Title: Spin - Phonon Coupling in Nickel Oxide Determined from Ultraviolet Raman Spectroscopy,
Abstract: Nickel oxide (NiO) has been studied extensively for various applications
ranging from electrochemistry to solar cells [1,2]. In recent years, NiO
attracted much attention as an antiferromagnetic (AF) insulator material for
spintronic devices [3-10]. Understanding the spin - phonon coupling in NiO is a
key to its functionalization, and enabling AF spintronics' promise of
ultra-high-speed and low-power dissipation [11,12]. However, despite its status
as an exemplary AF insulator and a benchmark material for the study of
correlated electron systems, little is known about the spin - phonon
interaction, and the associated energy dissipation channel, in NiO. In
addition, there is a long-standing controversy over the large discrepancies
between the experimental and theoretical values for the electron, phonon, and
magnon energies in NiO [13-23]. This gap in knowledge is explained by NiO
optical selection rules, high Neel temperature and dominance of the magnon band
in the visible Raman spectrum, which precludes a conventional approach for
investigating such interaction. Here we show that by using ultraviolet (UV)
Raman spectroscopy one can extract the spin - phonon coupling coefficients in
NiO. We established that unlike in other materials, the spins of Ni atoms
interact more strongly with the longitudinal optical (LO) phonons than with the
transverse optical (TO) phonons, and produce opposite effects on the phonon
energies. The peculiarities of the spin - phonon coupling are consistent with
the trends given by density functional theory calculations. The obtained
results shed light on the nature of the spin - phonon coupling in AF insulators
and may help in developing innovative spintronic devices.