Titre :

Redox-controlled conductance of polyoxometalate molecular junctions

Auteur(s) :

Huez, Cécile [Auteur]
Institut d’Électronique, de Microélectronique et de Nanotechnologie - UMR 8520 [IEMN]
Nanostructures, nanoComponents & Molecules - IEMN [NCM - IEMN]
Guérin, David [Auteur]
Institut d’Électronique, de Microélectronique et de Nanotechnologie - UMR 8520 [IEMN]
Nanostructures, nanoComponents & Molecules - IEMN [NCM - IEMN]
Lenfant, Stephane [Auteur]
Institut d’Électronique, de Microélectronique et de Nanotechnologie - UMR 8520 [IEMN]
Nanostructures, nanoComponents & Molecules - IEMN [NCM - IEMN]
Volatron, Florence [Auteur]
Institut Parisien de Chimie Moléculaire [IPCM]
Calame, Michel [Auteur]
Université de Bâle = University of Basel = Basel Universität [Unibas]
Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] [EMPA]
Perrin, Mickael [Auteur]
Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] [ETH Zürich]
Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] [EMPA]
Proust, Anna [Auteur]
Institut Parisien de Chimie Moléculaire [IPCM]
Vuillaume, Dominique [Auteur]
Institut d’Électronique, de Microélectronique et de Nanotechnologie - UMR 8520 [IEMN]
Nanostructures, nanoComponents & Molecules - IEMN [NCM - IEMN]

Titre de la revue :

Nanoscale

Pagination :

13790-13800

Éditeur :

Royal Society of Chemistry

Date de publication :

2022

ISSN :

2040-3364

Mot(s)-clé(s) en anglais :

molecular electronics
conductive AFM
machine learning
polyoxometalate
redox
electron transport

Discipline(s) HAL :

Chimie/Matériaux
Physique [physics]/Matière Condensée [cond-mat]/Systèmes mésoscopiques et effet Hall quantique [cond-mat.mes-hall]

Résumé en anglais : [en]

We demonstrate the reversible in situ photoreduction of molecular junctions of phosphomolybdate [PMo12O40]3- monolayer self-assembled on flat gold electrodes, connected by the tip of a conductive atomic force microscope. ...
Lire la suite >We demonstrate the reversible in situ photoreduction of molecular junctions of phosphomolybdate [PMo12O40]3- monolayer self-assembled on flat gold electrodes, connected by the tip of a conductive atomic force microscope. The conductance of the one electron reduced [PMo12O40]4- molecular junction is increased by ∼ 10, this open-shell state is stable in the junction in air at room temperature. The analysis of a large current-voltage dataset by unsupervised machine learning and clustering algorithms reveals that the electron transport in the pristine phosphomolybdate junctions leads to symmetric current-voltage curves, controlled by the lowest unoccupied molecular orbital (LUMO) at 0.6-0.7 eV above the Fermi energy with ∼25% of the junctions having a better electronic coupling to the electrodes than the main part of the dataset. This analysis also shows that a small fraction (∼ 18% of the dataset) of the molecules is already reduced. The UV light in situ photoreduced phosphomolybdate junctions are systematically featuring slightly asymmetric current-voltage behaviors, which is ascribed to electron transport mediated by the single occupied molecular orbital (SOMO) nearly at resonance with the Fermi energy of the electrode and by a closely located single unoccupied molecular orbital (SUMO) at ∼0.3 eV above the SOMO with a weak electronic coupling to the electrodes (∼ 50% of the dataset) or at ∼0.4 eV but with a better electrode coupling (∼ 50% of the dataset). These results shed lights to the electronic properties of reversible switchable redox polyoxometalates, a key point for potential applications in nanoelectronic devices.Lire moins >

Langue :

Anglais

Vulgarisation :

Non

Collections :

• Institut d'Électronique, de Microélectronique et de Nanotechnologie (IEMN) - UMR 8520

Source :

Harvested from HAL