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Register a new userContrasting chemical pressure effect on the moment direction in the Kondo semiconductor CeT$_2$Al$_{10}$ (T = Ru,Os)
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Amitava Bhattacharyya Dr
Publication date
2015
fields
Physics
and research's language is
English
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The opening of a spin gap in the orthorhombic compounds CeT$_2$Al$_{10}$ (T = Ru and Os) is followed by antiferromagnetic ordering at $T_N$ = 27 K and 28.5 K, respectively, with a small ordered moment (0.29$-$0.34$mu_B$) along the $c-$axis, which is not an easy axis of the crystal field (CEF). In order to investigate how the moment direction and the spin gap energy change with 10% La doping in Ce$_{1-x}$La$_x$T$_2$Al$_{10}$ (T = Ru and Os) and also to understand the microscopic nature of the magnetic ground state, we here report on magnetic, transport, and thermal properties, neutron diffraction (ND) and inelastic neutron scattering (INS) investigations on these compounds. Our INS study reveals the persistence of spin gaps of 7 meV and 10 meV in the 10% La-doped T = Ru and Os compounds, respectively. More interestingly our ND study shows a very small ordered moment of 0.18 $mu_B$ along the $b-$axis (moment direction changed compared with the undoped compound), in Ce$_{0.9}$La$_{0.1}$Ru$_2$Al$_{10}$, however a moment of 0.23 $mu_B$ still along the $c-$axis in Ce$_{0.9}$La$_{0.1}$Os$_2$Al$_{10}$. This contrasting behavior can be explained by a different degree of hybridization in CeRu$_2$Al$_{10}$ and CeOs$_2$Al$_{10}$, being stronger in the latter than in the former. Muon spin rotation ($mu$SR) studies on Ce$_{1-x}$La$_x$Ru$_2$Al$_{10}$ ($x$ = 0, 0.3, 0.5 and 0.7), reveal the presence of coherent frequency oscillations indicating a long$-$range magnetically ordered ground state for $x$ = 0 to 0.5, but an almost temperature independent Kubo$-$Toyabe response between 45 mK and 4 K for $x$ = 0.7. We will compare the results of the present investigations with those reported on the electron and hole$-$doping in CeT$_2$Al$_{10}$.
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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 recent discovery of topological Kondo insulating behaviour in strongly correlated electron systems has generated considerable interest in Kondo insulators both experimentally and theoretically. The Kondo semiconductors CeT2Al10 (T=Fe, Ru and Os) possessing a c-f hybridization gap have received considerable attention recently because of the unexpected high magnetic ordering temperature of CeRu2Al10 (TN=27 K) and CeOs2Al10 (TN=28.5 K) and the Kondo insulating behaviour observed in the valence fluctuating compound CeFe2Al10 with a paramagnetic ground state down to 50 mK. We are investigating this family of compounds, both in polycrystalline and single crystal form, using inelastic neutron scattering to understand the role of anisotropic c-f hybridization on the spin gap formation as well as on their magnetic properties. We have observed a clear sign of a spin gap in all three compounds from our polycrystalline study as well as the existence of a spin gap above the magnetic ordering temperature in T=Ru and Os. Our inelastic neutron scattering studies on single crystals of CeRu2Al10 and CeOs2Al10 revealed dispersive gapped spin wave excitations below TN. Analysis of the spin wave spectrum reveals the presence of strong anisotropic exchange, along the c-axis (or z-axis) stronger than in the ab-plane. These anisotropic exchange interactions force the magnetic moment to align along the c-axis, competing with the single ion crystal field anisotropy, which prefers moments along the a-axis. In the paramagnetic state (below 50 K) of the Kondo insulator CeFe2Al10, we have also observed dispersive gapped magnetic excitations which transform into quasi-elastic scattering on heating to 100 K. We will discuss the origin of the anisotropic hybridization gap in CeFe2Al10 based on theoretical models of heavy-fermion semiconductors.
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.
The competition between magnetic ordering and the Kondo effect in Ce2RhSi3, ordering antiferromagnetically at 7 K, is investigated by the measurements of magnetization, heat capacity and electrical resistivity on the solid solutions, Ce(2-x)La(x)RhSi3, Ce(2-y)Y(y)RhSi3, and Ce2RhSi(3-z)Ge(z), as well as by high pressure studies on this compound. The trends in the Kondo and Neel temperature variations among these alloys are compared to infer the roles of unit-cell volume and electronic structure changes. On the basis of the results, we infer that this compound lies at the peak of Doniach-magnetic-phase-diagram. The high pressure electrical resistivity data indicate that the quantum critical point for this compound is in the vicinity of 4 GPa.
The Berry curvature in magnetic systems is attracting interest due to the potential tunability of topological features via the magnetic structure. $f$-electrons, with their large spin-orbit coupling, abundance of non-collinear magnetic structures and high electronic tunability, are attractive candidates to search for tunable topological properties. In this study, we measure anomalous Hall effect (AHE) in the distorted kagom$acute{e}$ heavy fermion antiferromagnet U$_3$Ru$_4$Al$_{12}$. A large intrinsic AHE in high fields reveals the presence of a large Berry curvature. Moreover, the fields required to obtain the large Berry curvature are significantly different between $B parallel a$ and $B parallel a^*$, providing a mechanism to control the topological response in this system. Theoretical calculations illustrate that this sensitivity may be due to the heavy fermion character of the electronic structure. These results shed light on the Berry curvature of a strongly correlated band structure in magnetically frustrated heavy fermion materials, but also emphasize 5$f$-electrons as an ideal playground for studying field-tuned topological states.
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