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

Manuel Corva, A. Ferrari, M. Rinaldi, Zhijing Feng, Matteo Roiaz, Christoph Rameshan, Günther Rupprechter, R. Costantini, M. Dell’Angela, G. Pastore, G. Comelli, N. Seriani, Erik Vesselli

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16 Citations (Scopus)

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 FeN 4 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.
Original languageEnglish
Article number4703
Number of pages8
JournalNature Communications
Volume9.2018
Issue number1
Early online date8 Nov 2018
DOIs
Publication statusPublished - 1 Dec 2018
Externally publishedYes

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Publisher Copyright: © 2018, The Author(s).

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