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Vibrational fingerprint of localized excitons in a two-dimensional metal-organic crystal

Author

Listed:
  • M. Corva

    (Dipartimento di Fisica, Università degli Studi di Trieste
    Istituto Officina dei Materiali CNR-IOM)

  • A. Ferrari

    (Dipartimento di Fisica, Università degli Studi di Trieste
    ICAMS, Ruhr-Universität Bochum)

  • M. Rinaldi

    (Dipartimento di Fisica, Università degli Studi di Trieste)

  • Z. Feng

    (Dipartimento di Fisica, Università degli Studi di Trieste
    University of California, Irvine)

  • M. Roiaz

    (Technische Universität Wien)

  • C. Rameshan

    (Technische Universität Wien)

  • G. Rupprechter

    (Technische Universität Wien)

  • R. Costantini

    (Dipartimento di Fisica, Università degli Studi di Trieste
    Istituto Officina dei Materiali CNR-IOM)

  • M. Dell’Angela

    (Istituto Officina dei Materiali CNR-IOM)

  • G. Pastore

    (Dipartimento di Fisica, Università degli Studi di Trieste)

  • G. Comelli

    (Dipartimento di Fisica, Università degli Studi di Trieste
    Istituto Officina dei Materiali CNR-IOM)

  • N. Seriani

    (The Abdus Salam International Centre for Theoretical Physics)

  • E. Vesselli

    (Dipartimento di Fisica, Università degli Studi di Trieste
    Istituto Officina dei Materiali CNR-IOM)

Abstract

Long-lived excitons formed upon visible light absorption play an essential role in photovoltaics, photocatalysis, and even in high-density information storage. Here, we describe a self-assembled two-dimensional metal-organic crystal, composed of graphene-supported macrocycles, each hosting a single FeN4 center, where a single carbon monoxide molecule can adsorb. In this heme-like biomimetic model system, excitons are generated by visible laser light upon a spin transition associated with the layer 2D crystallinity, and are simultaneously detected via the carbon monoxide ligand stretching mode at room temperature and near-ambient pressure. The proposed mechanism is supported by the results of infrared and time-resolved pump-probe spectroscopies, and by ab initio theoretical methods, opening a path towards the handling of exciton dynamics on 2D biomimetic crystals.

Suggested Citation

  • M. Corva & A. Ferrari & M. Rinaldi & Z. Feng & M. Roiaz & C. Rameshan & G. Rupprechter & R. Costantini & M. Dell’Angela & G. Pastore & G. Comelli & N. Seriani & E. Vesselli, 2018. "Vibrational fingerprint of localized excitons in a two-dimensional metal-organic crystal," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-07190-1
    DOI: 10.1038/s41467-018-07190-1
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