TY - JOUR
T1 - Vibrational fingerprint of localized excitons in a two-dimensional metal-organic crystal
AU - Corva, Manuel
AU - Ferrari, A.
AU - Rinaldi, M.
AU - Feng, Zhijing
AU - Roiaz, Matteo
AU - Rameshan, Christoph
AU - Rupprechter, Günther
AU - Costantini, R.
AU - Dell’Angela, M.
AU - Pastore, G.
AU - Comelli, G.
AU - Seriani, N.
AU - Vesselli, Erik
N1 - Publisher Copyright: © 2018, The Author(s).
PY - 2018/12/1
Y1 - 2018/12/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85056219077&partnerID=8YFLogxK
U2 - 10.1038/s41467-018-07190-1
DO - 10.1038/s41467-018-07190-1
M3 - Article
C2 - 30409974
AN - SCOPUS:85056219077
SN - 2041-1723
VL - 9.2018
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 4703
ER -