Phase competition in transition metal oxides has attracted remarkable interest for fundamental aspects and technological applications. Here, we report a concurrent study of the phase transitions in undoped and Cr-doped VO$$_2$$ 2 thin films. The structural, morphological and electrical properties of our films are examined and the microstructural effect on the metal–insulator transition (MIT) are highlighted. We further present a distinctive approach for analyzing the Raman data of undoped and Cr-doped VO$$_2$$ 2 thin films as a function of temperature, which are quantitatively correlated to the electrical measurements of VO$$_2$$ 2 films to give an insight into the coupling between the structural phase transition (SPT) and the MIT. These data are also combined with reported EXAFS measurements and a connection between the Raman intensities and the mean Debye–Waller factors $$\sigma ^2$$ σ 2 is established. We found that the temperature dependence of the $$\sigma _{R}^{2}(V-V)$$ σ R 2 ( V - V ) as calculated from the Raman intensity retraces the temperature profile of the $$\sigma _{EXAFS}^{2}(V-V)$$ σ EXAFS 2 ( V - V ) as obtained from the EXAFS data analysis. Our findings provide an evidence on the critical role of the thermal vibrational disorder in the VO$$_2$$ 2 phase transitions. Our study demonstrates that correlating Raman data with EXAFS analysis, the lattice and electronic structural dynamics can be probed.
The multiferroic and the rotating magnetocaloric properties of Nd 0.8 Tb 0.2 Mn 2 O 5 are investigated by microscopic optical probes and macroscopic magnetic measurements. Raman-active phonons as a function of temperature, and Nd 3+ and Tb 3+ infrared active crystal-field (CF) excitations as a function of temperature and under magnetic fields up to 11 T have been studied in Nd 0.8 Tb 0.2 Mn 2 O 5 . The obtained results are compared to those of NdMn 2 O 5 and TbMn 2 O 5 reference compounds. The observation of one set of Raman-active phonons and CF excitations rule out possible twinning while their energy positions and thermal evolutions indicate noticeable changes of Mn1-O3-Mn1 and TbO 8 structural units. This would explain the nature of separated magnetic phases in Nd 0.8 Tb 0.2 Mn 2 O 5 . The degeneracy of the ground-state Kramers doublet is lifted ( 0 ∼ 9 cm -1 ), indicating that the Nd 3+ -Mn 3+ interaction impacts the magnetic and ferroelectric properties of Nd 0.8 Tb 0.2 Mn 2 O 5 . The Zeeman splitting of excited crystal-field levels of the Nd 3+ ions at low temperatures shows that the g z factor is weak compared to that in NdMn 2 O 5 . This indicates that the R 3+ spins in Nd 0.8 Tb 0.2 Mn 2 O 5 are mostly aligned within the ab-plane. The nature of magnetocrystalline anisotropy in Nd 0.8 Tb 0.2 Mn 2 O 5 as well as in all RMn 2 O 5 compounds is quantitatively investigated by studying the anisotropy of paramagnetic Curie temperatures along (θ || ) and perpendicular (θ ⊥ ) to the c axis, (θ || − θ ⊥ ), as a function of the rare-earth atomic number. It is particularly found that the magnetocrystalline anisotropy is mainly determined by the quadrupolar charge distribution of 4 f shells. The rotating magnetocaloric effect in Nd 0.8 Tb 0.2 Mn 2 O 5 is also evaluated and compared to that in NdMn 2 O 5 and TbMn 2 O 5 . Our findings show that Nd-and Tb-separated magnetic phases independently contribute to the magnetocaloric effect of Nd 0.8 Tb 0.2 Mn 2 O 5 .
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