NDLI: Dynamics of intramolecular spin exchange interaction of a nitronyl nitroxide diradical in solution and on surfaces

Content Provider	Royal Society of Chemistry (RSC)
Author	Vidal-Gancedo, J. Lloveras, V. Badetti, E. Veciana, J.
Copyright Year	2016
Abstract	In this paper we report the study of the dynamics of a thermally modulated intramolecular spin exchange interaction of a novel diradical nitronyl nitroxide-substituted disulfide in solution and when it is grafted on a gold surface. The structure of this diradical was designed to have flexible chains leading to intramolecular collisions and hence spin exchange interaction, and with an appropriate binding group to be grafted on the gold surface to study its behavior on the surface. In solution, this diradical shows a strong spin exchange interaction between both radicals which is modulated by temperature, but also gold nanoparticles (AuNPs) functionalized with this diradical permit investigation of such a phenomenon in surface-grafted radicals. The spin-labelled AuNP synthesis was optimized to obtain high coverage of spin labels to lead to high spin exchange interaction. The obtained AuNPs were studied by Electron Paramagnetic Resonance (EPR), UV-Vis, and IR spectroscopies, HR-TEM microscopy, Cyclic Voltammetry (CV), Energy Dispersive X-ray analysis (EDX) and Thermogravimetric Analysis (TGA). This inorganic–organic hybrid material also showed dipolar interactions between its radicals which were confirmed by the appearance in the EPR spectra of an \|Δms\| = 2 transition at half-field. This signal gives direct evidence of the presence of a high-spin state and permitted us to study the nature of the magnetic coupling between the spins which was found to be antiferromagnetic. Self-Assembled Monolayers (SAMs) of these radicals on the Au (111) substrate were also prepared and studied by contact angle, X-Ray Photoelectron Spectroscopy (XPS), Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS), Cyclic Voltammetry and EPR. The magnetic as well as the electrochemical properties of the hybrid surfaces were studied and compared with the properties of this diradical in solution. Analogies between the properties of AuNPs with high coverage of radicals and those of SAM were observed.
Starting Page	5049
Ending Page	5058
Page Count	10
File Format	HTM / HTML PDF
ISSN	20403364
Volume Number	8
Issue Number	9
Journal	Nanoscale
DOI	10.1039/c5nr08824k
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Antiferromagnetism Photoelectron Spectroscopy Thermogravimetric analysis EPR Cyclic Voltammetry Contact angle Cyclic voltammetry X-ray crystallography Diradical Microscopy Electron Paramagnetic Resonance Exchange interaction Disulfide Electrochemistry Electron paramagnetic resonance
Content Type	Text
Resource Type	Article
Subject	Nanoscience and Nanotechnology

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