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Register a new userTuning the hybridization and magnetic ground state of electron and hole doped CeOs$_2$Al$_{10}$: an x-ray spectroscopy study
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Here we present linear and circular polarized soft x-ray absorption spectroscopy (XAS) data at the Ce $M_{4,5}$ edges of the electron (Ir) and hole-doped (Re) Kondo semiconductor CeOs$_2$Al$_{10}$. Both substitutions have a strong impact on the unusual high N$acute{e}$el temperature, $T_N$=28.5,K, and also the direction of the ordered moment in case of Ir. The substitution dependence of the linear dichroism is weak thus validating the crystal-field description of CeOs$_2$Al$_{10}$ being representative for the Re and Ir substituted compounds. The impact of electron- and hole-doping on the hybridization between conduction and 4$f$ electrons is related to the amount of $f^0$ in the ground state and reduction of x-ray magnetic circular dichroism. A relationship of $cf$-hybridization strength and enhanced $T_N$ is discussed. The direction and doping dependence of the circular dichroism is in agreement with strong Kondo screening along the crystallographic $a$ direction.
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The Kondo semiconductor CeOs$_{2}$Al$_{10}$ exhibits an antiferromagnetic (AFM) order at $T_mathrm{N}= 28.5$ K, whose temperature is unexpectedly high for the small ordered moment of $0.3$ $mu_mathrm{B}/$Ce. We have studied the effects of electron- and hole-doping on the hybridization gap and AFM order by measuring the magnetization $M$, magnetic susceptibility $chi$, electrical resistivity $rho$, and specific heat $C$ on single crystals of Ce(Os$_{1-x}$Ir$_{x}$)$_{2}$Al$_{10}$($x le 0.15$) and Ce(Os$_{1-y}$Re$_{y}$)$_{2}$Al$_{10}$($y le 0.1$). The results of $M (B)$ indicates that the AFM ordered moment $mu_mathrm{AF}$ changes the direction from the $c$-axis for $x = 0$ to the $a$-axis for $x = 0.03$. With increasing $x$ up to 0.15, $T_mathrm{N}$ gradually decreases although the $4f$ electron state becomes localized and the magnitude of $mu_mathrm{AF}$ is increased to $1$ $mu_mathrm{B}/$Ce. With increasing $y$, the $4f$ electron state is more delocalized and the AFM order disappears at a small doping level $y = 0.05$. In both electron- and hole-doped systems, the suppression of $T_mathrm{N}$ is well correlated with the increase of the Sommerfeld coefficient $gamma$ in $C(T)$. Furthermore, the simultaneous suppression of $T_mathrm{N}$ and the semiconducting gap in $rho (T)$ at $T > T_mathrm{N}$ indicates that the presence of the hybridization gap is indispensable for the unusual AFM order in CeOs$_{2}$Al$_{10}$.
A Kondo semiconductor CeRu$_2$Al$_{10}$ with an orthorhombic crystal structure shows an unusual antiferromagnetic ordering at rather high temperature $T_0$ of 27.3 K, which is lower than the Kondo temperature $T_{rm K}sim$ 60 K. In optical conductivity [$sigma(omega)$] spectra that directly reflect electronic structure, the $c$-$f$ hybridization gap between the conduction and $4f$ states is observed at around 40 meV along the three principal axes. However, an additional peak at around 20 meV appears only along the $b$ axis. With increasing $x$ to 0.05 in Ce(Ru$_{1-x}$Rh$_x$)$_2$Al$_{10}$, the $T_0$ decreases slightly from 27.3 K to 24 K, but the direction of the magnetic moment changes from the $c$ axis to the $a$ axis. Thereby, the $c$-$f$ hybridization gap in the $sigma(omega)$ spectra is strongly suppressed, but the intensity of the 20-meV peak remains as strong as for $x=0$. These results suggest that the change of the magnetic moment direction originates from the decreasing of the $c$-$f$ hybridization intensity. The magnetic ordering temperature $T_0$ is not directly related to the $c$-$f$ hybridization but is related to the charge excitation at 20 meV observed along the $b$ axis.
