Strain-Modulated Interlayer Charge and Energy Transfers in MoS2/WS2Heterobilayer

Joon Seok Kim; Nikhilesh Maity; Myungsoo Kim; Suyu Fu; Rinkle Juneja; Abhishek Singh; Deji Akinwande; Jung Fu Lin

doi:10.1021/acsami.2c10982

Strain-Modulated Interlayer Charge and Energy Transfers in MoS₂/WS₂Heterobilayer

Joon Seok Kim, Nikhilesh Maity, Myungsoo Kim, Suyu Fu, Rinkle Juneja, Abhishek Singh, Deji Akinwande, Jung Fu Lin

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

Excitonic properties in 2D heterobilayers are closely governed by charge transfer (CT) and excitonic energy transfer (ET) at van der Waals interfaces. Various means have been employed to modulate the interlayer CT and ET, including electrical gating and modifying interlayer spacing, but with limited extent in their controllability. Here, we report a novel method to modulate these transfers in the MoS2/WS2 heterobilayer by applying compressive strain under hydrostatic pressure. Raman and photoluminescence measurements, combined with density functional theory calculations, show pressure-enhanced interlayer interaction of the heterobilayer. Heterobilayer-to-monolayer photoluminescence intensity ratio (η) of WS2 decreases by five times up to ≈4 GPa, suggesting enhanced ET, whereas it increases by an order of magnitude at higher pressures and reaches almost unity. Theoretical calculations show that orbital switching and charge transfers in the heterobilayer's hybridized conduction band are responsible for the non-monotonic modulation of the transfers. Our findings provide a compelling approach toward effective mechanical control of CT and ET in 2D excitonic devices.

Original language	English
Pages (from-to)	46841-46849
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	14
Issue number	41
DOIs	https://doi.org/10.1021/acsami.2c10982
State	Published - Oct 19 2022
Externally published	Yes

Funding

J.-S.K. and D.A. acknowledge support from the Defense Threat Reduction Agency (DTRA). J.-S.K. acknowledge support from NSF MRSEC program (DMR-1720139), and M.K. from NSF NASCENT ERC Center, respectively. N.M., R.J., and A.S. thank Materials Research Centre and Thematic Unit of Excellence, Indian Institute of Science, for providing the computational facilities. N.M., R.J., and A.S. acknowledge the support from Institute of Eminence (IoE) MHRD grant of Indian Institute of Science, and the grant from DST Korea. J.F.L. acknowledges support for the Renishaw inVia Raman system from Department of Geological Sciences and Jackson School of Geosciences at the University of Texas at Austin. J.-S.K. and D.A. acknowledge support from the Defense Threat Reduction Agency (DTRA). J.-S.K. acknowledge support from NSF MRSEC program (DMR-1720139), and M.K. from NSF NASCENT ERC Center respectively. N.M., R.J., and A.S. thank Materials Research Centre and Thematic Unit of Excellence, Indian Institute of Science, for providing the computational facilities. N.M., R.J., and A.S. acknowledge the support from Institute of Eminence (IoE) MHRD grant of Indian Institute of Science, and the grant from DST Korea. J.F.L. acknowledges support for the Renishaw inVia Raman system from Department of Geological Sciences and Jackson School of Geosciences at the University of Texas at Austin.

Keywords

Charge Transfer
Density Functional Theory
Diamond Anvil Cell
Energy Transfer
Heterobilayer
Strain Engineering

Access to Document

10.1021/acsami.2c10982

Cite this

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title = "Strain-Modulated Interlayer Charge and Energy Transfers in MoS2/WS2Heterobilayer",

abstract = "Excitonic properties in 2D heterobilayers are closely governed by charge transfer (CT) and excitonic energy transfer (ET) at van der Waals interfaces. Various means have been employed to modulate the interlayer CT and ET, including electrical gating and modifying interlayer spacing, but with limited extent in their controllability. Here, we report a novel method to modulate these transfers in the MoS2/WS2 heterobilayer by applying compressive strain under hydrostatic pressure. Raman and photoluminescence measurements, combined with density functional theory calculations, show pressure-enhanced interlayer interaction of the heterobilayer. Heterobilayer-to-monolayer photoluminescence intensity ratio (η) of WS2 decreases by five times up to ≈4 GPa, suggesting enhanced ET, whereas it increases by an order of magnitude at higher pressures and reaches almost unity. Theoretical calculations show that orbital switching and charge transfers in the heterobilayer's hybridized conduction band are responsible for the non-monotonic modulation of the transfers. Our findings provide a compelling approach toward effective mechanical control of CT and ET in 2D excitonic devices.",

keywords = "Charge Transfer, Density Functional Theory, Diamond Anvil Cell, Energy Transfer, Heterobilayer, Strain Engineering",

author = "Kim, {Joon Seok} and Nikhilesh Maity and Myungsoo Kim and Suyu Fu and Rinkle Juneja and Abhishek Singh and Deji Akinwande and Lin, {Jung Fu}",

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AU - Fu, Suyu

AU - Juneja, Rinkle

AU - Singh, Abhishek

AU - Akinwande, Deji

AU - Lin, Jung Fu

PY - 2022/10/19

Y1 - 2022/10/19

N2 - Excitonic properties in 2D heterobilayers are closely governed by charge transfer (CT) and excitonic energy transfer (ET) at van der Waals interfaces. Various means have been employed to modulate the interlayer CT and ET, including electrical gating and modifying interlayer spacing, but with limited extent in their controllability. Here, we report a novel method to modulate these transfers in the MoS2/WS2 heterobilayer by applying compressive strain under hydrostatic pressure. Raman and photoluminescence measurements, combined with density functional theory calculations, show pressure-enhanced interlayer interaction of the heterobilayer. Heterobilayer-to-monolayer photoluminescence intensity ratio (η) of WS2 decreases by five times up to ≈4 GPa, suggesting enhanced ET, whereas it increases by an order of magnitude at higher pressures and reaches almost unity. Theoretical calculations show that orbital switching and charge transfers in the heterobilayer's hybridized conduction band are responsible for the non-monotonic modulation of the transfers. Our findings provide a compelling approach toward effective mechanical control of CT and ET in 2D excitonic devices.

AB - Excitonic properties in 2D heterobilayers are closely governed by charge transfer (CT) and excitonic energy transfer (ET) at van der Waals interfaces. Various means have been employed to modulate the interlayer CT and ET, including electrical gating and modifying interlayer spacing, but with limited extent in their controllability. Here, we report a novel method to modulate these transfers in the MoS2/WS2 heterobilayer by applying compressive strain under hydrostatic pressure. Raman and photoluminescence measurements, combined with density functional theory calculations, show pressure-enhanced interlayer interaction of the heterobilayer. Heterobilayer-to-monolayer photoluminescence intensity ratio (η) of WS2 decreases by five times up to ≈4 GPa, suggesting enhanced ET, whereas it increases by an order of magnitude at higher pressures and reaches almost unity. Theoretical calculations show that orbital switching and charge transfers in the heterobilayer's hybridized conduction band are responsible for the non-monotonic modulation of the transfers. Our findings provide a compelling approach toward effective mechanical control of CT and ET in 2D excitonic devices.

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