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Register a new userDoping Effects on the Electronic Structure of an Anisotropic Kondo Semiconductor CeOs$_2$Al$_{10}$: An Optical Study with Re and Ir Substitution
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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.
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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$_{10}$.
Magnetic ground state of Rh-doped Kondo semiconductor CeRu$_2$Al$_{10}$ [Ce(Ru$_{1-x}$Rh$_x$)$_2$Al$_{10}$] is investigated by muon-spin relaxation method. Muon-spin precession with two frequencies is observed in the $x$ = 0 sample, while only one frequency is present in the $x$ = 0.05 and 0.1 samples, which is attributed to the broad static field distribution at the muon site. The internal field at the muon site is enhanced from about 180 G in $x$ = 0 sample to about 800 G in the Rh-doped samples, supporting the spin-flop transition as suggested by macroscopic measurements, and the boundary of different magnetic ground states is identified around $x$ = 0.03. The drastic change of magnetic ground state by a small amount of Rh-doping (3%) indicates that the magnetic structure in CeRu$_2$Al$_{10}$ is not robust and can be easily tuned by external perturbations such as electron doping. The anomalous temperature dependence of internal field in CeRu$_2$Al$_{10}$ is suggested to be attributed to the hyperfine interaction between muons and conduction electrons.
We report temperature-dependent polarized optical conductivity [$sigma(omega)$] spectra of CeFe$_2$Al$_{10}$, which is a reference material for CeRu$_2$Al$_{10}$ and CeOs$_2$Al$_{10}$ with an anomalous magnetic transition at 28 K. The $sigma(omega)$ spectrum along the b-axis differs greatly from that in the $ac$-plane, indicating that this material has an anisotropic electronic structure. At low temperatures, in all axes, a shoulder structure due to the optical transition across the hybridization gap between the conduction band and the localized $4f$ states, namely $c$-$f$ hybridization, appears at 55 meV. However, the gap opening temperature and the temperature of appearance of the quasiparticle Drude weight are strongly anisotropic indicating the anisotropic Kondo temperature. The strong anisotropic nature in both electronic structure and Kondo temperature is considered to be relevant the anomalous magnetic phase transition in CeRu$_2$Al$_{10}$ and CeOs$_2$Al$_{10}$.
We report a systematic study of the $5d$-electron-doped system Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($0 leq x leq 0.15$). With increasing $x$, the orthorhombic $b$~axis decreases slightly while accompanying changes in $a$ and $c$ leave the unit cell volume almost unchanged. Inelastic neutron scattering, along with thermal and transport measurements, reveal that for the Kondo semiconductor CeFe$_2$Al$_{10}$, the low-temperature energy gap which is proposed to be a consequence of strong $c mhyphen f$ hybridization, is suppressed by a small amount of Ir substitution for Fe, and that the system adopts a metallic ground state with an increase in the density of states at the Fermi level. The charge or transport gap collapses (at $x=$~0.04) faster than the spin gap with Ir substitution. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements demonstrate that the system undergoes long-range antiferromagnetic order below a Neel temperature, $T_{mathrm{N}}$, of 3.1(2)~K for $x = 0.15$. The ordered moment is estimated to be smaller than 0.07(1)~$mu_mathrm{B}$/Ce although the trivalent state of Ce is confirmed by Ce L$_3$-edge x-ray absorption near edge spectroscopy. It is suggested that the $c mhyphen f$ hybridization gap, which plays an important role in the unusually high ordering temperatures observed in Ce$T_2$Al$_{10}$ ($T$ = Ru and Os), may not be necessary for the onset of magnetic order with a low $T_{mathrm{N}}$ seen here in Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$.
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.
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