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Contrasting electron and hole doping effects on the spin gap of the caged type Kondo semimetal CeOs$_2$Al$_{10}$: A muon spin relaxation and inelastic neutron scattering investigation

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 Publication date 2014
  fields Physics
and research's language is English




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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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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$_{10}$.
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.
Nd2Hf2O7, belonging to the family of geometrically frustrated cubic rare earth pyrochlore oxides, was recently identified to order antiferromagnetically below T_N = 0.55 K with an all-in/all-out arrangement of Nd3+ moments, however with a much reduced ordered state moment. Herein we investigate the spin dynamics and crystal field states of Nd2Hf2O7 using muon spin relaxation (muSR) and inelastic neutron scattering (INS) measurements. Our muSR study confirms the long range magnetic ordering and shows evidence for coexisting persistent dynamic spin fluctuations deep inside the ordered state down to 42 mK. The INS data show the crytal electric field (CEF) excitations due to the transitions both within the ground state multiplet and to the first excited state multiplet. The INS data are analyzed by a model based on CEF and crystal field states are determined. Strong Ising-type anisotropy is inferred from the ground state wavefunction. The CEF parameters indicate the CEF-split Kramers doublet ground state of Nd3+ to be consistent with the dipolar-octupolar character.
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.
The magnetic states of the non-centrosymmetric, pressure induced superconductor CeCoGe3 have been studied with magnetic susceptibility, muon spin relaxation(muSR), single crystal neutron diffraction and inelastic neutron scattering (INS). CeCoGe3 exhibits three magnetic phase transitions at T_N1 = 21 K, T_N2 = 12 K and T_N3 = 8 K. The presence of long range magnetic order below T_N1 is revealed by the observation of oscillations of the asymmetry in the muSR spectra between 13 K and 20 K and a sharp increase in the muon depolarization rate. Single crystal neutron diffraction measurements reveal magnetic Bragg peaks consistent with propagation vectors of k = 2/3 between T_N1 and T_N2, k = 5/8between T_N2 and T_N3 and k = 1/2 below T_N3. An increase in intensity of the (1 1 0) reflection between T_N1 and T_N3 also indicates a ferromagnetic component in these phases. These measurements are consistent with an equal moment, two-up, two-down magnetic structure below T_N3, with a magnetic moment of 0.405(5) mu_B/Ce. Above T_N2, the results are consistent with an equal moment, two-up, one-down structure with a moment of 0.360(6) mu_B/Ce. INS studies reveal two crystal-field (CEF) excitations at 19 and 27 meV. From an analysis with a CEF model, the wave-functions of the J = 5/2 multiplet are evaluated along with a prediction for the magnitude and direction of the ground state magnetic moment. Our model correctly predicts that the moments order along the c axis but the observed magnetic moment of 0.405(5) mu_B is reduced compared to the predicted moment of 1.01 mu_B. This is ascribed to hybridization between the localized Ce^3+ f-electrons and the conduction band. This suggests that CeCoGe3 has a degree of hybridization between that of CeRhGe3 and the non-centrosymmetric superconductor CeRhSi3.
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