No Arabic abstract
We have studied the electronic and magnetic states of Co and Mn atoms at the interface of the Co$_mathrm{2}$Mn$_{beta}$Si (CMS)/MgO ($beta$=0.69, 0.99, 1.15 and 1.29) magnetic tunnel junction (MTJ) by means of x-ray magnetic circular dichroism. In particular, the Mn composition ($beta$) dependences of the Mn and Co magnetic moments were investigated. The experimental spin magnetic moments of Mn, $m_mathrm{spin}$(Mn), derived from XMCD weakly decreased with increasing Mn composition $beta$ in going from Mn-deficient to Mn-rich CMS films. This behavior was explained by first-principles calculations based on the antisite-based site-specific formula unit (SSFU) composition model, which assumes the formation of only antisite defect, not vacancies, to accommodate off-stoichiometry. Furthermore, the experimental spin magnetic moments of Co, $m_mathrm{spin}$(Co), also weakly decreased with increasing Mn composition. This behavior was consistently explained by the antisite-based SSFU model, in particular, by the decrease in the concentration of Co$_mathrm{Mn}$ antisites detrimental to the half-metallicity of CMS with increasing $beta$. This finding is consistent with the higher TMR ratios which have been observed for CMS/MgO/CMS MTJs with Mn-rich CMS electrodes.
We have studied the local electronic structure of LaMn0.5Co0.5O3 using soft-x-ray absorption spectroscopy at the Co-L_3,2 and Mn-L_3,2 edges. We found a high-spin Co^{2+}--Mn^{4+} valence state for samples with the optimal Curie temperature. We discovered that samples with lower Curie temperatures contain low-spin nonmagnetic Co^{3+} ions. Using soft-x-ray magnetic circular dichroism we established that the Co^{2+} and Mn^{4+} ions are ferromagnetically aligned. We revealed also that the Co^{2+} ions have a large orbital moment: m_orb/m_spin ~ 0.47. Together with model calculations, this suggests the presence of a large magnetocrystalline anisotropy in the material and predicts a non-trivial temperature dependence for the magnetic susceptibility.
We have investigated the electronic structure of ZnO:Mn and ZnO:Mn,N thin films using x-ray magnetic circular dichroism (XMCD) and resonance-photoemission spectroscopy. From the Mn 2$p$$rightarrow3d$ XMCD results, it is shown that, while XMCD signals only due to paramagnetic Mn$^{2+}$ ions were observed in ZnO:Mn, nonmagnetic, paramagnetic and ferromagnetic Mn$^{2+}$ ions coexist in ZnO:Mn,N. XMCD signals of ZnO:Mn,N revealed that the localized Mn$^{2+}$ ground state and Mn$^{2+}$ state hybridized with ligand hole coexisted, implying $p$-$d$ exchange coupling. In the valence-band spectra, spectral weight near the Fermi level was suppressed, suggesting that interaction between magnetic moments in ZnO:Mn,N has localized nature.
We study the spin-dependent electronic structure of UTe and UT_{2}Si_{2} (T=Cu and Mn) compounds with a combination of x-ray magnetic circular dichroism measurements and first principle calculations. By exploiting the presence of sizable quadrupolar and dipolar contributions to the U L_{2,3}-edge x-ray absorption cross section we are able to provide unique information on the extent of hybridization between 5f and 6d/3d electronic states, a key parameter regulating the physical properties of all actinide materials. Since this information is hardly accessible to other probes, the new methodology opens up new venues for investigating this important class of materials.
We have studied the electronic structure of the molecular ferromagnet $beta$-Mn phthalocyanine ($beta$-MnPc) in a polycrystalline form, which has been reported to show ferromagnetism at T$<$8.6 K, by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD). From the experimental results and subsequent cluster-model calculation, we find that the ferromagnetic Mn ion in $beta$-MnPc is largely in the $^4$$E$$_g$ ground state arising from the ($e$$_{g}$)$^3$($b$$_{2g}$)$^1$($a$$_{1g}$)$^1$ [($d_{xz,yz}$)$^3$($d_{xy}$)$^1$($d_{z^{2}}$)$^1$] configuration of the Mn$^{2+}$ state. Considering that the highest occupied molecular orbital (HOMO) of MnPc with the $^4$$E$$_g$ ground state originates from the $a$$_{1g}$ orbital of the Mn$^{2+}$ ion, it is proposed that $a$$_{1g}$-$a$$_{1g}$ exchange coupling via the $pi$ orbitals of the phthalocyanine ring plays a crucial role in the ferromagnetism of $beta$-MnPc.
GdNi is a ferrimagnetic material with a Curie temperature Tc = 69 K which exhibits a large magnetocaloric effect, making it useful for magnetic refrigerator applications. We investigate the electronic structure of GdNi by carrying out x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at T = 25 K in the ferrimagnetic phase. We analyze the Gd M$_{4,5}$-edge ($3d$ - $4f$) and Ni L$_{2,3}$-edge ($2p$ - $3d$) spectra using atomic multiplet and cluster model calculations, respectively. The atomic multiplet calculation for Gd M$_{4,5}$-edge XAS indicates that Gd is trivalent in GdNi, consistent with localized $4f$ states. On the other hand, a model cluster calculation for Ni L$_{2,3}$-edge XAS shows that Ni is effectively divalent in GdNi and strongly hybridized with nearest neighbour Gd states, resulting in a $d$-electron count of 8.57. The Gd M$_{4,5}$-edge XMCD spectrum is consistent with a ground state configuration of S = 7/2 and L=0. The Ni L$_{2,3}$-edge XMCD results indicate that the antiferromagnetically aligned Ni moments exhibit a small but finite magnetic moment ( $m_{tot}$ $sim$ 0.12 $mu_B$ ) with the ratio $m_{o}/m_{s}$ $sim$ 0.11. Valence band hard x-ray photoemission spectroscopy shows Ni $3d$ features at the Fermi level, confirming a partially filled $3d$ band, while the Gd $4f$ states are at high binding energies away from the Fermi level. The results indicate that the Ni $3d$ band is not fully occupied and contradicts the charge-transfer model for rare-earth based alloys. The obtained electronic parameters indicate that GdNi is a strongly correlated charge transfer metal with the Ni on-site Coulomb energy being much larger than the effective charge-transfer energy between the Ni $3d$ and Gd $4f$ states.