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Register a new userElectronic configuration of Mn ions in the $pi$-d molecular ferromagnet $beta$-Mn phthalocyanine studied by soft x-ray magnetic circular dichroism
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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.
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The magnetic properties of as-grown Ga$_{1-x}$Mn$_{x}$As have been investigated by the systematic measurements of temperature and magnetic field dependent soft x-ray magnetic circular dichroism (XMCD). The {it intrinsic} XMCD intensity at high temperatures obeys the Curie-Weiss law, but residual spin magnetic moment appears already around 100 K, significantly above Curie temperature ($T_C$), suggesting that short-range ferromagnetic correlations are developed above $T_C$. The present results also suggest that antiferromagnetic interaction between the substitutional and interstitial Mn (Mn$_{int}$) ions exists and that the amount of the Mn$_{int}$ affects $T_C$.
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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.
X-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectra at the L$_{2,3}$ edges of Mn in (Ge,Mn) compounds have been measured and are compared to the results of first principles calculation. Early textit{ab initio} studies show that the Density Functional Theory (DFT) can very well describe the valence band electronic properties but fails to reproduce a characteristic change of sign in the L$_{3}$ XMCD spectrum of Mn in Ge$_3$Mn$_5$, which is observed in experiments. In this work we demonstrate that this disagreement is partially related to an underestimation of the exchange splitting of Mn 2$p$ core states within the local density approximation. It is shown that the change in sign experimentally observed is reproduced if the exchange splitting is accurately calculated within the Hartree-Fock approximation, while the final states can be still described by the DFT. This approach is further used to calculate the XMCD in different (Ge,Mn) compounds. It demonstrates that the agreement between experimental and theoretical spectra can be improved by combining state of the art calculations for the core and valence states respectively.
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