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Photoemission and X-ray Absorption Studies of the Diluted Magnetic Semiconductor Ba$_{1-y}$K$_{y}$(Zn$_{1-x}$Mn$_{x}$)$_{2}$As$_{2}$ Isostructural to Fe-based Superconductors

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 Added by Hakuto Suzuki
 Publication date 2014
  fields Physics
and research's language is English




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The electronic and magnetic properties of a new diluted magnetic semiconductor (DMS) Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$, which is isostructural to so-called 122-type Fe-based superconductors, are investigated by x-ray absorption spectroscopy (XAS) and resonance photoemission spectroscopy (RPES). Mn $L_{2,3}$-edge XAS indicates that the doped Mn atoms have the valence 2+ and strongly hybridize with the $4p$ orbitals of the tetrahedrally coordinating As ligands. The Mn $3d$ partial density of states (PDOS) obtained by RPES shows a peak around 4 eV and relatively high between 0-2 eV below the Fermi level ($E_{F}$) with little contribution at $E_{F}$, similar to that of the archetypal DMS Ga$_{1-x}$Mn$_{x}$As. This energy level creates $d^{5}$ electron configuration with $S=5/2$ local magnetic moments at the Mn atoms. Hole carriers induced by K substitution for Ba atoms go into the top of the As $4p$ valence band and are weakly bound to the Mn local spins. The ferromagnetic correlation between the local spins mediated by the hole carriers induces ferromagnetism in Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$

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154 - H. Suzuki , G. Q. Zhao , K. Zhao 2015
The electronic structure of the new diluted magnetic semiconductor Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ ($x=0.30$, $y=0.15$) in single crystal form has been investigated by angle-resolved photoemission spectroscopy (ARPES). %High density of states of nondispersive bands composed of the Zn $3d$ orbitals are observed with ultraviolet incident light. Measurements with soft x-rays clarify the host valence-band electronic structure primarily composed of the As $4p$ states. Two hole pockets around the $Gamma$ point, a hole corrugated cylinder surrounding the $Gamma$ and Z points, and an electron pocket around the Z point are observed, and explain the metallic transport of Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$. This is contrasted with Ga$_{1-x}$Mn$_{x}$As (GaMnAs), where it is located above the As $4p$ valence-band maximum (VBM) and no Fermi surfaces have been clearly identified. Resonance soft x-ray ARPES measurements reveal a nondispersive (Kondo resonance-like) Mn $3d$ impurity band near the Fermi level, as in the case of GaMnAs. However, the impurity band is located well below the VBM, unlike the impurity band in GaMnAs, which is located around and above the VBM. We conclude that, while the strong hybridization between the Mn $3d$ and the As $4p$ orbitals plays an important role in creating the impurity band and inducing high temperature ferromagnetism in both systems, the metallic transport may predominantly occur in the host valence band in Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ and in the impurity band in GaMnAs.
138 - H. Suzuki , T. Yoshida , S. Ideta 2013
We have studied the electronic structure of Ba(Fe$_{1-x}$Mn$_{x}$)$_{2}$As$_{2}$ ($x$=0.08), which fails to become a superconductor in spite of the formal hole doping like Ba$_{1-x}$K$_{x}$Fe$_{2}$As$_{2}$, by photoemission spectroscopy and X-ray absorption spectroscopy (XAS). With decreasing temperature, a transition from the paramagnetic phase to the antiferromagnetic phase was clearly observed by angle-resolved photoemission spectroscopy. XAS results indicated that the substituted Mn atoms form a strongly hybridized ground state. Resonance-photoemission spectra at the Mn $L_{3}$ edge revealed that the Mn 3d partial density of states is distributed over a wide energy range of 2-13 eV below the Fermi level ($E_F$), with little contribution around $E_F$. This indicates that the dopant Mn 3$d$ states are localized in spite of the strong Mn 3d-As $4p$ hybridization and split into the occupied and unoccupied parts due to the on-site Coulomb and exchange interaction. The absence of superconductivity in Ba(Fe$_{1-x}$Mn$_{x}$)$_{2}$As$_{2}$ can thus be ascribed both to the absence of carrier doping in the FeAs plane, and to the strong stabilizaiton of the antiferromagnetic order by the Mn impurities.
We used angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations to study the electronic structure of Ba(Fe1-x-yCoxMny)2As2 for x=0.06 and 0<=y <=0.07. From ARPES we derive that the substitution of Fe by Mn does not lead to hole doping, indicating a localization of the induced holes. An evaluation of the measured spectral function does not indicate a diverging effective mass or scattering rate near optimal doping. Thus the present ARPES results indicate a continuous evolution of the quasiparticle interaction and therefore question previous quantum critical scenarios.
We have performed x-ray magnetic circular dichroism (XMCD) and valence-band photoemission studies of the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te. XMCD signals due to ferromagnetism were observed at the Cr 2p absorption edge. Comparison with atomic multiplet calculations suggests that the magnetically active component of the Cr ion was divalent under the tetrahedral crystal field with tetragonal distortion along the crystalline a-, b-, and c-axes. In the valence-band spectra, spectral weight near the Fermi level was strongly suppressed, suggesting the importance of Jahn-Teller effect and the strong Coulomb interaction between the Cr 3d electrons.
We investigated the magnetic properties of (La$_{1-x}$Ba$_{x}$)(Zn$_{1-x}$Mn$_{x}$)AsO with $x$ varying from 0.005 to 0.05 at an external magnetic field of 1000 Oe. For doping levels of $x$ $leq$ 0.01, the system remains paramagnetic down to the lowest measurable temperature of 2 K. Only when the doping level increases to $x$ = 0.02 does the ferromagnetic ordering appear. Our analysis indicates that antiferromagnetic exchange interactions dominate for $x$ $leq$ 0.01, as shown by the negative Weiss temperature fitted from the magnetization data. The Weiss temperature becomes positive, i.e., ferromagnetic coupling starts to dominate, for $x$ $geq$ 0.02. The Mn-Mn spin interaction parameter $mid$$2J/k_B$$mid$ is estimated to be in the order of 10 K for both $x$ $leq$ 0.01 (antiferromagnetic ordered state) and $x$ $geq$ 0.02 (ferromagnetic ordered state). Our results unequivocally demonstrate the competition between ferromagnetic and antiferromagnetic exchange interactions in carrier-mediated ferromagnetic systems.
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