Vibronic Exciton-Phonon States in Stack-Engineered van der Waals Heterojunction Photodiodes

Fatemeh Barati, Trevor B. Arp, Shanshan Su, Roger K. Lake, Vivek Aji, Rienk Van Grondelle*, Mark S. Rudner, Justin C.W. Song, Nathaniel M. Gabor

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

Stack engineering, an atomic-scale metamaterial strategy, enables the design of optical and electronic properties in van der Waals heterostructure devices. Here we reveal the optoelectronic effects of stacking-induced strong coupling between atomic motion and interlayer excitons in WSe2/MoSe2 heterojunction photodiodes. To do so, we introduce the photocurrent spectroscopy of a stack-engineered photodiode as a sensitive technique for probing interlayer excitons, enabling access to vibronic states typically found only in molecule-like systems. The vibronic states in our stack are manifest as a palisade of pronounced periodic sidebands in the photocurrent spectrum in frequency windows close to the interlayer exciton resonances and can be shifted "on demand"through the application of a perpendicular electric field via a source-drain bias voltage. The observation of multiple well-resolved sidebands as well as their ability to be shifted by applied voltages vividly demonstrates the emergence of interlayer exciton vibronic structure in a stack-engineered optoelectronic device.

Original languageEnglish
Pages (from-to)5751-5758
Number of pages8
JournalNano Letters
Volume22
Issue number14
Early online date5 Jul 2022
DOIs
Publication statusPublished - 27 Jul 2022

Bibliographical note

Funding Information:
The authors acknowledge valuable discussions with Vasili Perebeinos. This work was supported by the Army Research Office Electronics Division Award no. W911NF2110260 (N.M.G., V.A., and T.B.A.), the Presidential Early Career Award for Scientists and Engineers (PECASE) through the Air Force Office of Scientific Research (award no. FA9550-20-1-0097; N.M.G. and T.B.A.), through support from the National Science Foundation Division of Materials Research CAREER Award (no. 1651247; N.M.G. and F.B.), and through the United States Department of the Navy Historically Black Colleges, Universities and Minority Serving Institutions (HBCU/MI) award no. N00014-19-1-2574 (N.M.G. and F.B.). T.B.A. acknowledges support from the Fellowships and Internships in Extremely Large Data Sets (FIELDS) program, a NASA MUREP Institutional Research Opportunity (MIRO) program (grant no. NNX15AP99A). R.v.G. acknowledges institutional support from the Royal Netherlands Academy of Arts and Sciences (KNAW) and the Canadian Institute of Solar Energy Research (CEA). J.C.W.S. acknowledges support from the Singapore Ministry of Education under its MOE AcRF Tier 3 Award (MOE2018-T3-1-002). M.S.R is grateful for the support of the European Research Council (ERC) under the European Union Horizon 2020 Research and Innovation Programme (grant agreement no. 678862) and the Villum Foundation. R.K.L. and S.S. acknowledge support from the NSF (EFRI-1433395). This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1053575 and allocation ID TG-DMR130081.

Publisher Copyright:
© 2022 American Chemical Society.

Funding

The authors acknowledge valuable discussions with Vasili Perebeinos. This work was supported by the Army Research Office Electronics Division Award no. W911NF2110260 (N.M.G., V.A., and T.B.A.), the Presidential Early Career Award for Scientists and Engineers (PECASE) through the Air Force Office of Scientific Research (award no. FA9550-20-1-0097; N.M.G. and T.B.A.), through support from the National Science Foundation Division of Materials Research CAREER Award (no. 1651247; N.M.G. and F.B.), and through the United States Department of the Navy Historically Black Colleges, Universities and Minority Serving Institutions (HBCU/MI) award no. N00014-19-1-2574 (N.M.G. and F.B.). T.B.A. acknowledges support from the Fellowships and Internships in Extremely Large Data Sets (FIELDS) program, a NASA MUREP Institutional Research Opportunity (MIRO) program (grant no. NNX15AP99A). R.v.G. acknowledges institutional support from the Royal Netherlands Academy of Arts and Sciences (KNAW) and the Canadian Institute of Solar Energy Research (CEA). J.C.W.S. acknowledges support from the Singapore Ministry of Education under its MOE AcRF Tier 3 Award (MOE2018-T3-1-002). M.S.R is grateful for the support of the European Research Council (ERC) under the European Union Horizon 2020 Research and Innovation Programme (grant agreement no. 678862) and the Villum Foundation. R.K.L. and S.S. acknowledge support from the NSF (EFRI-1433395). This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1053575 and allocation ID TG-DMR130081.

FundersFunder number
Canadian Institute of Solar Energy Research
HBCU/MIN00014-19-1-2574
United States Department of the Navy Historically Black Colleges, Universities and Minority Serving Institutions
National Science FoundationTG-DMR130081, EFRI-1433395, ACI-1053575
Division of Materials Research1651247
National Aeronautics and Space AdministrationNNX15AP99A
Air Force Office of Scientific ResearchFA9550-20-1-0097
Army Research OfficeW911NF2110260
Villum Fonden
Horizon 2020 Framework Programme
European Research Council
Ministry of Education - SingaporeMOE2018-T3-1-002
Koninklijke Nederlandse Akademie van Wetenschappen
Horizon 2020678862

    Keywords

    • interlayer excitons
    • photocurrent
    • stack engineering
    • van der Waals heterostructures
    • vibronic

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