Electronically Coupled 2D Polymer/MoS2 Heterostructures

Halleh B. Balch; Austin M. Evans; Raghunath R. Dasari; Hong Li; Ruofan Li; Simil Thomas; Danqing Wang; Ryan P. Bisbey; Kaitlin Slicker; Ioannina Castano; Sangni Xun; Lili Jiang; Chenhui Zhu; Nathan Gianneschi; Daniel C. Ralph; Jean-Luc Bredas; Seth R. Marder; William R. Dichtel; Feng Wang

doi:10.1021/jacs.0c10151

Electronically Coupled 2D Polymer/MoS2 Heterostructures

Halleh B. Balch, Austin M. Evans, Raghunath R. Dasari, Hong Li, Ruofan Li, Simil Thomas, Danqing Wang, Ryan P. Bisbey, Kaitlin Slicker, Ioannina Castano, Sangni Xun, Lili Jiang, Chenhui Zhu, Nathan Gianneschi, Daniel C. Ralph, Jean-Luc Bredas, Seth R. Marder, William R. Dichtel, Feng Wang

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29 Scopus citations

Abstract

Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS2 heterostructures. Control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.

Original language	English (US)
Journal	Journal of the American Chemical Society
DOIs	https://doi.org/10.1021/jacs.0c10151
State	Published - Dec 7 2020
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-12-14
Acknowledgements: We thank Yi Liu, Victoria Norman, Greg Stiehl, Shilong Zhao, Lindsey Young, and Sheng Wang. We also thank Ming-Yang Li and Lain-Jong Li at King Abdullah University of Science and Technology (KAUST) for providing the transition metal dichalcogenide substrates. This work was supported by the Army Research Office for a Multidisciplinary University Research Initiatives (MURI) award under grant W911NF15-1-0447. A.M.E. and I.C. were supported by the Ryan Fellowship and the Northwestern University International Institute for Nanotechnology and by NSF Graduate Research Fellowships [A.M.E. under grant DGE-1324585; I.C. under grant DGE-1842165]. J.L.B. and H.L. acknowledge support
from the College of Science, University of Arizona. This research used resources of the Advanced Light Source, a DOE Office of Science User Facility under contract no. DE-AC02- 05CH11231. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DEAC02−05CH11231.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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Balch, H. B., Evans, A. M., Dasari, R. R., Li, H., Li, R., Thomas, S., Wang, D., Bisbey, R. P., Slicker, K., Castano, I., Xun, S., Jiang, L., Zhu, C., Gianneschi, N., Ralph, D. C., Bredas, J.-L., Marder, S. R., Dichtel, W. R., & Wang, F. (2020). Electronically Coupled 2D Polymer/MoS2 Heterostructures. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.0c10151

@article{17fce8cd65aa438498e7cd39b9985dd0,

title = "Electronically Coupled 2D Polymer/MoS2 Heterostructures",

abstract = "Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS2 heterostructures. Control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.",

author = "Balch, {Halleh B.} and Evans, {Austin M.} and Dasari, {Raghunath R.} and Hong Li and Ruofan Li and Simil Thomas and Danqing Wang and Bisbey, {Ryan P.} and Kaitlin Slicker and Ioannina Castano and Sangni Xun and Lili Jiang and Chenhui Zhu and Nathan Gianneschi and Ralph, {Daniel C.} and Jean-Luc Bredas and Marder, {Seth R.} and Dichtel, {William R.} and Feng Wang",

note = "KAUST Repository Item: Exported on 2020-12-14 Acknowledgements: We thank Yi Liu, Victoria Norman, Greg Stiehl, Shilong Zhao, Lindsey Young, and Sheng Wang. We also thank Ming-Yang Li and Lain-Jong Li at King Abdullah University of Science and Technology (KAUST) for providing the transition metal dichalcogenide substrates. This work was supported by the Army Research Office for a Multidisciplinary University Research Initiatives (MURI) award under grant W911NF15-1-0447. A.M.E. and I.C. were supported by the Ryan Fellowship and the Northwestern University International Institute for Nanotechnology and by NSF Graduate Research Fellowships [A.M.E. under grant DGE-1324585; I.C. under grant DGE-1842165]. J.L.B. and H.L. acknowledge support from the College of Science, University of Arizona. This research used resources of the Advanced Light Source, a DOE Office of Science User Facility under contract no. DE-AC02- 05CH11231. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DEAC02−05CH11231. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2020",

month = dec,

day = "7",

doi = "10.1021/jacs.0c10151",

language = "English (US)",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

}

TY - JOUR

T1 - Electronically Coupled 2D Polymer/MoS2 Heterostructures

AU - Balch, Halleh B.

AU - Evans, Austin M.

AU - Dasari, Raghunath R.

AU - Li, Hong

AU - Li, Ruofan

AU - Thomas, Simil

AU - Wang, Danqing

AU - Bisbey, Ryan P.

AU - Slicker, Kaitlin

AU - Castano, Ioannina

AU - Xun, Sangni

AU - Jiang, Lili

AU - Zhu, Chenhui

AU - Gianneschi, Nathan

AU - Ralph, Daniel C.

AU - Bredas, Jean-Luc

AU - Marder, Seth R.

AU - Dichtel, William R.

AU - Wang, Feng

N1 - KAUST Repository Item: Exported on 2020-12-14 Acknowledgements: We thank Yi Liu, Victoria Norman, Greg Stiehl, Shilong Zhao, Lindsey Young, and Sheng Wang. We also thank Ming-Yang Li and Lain-Jong Li at King Abdullah University of Science and Technology (KAUST) for providing the transition metal dichalcogenide substrates. This work was supported by the Army Research Office for a Multidisciplinary University Research Initiatives (MURI) award under grant W911NF15-1-0447. A.M.E. and I.C. were supported by the Ryan Fellowship and the Northwestern University International Institute for Nanotechnology and by NSF Graduate Research Fellowships [A.M.E. under grant DGE-1324585; I.C. under grant DGE-1842165]. J.L.B. and H.L. acknowledge support from the College of Science, University of Arizona. This research used resources of the Advanced Light Source, a DOE Office of Science User Facility under contract no. DE-AC02- 05CH11231. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DEAC02−05CH11231. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2020/12/7

Y1 - 2020/12/7

N2 - Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS2 heterostructures. Control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.

AB - Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS2 heterostructures. Control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.

UR - http://hdl.handle.net/10754/666331

UR - https://pubs.acs.org/doi/10.1021/jacs.0c10151

U2 - 10.1021/jacs.0c10151

DO - 10.1021/jacs.0c10151

M3 - Article

C2 - 33284624

SN - 0002-7863

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

ER -

Electronically Coupled 2D Polymer/MoS2 Heterostructures

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