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Light–matter coupling in large-area van der Waals superlattices

Abstract

Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks of disparate 2D layers with multiple repeating units. Here we present optical dispersion engineering in a superlattice structure comprising alternating layers of 2D excitonic chalcogenides and dielectric insulators. By carefully designing the unit cell parameters, we demonstrate greater than 90% narrow band absorption in less than 4 nm of active layer excitonic absorber medium at room temperature, concurrently with enhanced photoluminescence in square-centimetre samples. These superlattices show evidence of strong light–matter coupling and exciton–polariton formation with geometry-tuneable coupling constants. Our results demonstrate proof of concept structures with engineered optical properties and pave the way for a broad class of scalable, designer optical metamaterials from atomically thin layers.

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Fig. 1: Structure and composition of multilayer excitonic quantum well superlattices.
Fig. 2: Thickness and optical property optimization.
Fig. 3: Maintenance of monolayer properties.
Fig. 4: Observation of exciton polaritons in unpatterned multilayer superlattices.
Fig. 5: Waveguide characterization within the multilayer superlattice.

Data availability

The data that support the conclusions of this study are available from the corresponding author on request.

Code availability

The TMM codes used in this study for plotting and modelling are available from the corresponding author on request.

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Acknowledgements

D.J. acknowledges primary support for this work by the US Army Research Office under contract number W911NF-19-1-0109 and Air Force Office of Scientific Research (AFOSR) grant no. FA9550-21-1-0035. D.J. and J.L. also acknowledge partial support from grant nos. FA2386-20-1-4074 and FA2386-21-1-4063 and the University Research Foundation at Penn. D.J., E.A.S. and P.K. acknowledge support from the National Science Foundation (NSF) (grant no. DMR-1905853) and support from University of Pennsylvania Materials Research Science and Engineering Center (MRSEC) (grant no. DMR-1720530) in addition to usage of MRSEC supported facilities. The sample fabrication, assembly and characterization were carried out at the Singh Center for Nanotechnology at the University of Pennsylvania, which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program grant no. NNCI-1542153. F.B. is supported by the Vagelos Integrated Program in Energy Research. H.Z. was supported by Vagelos Institute of Energy Science and Technology graduate fellowship. S.B.A acknowledges support from Swiss National Science Foundation Early Postdoc Mobility Program (P2ELP2_187977). A.R.D. acknowledges support of NG Next, UCLA Council on Research Faculty Research grant and the Hellman Foundation. The TMDC monolayer samples were provided by the 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) facility at the Pennsylvania State University, which is funded by the NSF under cooperative agreement no. DMR-1539916. M.S. and N.R.G. acknowledge support from the Air Force Office of Scientific Research under award no. FA9550-19RYCOR050. This research used resources of the Center for Functional Nanomaterials, which is a US Department of Energy Office of Science User Facility, at Brookhaven National Laboratory under contract no. DE-SC0012704. We acknowledge helpful discussions on light coupling with M. W. Knight.

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Authors and Affiliations

Authors

Contributions

D.J. and A.R.D. conceived the idea/concept. D.J. directed the collaboration and execution. F.B. and J.L. optimized the superlattice design computationally. P.K. reduced the design to experiments including performing all superlattice fabrication, mechanical exfoliated sample preparation, Cross-sectional TEM sample preparation with help of K.K., optical spectroscopy (including low temperature measurements) and electron microscopy characterization (aberration-corrected STEM and EDS imaging). J.L. with the help of H.L. and J.D. performed simulations and fitting of the experimental data to computational models. B.S. assisted with measurement, optimization and fitting of optical constants. H. Zhang and S.B.A. assisted in sample preparation and characterization, respectively. M.K. assisted with theoretical modelling and interpretation. H. Zhu, T.H.C. and J.M.R. synthesized MoS2 and WS2 samples used in Al2O3 spaced superlattices. C. McAleese, X.W., B.R.C. and O.W. led the synthesis of WS2 and h-BN used in the h-BN spaced superlattice samples. M.J.M., M.S., C.M. and N.J.G. synthesized and characterized the MoSe2 samples. E.A.S. supervised the electron microscopy experiments. P.K., J.L. and D.J. wrote the paper and all authors contributed to the writing and editing of the paper.

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Correspondence to Artur R. Davoyan or Deep Jariwala.

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Competing interests

D.J., P.K., F.B., A.R.D., J.L. and E.A.S. have filed an invention disclosure based on this work. The authors declare no other competing interests.

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Supplementary Information, Figs. 1–34 and Discussion.

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Kumar, P., Lynch, J., Song, B. et al. Light–matter coupling in large-area van der Waals superlattices. Nat. Nanotechnol. 17, 182–189 (2022). https://doi.org/10.1038/s41565-021-01023-x

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