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Register a new userOptical Spectroscopy in CoO: Phonons, Electric, and Magnetic Excitations
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The reflectivity of single-crystalline CoO has been studied by optical spectroscopy for wave numbers ranging from 100 to 28,000wn and for temperatures 8 $< T <$ 325 K@. A splitting of the cubic IR-active phonon mode on passing the antiferromagnetic phase transition at $T_N$ = 289 K has been observed. At low temperatures the splitting amounts to 15.0wn. In addition, we studied the splitting of the cubic crystal field ground state of the Co$^{2+}$ ions due to spin-orbit coupling, a tetragonal crystal field, and exchange interaction. Below $T_N$, magnetic dipole transitions between the exchange-split levels are identified and the energy-level scheme can be well described with a spin-orbit coupling $lambda = 151.1wn$, an exchange constant $J = 17.5wn$, and a tetragonal crystal-field parameter $D = -47.8wn$. Already in the paramagnetic state electric quadrupole transitions between the spin-orbit split level have been observed. At high frequencies, two electronic levels of the crystal-field-split $d$-manifold were identified at 8,000 and 18,500wn.
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We have measured the intricate temperature dependence of the Co L2,3 x-ray absorption spectra (2p-3d excitations) of CoO. To allow for accurate total electron yield measurements, the material has been grown in thin film form on a metallic substrate in order to avoid charging problems usually encountered during electron spectroscopic studies on bulk CoO samples. The changes in spectra due to temperature are in good agreement with detailed ligand-field calculations indicating that these changes are mostly due to thermal population of closely lying excited states, originating from degenerate t2g levels lifted by the spin-orbit coupling. Magnetic coupling in the ordered phase, modeled as a mean-field exchange field, mixes in excited states inducing a tetragonal charge density. The spin-orbit coupling induced splitting of the low energy states results in a non-trivial temperature dependence for the magnetic susceptibility.
We have investigated the phonon and the magnetic excitations in LaCoO3 by inelastic neutron scattering measurements. The acoustic phonon dispersions show some characteristic features of the folded Brillouin zone (BZ) for the rhombohedrally distorted perovskite structure containing two chemical formula units of LaCoO3 in the unit cell. We observed two transverse optical (TO) phonon branches along (delta, delta, delta), consistent with previously reported Raman active Eg modes which show remarkable softening associated with the spin-state transition [Ishikawa et al., (Phys. Rev. Lett. 93 (2004) 136401.)]. We found that the softening takes place in the TO mode over the whole BZ. In contrast, the acoustic phonons show no anomalous softening associated with the spin-state transition. The low-energy paramagnetic scattering at 8 K is weak, increasing towards a maximum at E > 15 meV, consistent with excitation of the nonmagnetic low-spin to magnetic intermediate-spin state of Co 3+ ions.
We determine the nature of coupled phonons and magnetic excitations in AlFeO3 using inelastic light scattering from 5 K to 315 K covering a spectral range from 100-2200 cm-1 and complementary first-principles density functional theory-based calculations. A strong spin-phonon coupling and magnetic ordering induced phonon renormalization are evident in (a) anomalous temperature dependence of many modes with frequencies below 850 cm-1, particularly near the magnetic transition temperature Tc ~ 250 K, (b) distinct changes in band positions of high frequency Raman bands between 1100-1800 cm-1, in particular a broad mode near 1250 cm-1 appears only below Tc attributed to the two-magnon Raman scattering. We also observe weak anomalies in the mode frequencies at ~ 100 K, due to a magnetically driven ferroelectric phase transition. Understanding of these experimental observations has been possible on the basis of first-principles calculations of phonons spectrum and their coupling with spins.
We report on the optical excitation spectra in Sr$_2$VO$_4$. The phonon modes are assigned and their evolution with temperature is discussed in the frame of the different phase transitions crossed upon cooling. Besides the expected infrared-active phonons we observe two additional excitations at about 290 cm$^{-1}$ and 840 cm$^{-1}$ which could correspond to electronic transitions of the V$^{4+}$ ions. Our experimental results are discussed in the context of recent experimental and theoretical studies of this material with a unique spin-orbital ground state.
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