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Epitaxial strain induced magnetic transitions and phonon instabilities of the tetragonal SrRuO3

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 Added by Shijing Gong
 Publication date 2012
  fields Physics
and research's language is English




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Using density-functional theory calculations, we investigate the magnetic as well as the dynamical properties of tetragonal SrRuO3 (SRO) under the influence of epitaxial strain. It is found that both the tensile and compressive strain in the xy-plane could induce the abrupt change in the magnetic moment of Ru atom. In particular, under the in-plane ~4% compressive strain, a ferromagnetic to nonmagnetic transition is induced. Whereas for the tensile strain larger than 3%, the Ru magnetic moment drops gradually with the increase of the strain, exhibiting a weak ferromagnetic state. We find that such magnetic transitions could be qualitatively explained by the Stoner model. In addition, frozen phonon calculations at {Gamma} point reveal structural instabilities could occur under both compressive and tensile strains. Such instabilities are very similar to those of the ferroelectric perovskite oxides, even though SRO remains to be metallic in the range we studied. These might have influence on the physical properties of oxide supercells taking SRO as constituent.



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Thin films of the ferromagnetic metal SrRuO3 (SRO) show a varying easy magnetization axis depending on the epitaxial strain and undergo a metal-to-insulator transition with decreasing film thickness. We have investigated the magnetic properties of SRO thin films with varying thicknesses fabricated on SrTiO3(001) substrates by soft x-ray magnetic circular dichroism (XMCD) at the Ru M2,3 edge. Results have shown that, with decreasing film thickness, the film changes from ferromagnetic to non-magnetic around 3monolayer thickness, consistent with previous magnetization and magneto-optical Kerr effect measurements. The orbital magnetic moment perpendicular to the film was found to be ~ 0.1{mu}B/Ru atom, and remained nearly unchanged with decreasing film thickness while the spin magnetic moment decreases. Mechanism for the formation of the orbital magnetic moment is discussed based on the electronic structure of the compressively strained SRO film.
We present evidence of strain-induced modulation of electron correlation effects and increased orbital anisotropy in the rutile phase of epitaxial VO$_2$/TiO$_2$ films from hard x-ray photoelectron spectroscopy and soft V L-edge x-ray absorption spectroscopy, respectively. By using the U(1) slave spin formalism, we further argue that the observed anisotropic correlation effects can be understood by a model of orbital selective Mott transition at a filling that is non-integer, but close to the half-filling. Because the overlaps of wave functions between $d$ orbitals are modified by the strain, orbitally-dependent renormalizations of the bandwidths and the crystal fields occur with the application of strain. These renormalizations generally result in different occupation numbers in different orbitals. We find that if the system has a non-integer filling number near the half-filling such as for VO$_2$, certain orbitals could reach an occupation number closer to half-filling under the strain, resulting in a strong reduction in the quasiparticle weight $Z_{alpha}$ of that orbital. Moreover, an orbital selective Mott transition, defined as the case with $Z_{alpha} = 0$ in some, but not all orbitals, could be accessed by epitaxial strain-engineering of correlated electron systems.
Enhanced magnetic moment and coercivity in SrRuO3 thin films are significant issues for advanced technological usages and hence are researched extensively in recent times. Most of the previous reports on thin films with enhanced magnetic moment attributed the high spin state for the enhancement. Our magnetization results show high magnetic moment of 3.3 Bohr-magnetron/Ru ion in the epitaxial thin films grown on LSAT substrate against 1.2 Bohr-magnetron/Ru ion observed in bulk compound. Contrary to the expectation the Ru ions are found to be in low spin state and the orbital moment is shown to be contributing significantly in the enhancement of magnetic moment. We employed x-ray absorption spectroscopy and resonant valance band spectroscopy to probe the spin state and orbital contributions in these films. The existence of strong spin-orbit coupling responsible for the de-quenching of the 4d orbitals is confirmed by the observation of the non-statistical large branching ratio at the Ru M2,3 absorption edges. The relaxation of orbital quenching by strain engineering provides a new tool for enhancing magnetic moment. Strain disorder is shown to be an efficient mean to control the spin-orbit coupling.
Epitaxial thin films of SrRuO3 with large strain disorder were grown using pulsed laser deposition method which showed two distinct transition temperatures in Magnetic measurements. For the first time, we present visual evolution of magnetic domains across the two transitions using Magnetic force microscopy on these films. The study clearly showed that the magnetic anisotropy corresponding to the two transitions is different. It is observed that the perpendicular magnetic anisotropy is dominating in films which results in domain spin orientation preferably in out of plane direction. The Raman studies showed that the lattice is highly influenced by the magnetic order. The analysis of the phonon spectra around magnetic transition reveals the existence of strong spin-phonon coupling and the calculations resulted in spin-phonon coupling strength ({lambda}) values of {lambda} ~ 5 cm-1 and {lambda} ~ 8.5 cm-1, for SrRuO3 films grown on LSAT and SrTiO3 single crystal substrates, respectively.
The quadruple Calcium manganite (CaMn7O12) is a multiferroic material that exhibits a giant magnetically-induced ferroelectric polarization which makes it very interesting for magnetoelectric applications. Here, we report the Raman spectroscopy study on this compound of both the phonon modes and the low energy excitations from 4 K to room temperature. A detailed study of the Raman active phonon excitations shows that three phonon modes evidence a spin-phonon coupling at TN2 = 50 K. In particular, we show that the mode at 432 cm-1 associated to Mn(B)O6 (B position of the perovskite) rotations around the [111] cubic diagonal is impacted by the magnetic transition at 50 K and its coupling to the new modulation of the Mn spin in the (a,b) plane. At low energies, two large low energy excitations are observed at 25 and 47 cm-1. The first one disappears at 50 K and the second one at 90 K. We have associated these excitations to electro-magneto-active modes.
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