Letter | Published:

Giant nonlinear response from plasmonic metasurfaces coupled to intersubband transitions

Nature volume 511, pages 6569 (03 July 2014) | Download Citation

Abstract

Intersubband transitions in n-doped multi-quantum-well semiconductor heterostructures make it possible to engineer one of the largest known nonlinear optical responses in condensed matter systems—but this nonlinear response is limited to light with electric field polarized normal to the semiconductor layers1,2,3,4,5,6,7. In a different context, plasmonic metasurfaces (thin conductor–dielectric composite materials) have been proposed as a way of strongly enhancing light–matter interaction and realizing ultrathin planarized devices with exotic wave properties8,9,10,11. Here we propose and experimentally realize metasurfaces with a record-high nonlinear response based on the coupling of electromagnetic modes in plasmonic metasurfaces with quantum-engineered electronic intersubband transitions in semiconductor heterostructures. We show that it is possible to engineer almost any element of the nonlinear susceptibility tensor of these structures, and we experimentally verify this concept by realizing a 400-nm-thick metasurface with nonlinear susceptibility of greater than 5 × 104 picometres per volt for second harmonic generation at a wavelength of about 8 micrometres under normal incidence. This susceptibility is many orders of magnitude larger than any second-order nonlinear response in optical metasurfaces measured so far12,13,14,15. The proposed structures can act as ultrathin highly nonlinear optical elements that enable efficient frequency mixing with relaxed phase-matching conditions, ideal for realizing broadband frequency up- and down-conversions, phase conjugation and all-optical control and tunability over a surface.

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Acknowledgements

This work was supported by NSF EAGER grant no. 1348049 (to M.A.B. and A.A.), AFOSR YIP award no. FA9550-10-1-0076 (M.A.B.), AFOSR YIP award no. FA9550-11-1-0009 (A.A.), and ONR MURI grant no. N00014-10-1-0942 (A.A.). The Walter Schottky Institute group acknowledges support from the Excellence Cluster ‘Nano Initiative Munich (NIM)’. Sample fabrication was carried out in the Microelectronics Research Center at the University of Texas at Austin, which is a member of the National Nanotechnology Infrastructure Network.

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Affiliations

  1. Department of Electrical and Computer Engineering, The University of Texas at Austin, Austin, Texas 78712, USA

    • Jongwon Lee
    • , Mykhailo Tymchenko
    • , Christos Argyropoulos
    • , Pai-Yen Chen
    • , Feng Lu
    • , Andrea Alù
    •  & Mikhail A. Belkin
  2. Walter Schottky Institut, Technische Universität München, Am Coulombwall 4, Garching 85748, Germany

    • Frederic Demmerle
    • , Gerhard Boehm
    •  & Markus-Christian Amann

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Contributions

J.L. designed the semiconductor heterostructure, calculated physical parameters and performed all fabrication and experimental measurements; M.T., C.A. and P.-Y.C. performed theoretical computations and structure optimization; F.L. assisted in experimental measurements; F.D., G.B. and M.-C.A. performed the semiconductor heterostructure growth; M.A.B. conceived the concept and the experiment; M.A.B. and A.A. developed the concept and planned and directed the research; and J.L., M.T., C.A., A.A. and M.A.B. wrote the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Mikhail A. Belkin.

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https://doi.org/10.1038/nature13455

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