Mechanism of Electronic Coupling in Hybrid Transition Metal Dichalcogenide-2D Perovskite Heterostructures

Miriam Karpińska^a^,^b, Jakub Jasiński^a^,^c, Minpeng Liang^d, Roman Kempt^e, Jonas Ziegler^f, Kati Finzel^f, Harry Sansom^g, Takashi Taniguchi^h, Kenji Watanabeⁱ, Henry Snaith^g, Machteld Kamminga^d, Nan Zhang^a, Catherine Knodlseder^a, Mateusz Dyksik^a^,^c, Jianting Ye^d, Alessandro Surrente^c, Duncan Maude^a, Michał Baranowski^a^,^c, Łukasz Kłopotowski^b, Alexey Chernikov^f^,^j, Agnieszka Kuc^k, Paulina Plochocka^a

^aLaboratoire National des Champs Magnétiques Intenses, UPR 3228,CNRS-UGA-UPS-INSA, Grenoble and Toulouse, France

^bInstitute of Physics, Polish Academy of Sciences, Warsaw, Poland, aleja Lotników, 32/46, Warszawa, Poland

^cDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, Wroclaw, Poland

^dZernike Institute for Advanced Materials, University of Groningen, The Netherlands, Nijenborgh, 7, Groningen, Netherlands

^eTechnical University (TU) Dresden, DE

^fInstitut für Experimentelle und Angewandte Physik, Universität Regensburg, Universitätsstraße 31, 93053 Regensburg, Germany

^gDepartment of Physics, University of Oxford, Clarendon Laboratory, Oxford, OX1 3PU, UK, Parks Road, Oxford, United Kingdom

^hWPI International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), Tsukuba, Ibaraki 305-0044, Japan

ⁱWPI International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), Tsukuba, Ibaraki 305-0044, Japan

^jResearch Center For Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Japan

^kHelmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstraße 400, 01328 Dresden, Germany

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)

#LowEnOpto22. Low-dimensional Semiconductors for Energy and Optoelectronic Research: a Journey from 0 to 2D

Online, Spain, 2022 March 7th - 11th

Organizers: Ilka Kriegel, Teresa Gatti and Francesco Scotognella

Contributed talk, Miriam Karpińska, presentation 324
DOI: https://doi.org/10.29363/nanoge.nsm.2022.324
Publication date: 7th February 2022

In this work, we combine experimental and theoretical studies of the excitation transfer in heterostructures consisting of two different van der Waals materials: a monolayer transition metal dichalcogenide (TMD) and a 2D perovskite. Our results show that the band alignment inhibits the electron transfer. We present evidence for the excitation transfer and show that it is dominated by either non-radiative energy transfer or by hole transfer, depending on the alignment of exciton states.

Due to the unprecedented flexibility offered by the total relaxation of lattice matching requirements, stacks of van der Waals semiconductors are currently the focus of intense investigations with view of applications in ultrathin optoelectronics. Such heterostructures (HSs) exhibit novel properties, absent from the constituent materials. Excitation transfer between the stacked layers can occur via a charge [1] or energy [2] transfer. Design of future devices requires a thorough understanding, which of the mechanisms dominates. This knowledge is, at present, lacking.

Here, we present a combined spectroscopic and density functional theory (DFT) studies of three samples: PEA₂PbI₄ /MoSe₂ (PEPI/MoSe₂), PEA₂PbI₄ /WS₂ (PEPI/WS₂) stacks (where PEA stands for phenylethylammonium) and BA₂PbI₄ /MoSe₂ (BAPI/MoSe₂, where BA is butylammonium). For all three HSs, the DFT calculations have shown that the obtained stacks exhibit a type II band alignment with valence band edge (VBE) in the perovskite and conduction band edge (CBE) in the TMD layer. However, the electron transfer between materials is hindered by the presence of organic spacer layers in-between slabs of PbI₄ octahedra.

Low temperature photoluminescene (PL) mapping, PL excitation, and time-resolved PL measurements provided compelling evidence for the excitation transfer in all the studied HSs. However, the nature of the transfer depends on the energy alignment of the exciton states. Namely, in PEPI/WS₂, where the PEPI exciton is in resonance with the B-exciton of WS₂, a non-radiative resonant energy transfer together with hole transfer, are observed. On the other hand, in PEPI/MoSe₂ and BAPI/MoSe₂, where the B-exciton lies lower in energy, the resonant transfer is inhibited and a hole transfer dominates in the systems. It leads to an appearance of a long lived interlayer exciton, demonstrated for the first time in these HSs.

References:

[1] Rivera, P., Schaibley, J., Jones, A. et al. Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures. Nat Commun 6, 6242, 1-6 (2015)

[2] Froehlicher, G. et al.Charge Versus Energy Transfer in Atomically Thin Graphene-Transition Metal Dichalcogenide van der Waals Heterostructures Phys. Rev. X 8, 011007, 1-15 (2018)

Acknowledgements:

We would like to thank Omer Yaffe and Matan Menaham for providing the PEPI bulk crystals.

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