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Giant Mechano-Optoelectronic Effect in an Atomically Thin Semiconductor

  • Wei Wu
    Wei Wu
    Department of Mechanical Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
    Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, United States
    More by Wei Wu
  • Jin Wang
    Jin Wang
    Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, United States
    Department of Materials Science and Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
    More by Jin Wang
  • Peter Ercius
    Peter Ercius
    Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    More by Peter Ercius
  • Nicomario C. Wright
    Nicomario C. Wright
    Department of Mechanical Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
  • Danielle M. Leppert-Simenauer
    Danielle M. Leppert-Simenauer
    Department of Mechanical Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
    Department of Physics, DePaul University, Chicago, Illinois 60614, United States
  • Robert A. Burke
    Robert A. Burke
    U.S. Army Research Laboratory, Adelphi, Maryland 20783, United States
    General Technical Services, LLC, Wall, New Jersey 07727, United States
  • Madan Dubey
    Madan Dubey
    U.S. Army Research Laboratory, Adelphi, Maryland 20783, United States
    More by Madan Dubey
  • Avinash M. Dogare
    Avinash M. Dogare
    Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, United States
    Department of Materials Science and Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
  • , and 
  • Michael T. Pettes*
    Michael T. Pettes
    Department of Mechanical Engineering, University of Connecticut, Storrs, Connecticut 06269, United States
    Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, United States
    *E-mail: [email protected]
Cite this: Nano Lett. 2018, 18, 4, 2351–2357
Publication Date (Web):March 20, 2018
https://doi.org/10.1021/acs.nanolett.7b05229
Copyright © 2018 American Chemical Society

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    Abstract

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    Transition metal dichalcogenides (TMDs) are particularly sensitive to mechanical strain because they are capable of experiencing high atomic displacements without nucleating defects to release excess energy. Being promising for photonic applications, it has been shown that as certain phases of layered TMDs MX2 (M = Mo or W; X = S, Se, or Te) are scaled to a thickness of one monolayer, the photoluminescence response is dramatically enhanced due to the emergence of a direct electronic band gap compared with their multilayer or bulk counterparts, which typically exhibit indirect band gaps. Recently, mechanical strain has also been predicted to enable direct excitonic recombination in these materials, in which large changes in the photoluminescence response will occur during an indirect-to-direct band gap transition brought on by elastic tensile strain. Here, we demonstrate an enhancement of 2 orders of magnitude in the photoluminescence emission intensity in uniaxially strained single crystalline WSe2 bilayers. Through a theoretical model that includes experimentally relevant system conditions, we determine this amplification to arise from a significant increase in direct excitonic recombination. Adding confidence to the high levels of elastic strain achieved in this report, we observe strain-independent, mode-dependent Grüneisen parameters over the entire range of tensile strain (1–3.59%), which were obtained as 1.149 ± 0.027, 0.307 ± 0.061, and 0.357 ± 0.103 for the E2g, A1g, and A21g optical phonon modes, respectively. These results can inform the predictive strain-engineered design of other atomically thin indirect semiconductors, in which a decrease in out-of-plane bonding strength may lead to an increase in the strength of strain-coupled optoelectronic effects.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.7b05229.

    • Additional synthesis, structural characterization, strain-validation experiment and model, and experimental details. Figures showing AFM and STEM analysis, photoluminescence-based layer number determination, the custom four-point bending apparatus, schematic of the Poisson effect on a bilayer, the reproducibility of strain-controlled PL emission spectra, patterned graphene, Raman spectra and Grüneisen parameters, PL spectra, and indirect-to-direct electronic band transition conversion. (PDF)

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