice," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    9. Riya Sebait & Roberto Rosati & Seok Joon Yun & Krishna P. Dhakal & Samuel Brem & Chandan Biswas & Alexander Puretzky & Ermin Malic & Young Hee Lee, 2023. "Sequential order dependent dark-exciton modulation in bi-layered TMD heterostructure," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    10. Mengqi Huang & Zeliang Sun & Gerald Yan & Hongchao Xie & Nishkarsh Agarwal & Gaihua Ye & Suk Hyun Sung & Hanyi Lu & Jingcheng Zhou & Shaohua Yan & Shangjie Tian & Hechang Lei & Robert Hovden & Rui He , 2023. "Revealing intrinsic domains and fluctuations of moiré magnetism by a wide-field quantum microscope," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    11. Jinjae Kim & Jiwon Park & Hyojin Choi & Taeho Kim & Soonyoung Cha & Yewon Lee & Kenji Watanabe & Takashi Taniguchi & Jonghwan Kim & Moon-Ho Jo & Hyunyong Choi, 2024. "Correlation-driven nonequilibrium exciton site transition in a WSe2/WS2 moiré supercell," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    12. Elena Blundo & Federico Tuzi & Salvatore Cianci & Marzia Cuccu & Katarzyna Olkowska-Pucko & Łucja Kipczak & Giorgio Contestabile & Antonio Miriametro & Marco Felici & Giorgio Pettinari & Takashi Tanig, 2024. "Localisation-to-delocalisation transition of moiré excitons in WSe2/MoSe2 heterostructures," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    13. Hulin Yao & Pengcheng Zheng & Shibin Zhang & Chuanjie Hu & Xiaoli Fang & Liping Zhang & Dan Ling & Huanyang Chen & Xin Ou, 2024. "Twist piezoelectricity: giant electromechanical coupling in magic-angle twisted bilayer LiNbO3," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    14. N. Fang & Y. R. Chang & S. Fujii & D. Yamashita & M. Maruyama & Y. Gao & C. F. Fong & D. Kozawa & K. Otsuka & K. Nagashio & S. Okada & Y. K. Kato, 2024. "Room-temperature quantum emission from interface excitons in mixed-dimensional heterostructures," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    15. Valerio Di Giulio & P. A. D. Gonçalves & F. Javier García de Abajo, 2022. "An image interaction approach to quantum-phase engineering of two-dimensional materials," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    16. Yufei Sun & Yujia Wang & Enze Wang & Bolun Wang & Hengyi Zhao & Yongpan Zeng & Qinghua Zhang & Yonghuang Wu & Lin Gu & Xiaoyan Li & Kai Liu, 2022. "Determining the interlayer shearing in twisted bilayer MoS2 by nanoindentation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    17. Madeline Winkle & Isaac M. Craig & Stephen Carr & Medha Dandu & Karen C. Bustillo & Jim Ciston & Colin Ophus & Takashi Taniguchi & Kenji Watanabe & Archana Raja & Sinéad M. Griffin & D. Kwabena Bediak, 2023. "Rotational and dilational reconstruction in transition metal dichalcogenide moiré bilayers," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Meng Zhao & Zhongjie Wang & Lu Liu & Chunzheng Wang & Cheng-Yen Liu & Fang Yang & Hua Wu & Chunlei Gao, 2024. "Atomic-scale visualization of the interlayer Rydberg exciton complex in moiré heterostructures," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    19. Andrew Y. Joe & Andrés M. Mier Valdivia & Luis A. Jauregui & Kateryna Pistunova & Dapeng Ding & You Zhou & Giovanni Scuri & Kristiaan De Greve & Andrey Sushko & Bumho Kim & Takashi Taniguchi & Kenji W, 2024. "Controlled interlayer exciton ionization in an electrostatic trap in atomically thin heterostructures," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    20. Jiaxin Zhao & Antonio Fieramosca & Kevin Dini & Ruiqi Bao & Wei Du & Rui Su & Yuan Luo & Weijie Zhao & Daniele Sanvitto & Timothy C. H. Liew & Qihua Xiong, 2023. "Exciton polariton interactions in Van der Waals superlattices at room temperature," Nature Communications, Nature, vol. 14(1), pages 1-8, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42915-x. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.