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  Microscopic Understanding of Ultrafast Charge Transfer in van der Waals Heterostructures

Krause, R., Aeschlimann, S., Chavez Cervantes, M., Perea-Causin, R., Brem, S., Malic, E., et al. (2021). Microscopic Understanding of Ultrafast Charge Transfer in van der Waals Heterostructures. Physical Review Letters, 127(27): 276401. doi:10.1103/PhysRevLett.127.276401.

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Item Permalink: https://hdl.handle.net/21.11116/0000-0009-9EB8-6 Version Permalink: https://hdl.handle.net/21.11116/0000-000B-F1CA-1
Genre: Journal Article

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Supplemental Material: sample growth and characterization tr-ARPES setup and data analysis detailed comparison with literature description of microscopic model
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 Creators:
Krause, R.1, 2, Author           
Aeschlimann, S.1, 2, Author           
Chavez Cervantes, M.2, Author           
Perea-Causin, R.3, Author
Brem, S.4, Author
Malic, E.3, Author
Forti, S.5, Author
Fabbri, F.5, 6, 7, Author
Coletti, C.5, 7, Author
Gierz, I.1, Author
Affiliations:
1University of Regensburg, Institute for Experimental and Applied Physics, ou_persistent22              
2Ultrafast Electron Dynamics, Condensed Matter Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938295              
3Department of Physics, Chalmers University of Technology, ou_persistent22              
4Department of Physics, Philipps-Universität Marburg, ou_persistent22              
5Center for Nanotechnology Innovation at NEST, Istituto Italiano di Tecnologia, ou_persistent22              
6NEST, Istituto Nanoscienze, CNR and Scuola Normale Superiore, ou_persistent22              
7Graphene Labs, Istituto Italiano di Tecnologia, ou_persistent22              

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 Abstract: Van der Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS2/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS2 and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacancies. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices.

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Language(s): eng - English
 Dates: 2021-09-292021-05-032021-11-122021-12-272021-12
 Publication Status: Issued
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2012.09268
DOI: 10.1103/PhysRevLett.127.276401
 Degree: -

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Project name : -
Grant ID : 785219
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : -
Grant ID : 881603
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : We thank S. Latini, L. Xian, A. Rubio, and S. Refaely-Abramson for many fruitful discussions. This work was supported by the Deutsche Forschungsgemeinschaft through SFB 925, SFB 1083 and SFB 1277, by the European Unions Horizon 2020 research and innovation program under Grant Agreements No. 785219 and No. 881603, and by the Swedish Research Council (VR, Project No. 2018-00734). The computations were enabled by resources provided by the Swedish National Infrastructure for Computing (SNIC) at C3SE partially funded by the Swedish Research Council through Grant Agreement No. 2016-07213. R. P. C. acknowledges funding from the Excellence Initiative Nano (Chalmers) under the Excellence Ph.D. programme.
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Source 1

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Title: Physical Review Letters
  Abbreviation : Phys. Rev. Lett.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Physical Society
Pages: - Volume / Issue: 127 (27) Sequence Number: 276401 Start / End Page: - Identifier: ISSN: 0031-9007
CoNE: https://pure.mpg.de/cone/journals/resource/954925433406_1