Year: 2025
Type: article
Abstract: Single-molecule devices (SMDs) offer a transformative path beyond conventional electronics, leveraging the unique quantum properties of individual molecules. Fullerenes, particularly C 60, are highly attractive candidates for SMDs owing to their unique electronic properties and structural versatility. Gold is widely employed as an electrode material, making the C 60 –Au interface a key determinant of device performance. However, the interaction nature between C 60 and gold, even for a single gold atom, remains elusive. Herein, we report the Ar-tagged infrared multiple photon dissociation spectrum of the [C 60 Au] + cluster aided with density functional theory calculations. Our results suggest that the configurations of the atop (η 1 ) site and the bridge site between two hexagons (η 2(6–6) ) likely coexist for [C 60 Au] +, with the η 1 configuration being slightly more favorable. Charge analysis reveals that C 60 accumulates more positive charges (η 1, +0.70 e; η 2(6–6), +0.66 e ) and participates in the bonding with gold in the form of C 60 + . Energy decomposition analysis combined with extended transition state-natural orbitals for chemical valence calculations reveal that the C 60 + –Au interaction involves electron-sharing and dative bonding components, while in the neutral C 60 Au complex there are only dative bonds. These findings offer molecular-level insights into metal–fullerene interactions and contribute to the fundamental basis for designing fullerene-based single-molecule devices.
Authors: Hao Li, Jianzhi Xu, Jiaqi Xin, Olga V. Lushchikova, Ya-Ke Li, Joost M. Bakker, Ewald Janssens, Gao-Lei Hou
Language: English
Subfield: Organic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W4417050705