Room Temperature Spin‐Phonon Coupling in Cr 2 O 3 Nanocrystals

In this study, nanocrystals of antiferromagnetic Cr 2 O 3 are shown via Raman spectroscopy to display peculiar lattice dynamics in terms of phonon softening and the occurrence of an exceptionally strong spin‐phonon coupling. This effect, which is observed to persist well above the onset of the antiferromagnetic ordering temperature, is ascribed to locally correlated spin fluctuations due to the modulation of the magnetic exchange interactions as the chromium atoms oscillate about their equilibrium position. It is found that the spin‐phonon coupling strength is governed by the competing antiferromagnetic and ferromagnetic interactions, where changes in the surface spin configuration can also play a crucial role. Overall, this work proves the size dependence of the interplay between the crystalline and magnetic structures in 3D antiferromagnets varying the surface‐to‐volume ratio and helps establish the fundamentals for a spin‐phonon coupling engineering at the nanoscale via a simple route in a very stable and easy to synthesize material. More importantly, it demonstrates the possibility of coupling phononic excitations with the magnetization dynamics at room temperature, offering a highly prospective nanomaterial for the design of novel magnonic devices.