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Nickel oxide (NiO) has been studied extensively for various applicationsranging from electrochemistry to solar cells [1,2]. In recent years, NiOattracted much attention as an antiferromagnetic (AF) insulator material forspintronic devices [3-10]. Understanding the spin - phonon coupling in NiO is akey to its functionalization, and enabling AF spintronics' promise ofultra-high-speed and low-power dissipation [11,12]. However, despite its statusas an exemplary AF insulator and a benchmark material for the study ofcorrelated electron systems, little is known about the spin - phononinteraction, and the associated energy dissipation channel, in NiO. Inaddition, there is a long-standing controversy over the large discrepanciesbetween the experimental and theoretical values for the electron, phonon, andmagnon energies in NiO [13-23]. This gap in knowledge is explained by NiOoptical selection rules, high Neel temperature and dominance of the magnon bandin the visible Raman spectrum, which precludes a conventional approach forinvestigating such interaction. Here we show that by using ultraviolet (UV)Raman spectroscopy one can extract the spin - phonon coupling coefficients inNiO. We established that unlike in other materials, the spins of Ni atomsinteract more strongly with the longitudinal optical (LO) phonons than with thetransverse optical (TO) phonons, and produce opposite effects on the phononenergies. The peculiarities of the spin - phonon coupling are consistent withthe trends given by density functional theory calculations. The obtainedresults shed light on the nature of the spin - phonon coupling in AF insulatorsand may help in developing innovative spintronic devices.

Spin - Phonon Coupling in Nickel Oxide Determined from Ultraviolet Raman Spectroscopy