An anisotropic Kondo semiconductor CeOs$_2$Al$_{10}$ exhibits an unusual antiferromagnetic order at rather high transition temperature $T_0$ of 28.5 K. Two possible origins of the magnetic order have been proposed so far, one is the Kondo coupling of the hybridization between the conduction ($c$) and the $4f$ states and the other is the charge-density wave/charge ordering along the orthorhombic $b$ axis. To clarify the origin of the magnetic order, we have investigated the electronic structure of hole- and electron-doped CeOs$_2$Al$_{10}$ [Ce(Os$_{1-y}$Re$_y$)$_2$Al$_{10}$ and Ce(Os$_{1-x}$Ir$_x$)$_2$Al$_{10}$, respectively] by using optical conductivity spectra along the $b$ axis. The intensity of the $c$-$f$ hybridization gap at $hbaromegasim50$ meV continuously decreases from $y=0.10$ to $x=0.12$ via $x=y=0$. The intensity of the charge excitation observed at $hbaromegasim20$ meV has the maximum at $x=y=0$ as similar with the doping dependence of $T_{rm 0}$. The fact that the charge excitation is strongly related to the magnetic order strengthens the possibility of the charge density wave/charge ordering as the origin of the magnetic order.
The effects of electron (Ir) and hole (Re) doping on the hybridization gap and antiferromagnetic order have been studied by magnetization, muon spin relaxation ($mu^+$SR), and inelastic neutron scattering on the polycrystalline samples of Ce(Os$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($x$ = 0.08 and 0.15) and CeOs$_{1.94}$Re$_{0.06}$Al$_{10}$. $mu^+$SR spectra clearly reveals magnetic ordering below 20 and 10 K for $x$ = 0.08 and 0.15 samples respectively with a very weak signature of oscillations of the muon initial asymmetry at very short time scale. Our important findings are that small amount of electron doping (i) completely suppress the inelastic magnetic excitations near 11 meV down to 2K, which were observed in the undoped compound, and the response transforms into a broad quasielastic response and (ii) the internal field at the corresponding muon site is remarkably enhanced by about ten times compared with the parent compound. On the other hand with small amount of hole (3% Re) doping the intensity of the inelastic magnetic excitations near 11 meV is reduced significantly. The main origin of the observed doping effect is an extra 5$d$ electrons being carried by Ir and a hole carried by Re compared with that the Os atom. The obtained results demonstrate a great sensitivity of the carrier doping and provides additional ways to study their anomalous magnetic properties.
The orthorhombic compound NdFe$_2$Al$_{10}$ has been studied by powder and single-crystal neutron diffraction. Below $T_N$ = 3.9 K, the Nd$^{3+}$ magnetic moments order in a double-$k$ [$mathbf{k}_1 = (0, frac{3}{4}, 0)$, $mathbf{k}_2 = (0, frac{1}{4}, 0)$] collinear magnetic structure, whose unit cell consists of four orthorhombic units in the $b$ direction.The refinements show that this structure consists of (0 1 0) ferromagnetic planes stacked along $b$, in which the moments are oriented parallel to $a$ (the easy anisotropy axis according to bulk magnetization measurements) and nearly equal in magnitude ($approx 1.7-1.9 mu_B$). The alternating 8-plane sequence providing the best agreement to the data turns out to be that which yields the lowest exchange energy if one assumes antiferromagnetic near-neighbor exchange interactions with $J_1 gg J_2, J_3$. With increasing temperature, the single-crystal measurements indicate the suppression of the $mathbf{k}_2$ component at $T = 2.7$ K, supporting the idea that the anomalies previously observed around 2--2.5 K result from a squaring transition. In a magnetic field applied along the $a$ axis, the magnetic Bragg satellites disappear at $H_c = 2.45$ T, in agreement with earlier measurements. Comparisons are made with related magnetic orders occurring in Ce$T_2$Al$_{10}$ ($T$: Ru, Os) and TbFe$_2$Al$_{10}$.
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