Theoretical Insights into the Adsorption of Rare-Earth-Containing Single-Molecule Magnets on Solid Surfaces

Abstract

Single-molecule magnets (SMMs) offer stable quantum objects capable of exhibiting diverse magnetic states on the nanoscale, making them promising candidates for storing and processing quantized information at the molecular level. While substantial progress has been made in studying isolated SMMs over the past three decades, with particular emphasis on complexes containing rare-earth ions and endohedral metallofullerenes, the design of stable SMMs on solid surfaces remains a significant challenge for their practical application in electronic devices. In this Perspective, we reviewed recent advancements of SMMs on suitable solid surfaces that can retain and even enhance their magnetic properties. We discuss promising SMMs and the relevant physical parameters that contribute to their magnetic properties. By employing first-principles density functional theory methodologies, we primarily explore the intricate interactions between SMMs and surfaces, emphasizing the need for further theoretical investigations to bridge the gap and enable the design of functional SMMs on surfaces.

Development and Prospects in the Structure and Performance of Lanthanide Single-Molecule Magnets

“…Additionally, the distinctive f-electron of rare-earth atoms expands their development potential significantly in the realm of SMMs. Recent advancements in lanthanide SMMs research have demonstrated success in materials working above liquid nitrogen temperatures, presenting a unique chemical platform for the development of high-temperature SMMs. − Moreover, extensive magnetic research has given rise to hybrid systems based on Ln-SMMs, paving the way for intriguing multifunctional applications in future devices.…”

Electrode-Supported Endohedral Metallofullerenes: Insights into the Confined Internal Dynamics

“…Despite these observations, the mechanism by which the electrode affect thermal stability and the dynamics remains unclear, stemming from a lack of substantial understanding of the intricate interplay between electrostatic interactions, covalent bonds, and van der Waals (vdW) forces at the interface (Scheme ). − This hinders the rational adjustment of interfacial coupling to achieve an ordered arrangement of the encapsulated atom at elevated temperatures. Furthermore, the electric field, unavoidably introduced by the bias voltage, can also disturb stability due to the diverse intramolecular dipole moments of the EMFs with varied metal positions. , In this context, understanding the synergetic effect of the electrode and electric field on the stability of the encapsulated metal within the fullerene cage becomes crucial for comprehending the dynamics of EMFs and exploring their potential applications in molecular ferroelectricity and ferromagnetism, − which are still far less explored.…”

Perspective, Review, and Featured Articles of 2023

“…Single-molecule magnets have been studied for possible use in information storage. Liu and co-workers employed first-principles DFT calculations to understand orbital hybridization when the molecules are adsorbed on metal surfaces …”