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Inelastic Light Scattering Spectroscopy of Magnons and Phonons in Nickel Oxide: Effects of Temperature

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 Added by Alexander Balandin
 Publication date 2017
  fields Physics
and research's language is English




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We report results of an investigation of the temperature dependence of the magnon and phonon frequencies in NiO. A combination of Brillouin - Mandelstam and Raman spectroscopies allowed us to elucidate the evolution of the phonon and magnon spectral signatures from the Brillouin zone center (GHz range) to the second-order peaks from the zone boundary (THz range). The temperature-dependent behavior of the magnon and phonon bands in the NiO spectrum indicates the presence of antiferromagnetic (AF) order fluctuation or a persistent AF state at temperatures above the Neel temperature (T=523 K). Tuning the intensity of the excitation laser provides a method for disentangling the features of magnons from acoustic phonons without the application of a magnetic field. Our results are useful for interpretation of the inelastic-light scattering spectrum of NiO, and add to the knowledge of its magnon properties important for THz spintronic devices.

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We demonstrate the use of the micro-Brillouin light scattering (micro-BLS) technique as a local temperature sensor for magnons in a Permalloy thin film and phonons in the glass substrate. A systematic shift in the frequencies of two thermally excited perpendicular standing spin wave modes as the film is uniformly heated allows us to achieve a temperature resolution better than 2.5 K. We demonstrate that the micro-BLS spectra can be used to measure the local temperatures of phonons and magnons across a thermal gradient. Such local temperature sensors are useful for investigating spin caloritronic and thermal transport phenomena in general.
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The physics of mutual interaction of phonon quasiparticles with electronic spin degrees of freedom, leading to unusual transport phenomena of spin and heat, has been a subject of continuing interests for decades. Understanding phonon properties in the context of spin-phonon coupling is essential for engineering functional phononic and spintronic devices. By means of inelastic neutron scattering and first-principle calculations, anomalous scattering spectral intensity from acoustic phonon was identified in the exemplary collinear antiferromagnetic nickel (II) oxide, unveiling strong correlations between spin and lattice degrees of freedom that renormalize the polarization of acoustic phonon. Anomalously large spectral intensity from acoustic phonons observed at small momentum transfer decays with increasing temperature and is successfully modeled with a modified magneto-vibrational scattering cross section, suggesting the presence of phonon driven of spin precession. On the other hand, TA phonon intensity that are forbidden by the scattering geometry is observed at a wide span of momentum transfer, suggesting a renormalization of phonon eigenvector.
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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.
Perovskite oxides exhibit a rich variety of structural phases hosting different physical phenomena that generate multiple technological applications. We find that topological phonons, i.e., nodal rings, nodal lines, and Weyl points, are ubiquitous in oxide perovskites in terms of structures (tetragonal, orthorhombic, and rhombohedral), compounds (BaTiO3, PbTiO3, and SrTiO3), and external conditions (photoexcitation, strain, and temperature). In particular, in the tetragonal phase of these compounds, all types of topological phonons can simultaneously emerge when stabilized by photoexcitation, whereas the tetragonal phase stabilized by thermal fluctuations only hosts a more limited set of topological phonon states. Additionally, we find that the photoexcited carrier concentration can be used to tune the topological phonon states and induce topological transitions even without associated structural phase changes. Overall, we propose oxide perovskites as a versatile platform in which to study topological phonons and their manipulation with light.
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