Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling

Wang, Kai; Huang, Bing; Tian, Mengkun; Ceballos, Frank; Lin, Ming-Wei; Mahjouri-Samani, Masoud; Boulesbaa, Abdelaziz; Puretzky, Alexander A.; Rouleau, Christopher; Yoon, Mina; Zhao, Hui; Xiao, Kai; Duscher, G.; Geohegan, David B.

doi:10.1021/acsnano.6b01486

Title: Interlayer Interactions in Twisted WSe₂/WS₂ Bilayer Heterojunctions: Synthesis, Characterization, and Modeling

Journal Article · Thu Jun 16 00:00:00 EDT 2016 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.6b01486· OSTI ID:1324084

Wang, Kai ^[1]; Huang, Bing ^[1]; Tian, Mengkun ^[2]; Ceballos, Frank ^[3]; Lin, Ming-Wei ^[1]; Mahjouri-Samani, Masoud ^[1]; Boulesbaa, Abdelaziz ^[1]; Puretzky, Alexander A. ^[1]; Rouleau, Christopher ^[1]; Yoon, Mina ^[1]; Zhao, Hui ^[3]; Xiao, Kai ^[1]; Duscher, G. ^[2]; Geohegan, David B. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Kansas, Lawrence, KS (United States)

Twisting adjacent layers in van der Waals solids can significantly alter their interlayer interactions for tunable optical and electronic properties. Here, we report theoretical calculations, fabrication, and detailed characterizations of WSe₂/WS₂ bilayer heterojunctions with various twist angles that were synthesized by artificially stacking monolayers of CVD-grown WS₂ and WSe₂. Density functional calculations predicted the formation of type-II heterojunctions for the stamped bilayers, with band structures that strongly depend on the interlayer twist angle. Raman spectroscopy reveals strong interlayer coupling with the appearance of a layer-number sensitive mode of WS₂ at 311 cm^-1 in WSe₂/WS₂ bilayers. This strong interlayer coupling resulted in a 1~2 order of magnitude quenching of the photoluminescence. The broadening and shifts were observed in micro-absorption spectroscopy of WSe₂/WS₂ bilayers, which resulted in a net ~10% enhancement in integrated absorption strength across the visible spectrum with respect to the sum of the individual monolayer spectra. The observed 24 4 meV broadening of the WSe₂ A-exciton absorption band in the bilayers provided an estimate on the rate of charge transfer between the layers that ranged from 23 to 33 fs, and was supported by direct femtosecond pump-probe measurements. These results indicate that interlayer exciton formation and non-radiative decay channels dominate optical properties in these bilayers, which may be important for tunable future photovoltaics and detector applications.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1324084

Journal Information:: ACS Nano, Vol. 10, Issue 7; ISSN 1936-0851

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 234 works

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Ultrafast transition between exciton phases in van der Waals heterostructures Merkl, Philipp; Mooshammer, Fabian; Steinleitner, Philipp Universität Regensburg https://doi.org/10.5283/epub.41038	text	January 2019
Dark excitons and the elusive valley polarization in transition metal dichalcogenides Baranowski, M.; Surrente, A.; Maude, D. K. arXiv https://doi.org/10.48550/arxiv.1701.03070	text	January 2017
Thermal boundary conductance and phonon transmission in hexagonal boron nitride/graphene heterostructures Brown, David B.; Bougher, Thomas L.; Zhang, Xiang arXiv https://doi.org/10.48550/arxiv.1903.06385	text	January 2019

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Title: Interlayer Interactions in Twisted WSe₂/WS₂ Bilayer Heterojunctions: Synthesis, Characterization, and Modeling