Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling
Abstract
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 channelsmore »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- Univ. of Kansas, Lawrence, KS (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1324084
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Charge transfer; Interlayer coupling; Twist angle; Van der Waals heterostructures
Citation Formats
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., and Geohegan, David B. Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling. United States: N. p., 2016.
Web. doi:10.1021/acsnano.6b01486.
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. Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling. United States. https://doi.org/10.1021/acsnano.6b01486
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., and Geohegan, David B. Thu .
"Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling". United States. https://doi.org/10.1021/acsnano.6b01486. https://www.osti.gov/servlets/purl/1324084.
@article{osti_1324084,
title = {Interlayer Interactions in Twisted WSe2/WS2 Bilayer Heterojunctions: Synthesis, Characterization, and Modeling},
author = {Wang, Kai and Huang, Bing and Tian, Mengkun and Ceballos, Frank and Lin, Ming-Wei and Mahjouri-Samani, Masoud and Boulesbaa, Abdelaziz and Puretzky, Alexander A. and Rouleau, Christopher and Yoon, Mina and Zhao, Hui and Xiao, Kai and Duscher, G. and Geohegan, David B.},
abstractNote = {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.},
doi = {10.1021/acsnano.6b01486},
journal = {ACS Nano},
number = 7,
volume = 10,
place = {United States},
year = {Thu Jun 16 00:00:00 EDT 2016},
month = {Thu Jun 16 00:00:00 EDT 2016}
}
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