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

Publikation: Beitrag in FachzeitschriftArtikelForschungBegutachtung

16 Zitate (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.
OriginalspracheEnglisch
Aufsatznummer4703
Seitenumfang8
FachzeitschriftNature Communications
Jahrgang9.2018
Ausgabenummer1
Frühes Online-Datum8 Nov. 2018
DOIs
PublikationsstatusVeröffentlicht - 1 Dez. 2018
Extern publiziertJa

Bibliographische Notiz

Funding Information:
A.F. would like to acknowledge Jutta Rogal for helpful discussions. E.V. acknowledges Silvio Modesti and Peter Weinberger for their precious comments. Financial support from the University of Trieste through project FRA2016 and from Beneficentia Stiftung is kindly acknowledged. M.R. and G.R. acknowledge the FWF Doctorate School DK + Solids4Fun (W1243). Computational resources were provided by ICTP. M.D.A. and R.C. acknowledge support from the SIR grant SUNDYN [Nr. RBSI14G7TL, CUP B82I15000910001] of the Italian Ministry of Education Universities and Research MIUR. M.D.A. and R.C. thank Alberto Morgante and Albano Cossaro for fruitful discussions.

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

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