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

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 and E. Vesselli ()
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M. Corva: Dipartimento di Fisica, Università degli Studi di Trieste
A. Ferrari: Dipartimento di Fisica, Università degli Studi di Trieste
M. Rinaldi: Dipartimento di Fisica, Università degli Studi di Trieste
Z. Feng: Dipartimento di Fisica, Università degli Studi di Trieste
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
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
N. Seriani: The Abdus Salam International Centre for Theoretical Physics
E. Vesselli: Dipartimento di Fisica, Università degli Studi di Trieste

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-07190-1

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