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D. T. Adroja

Publications and source records attributed to D. T. Adroja.

At least 145 records · Page 8Linked to original sources

$μ$SR and inelastic neutron scattering investigations of the noncentrosymmetric antiferromagnet CeNiC$_2$

The magnetic state of the noncentrosymmetric antiferromagnet CeNiC$_2$ has been studied by magnetic susceptibility, heat capacity, muon spin relaxation ($μ$SR) and inelastic neutron scattering (INS) measurements. CeNiC$_2$ exhibits three magnetic phase transitions at $T_{N_1}$ = 20 K, $T_{N_2}$ = 10 K and $T_{N_3}$ = 2.5 K. The presence of long range magnetic order below 20 K is confirmed by the observation of oscillations in the $μ$SR spectra between 10 and 20 K and a sharp increase in the muon depolarization rate. INS studies reveal two well-defined crystal electric field (CEF) excitations around 8 and 30 meV. INS data have been analyzed using a CEF model and the wave functions were evaluated. We also calculated the direction and magnitude of the ground state moment using CEF wave functions and compare the results with that proposed from the neutron diffraction. Our CEF model correctly predicts that the moments order along the $b-$axis (or $y$-axis) and the observed magnetic moment is 0.687(5) $μ_B$, which is higher than the moment observed from the neutron diffraction (0.25 $μ_B$/Ce). We attribute the observed reduced moment due to the Kondo screening effect.

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Investigations of the superconducting states of noncentrosymmetric LaPdSi3 and LaPtSi3

The noncentrosymmetric superconductors LaPdSi3 and LaPtSi3 have been studied with magnetization, specific heat, resistivity and muon spin rotation/relaxation (muSR) measurements. These crystallize in the tetragonal BaNiSn3 structure and superconductivity is observed at Tc = 2.65 K for LaPdSi3 and Tc = 1.52(6) K for LaPtSi3. The results are consistent with both compounds being weakly coupled, fully gapped superconductors but muSR measurements reveal that LaPdSi3 is a bulk type-I superconductor while LaPtSi3 is a type-II material with a Ginzburg-Landau parameter of kappa = 2.49(4). This is further supported by specific heat measurements, where the transition in an applied field is first-order in LaPdSi3 but second-order in LaPtSi3. The electronic specific heat in the superconducting state was analyzed using an isotropic s-wave model that gave Delta/kTc = 1.757(4) for LaPdSi3 and 1.735(5) for LaPtSi3. The temperature dependence of the effective penetration depth of LaPtSi3 was extracted from muSR measurements and was fitted giving Delta/kTc = 1.60(8) and lambda(0) = 239(3) nm. A critical field of Bc(0) = 182.7 G was obtained for LaPdSi3 from muSR measurements, which is in good agreement with the calculated thermodynamic critical field.

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Exotic magnetism on the quasi-FCC lattices of the $d^3$ double perovskites La$_2$NaB$'$O$_6$ (B$'$ $=$ Ru, Os)

We find evidence for long-range and short-range ($ζ$ $=$ 70 Å~at 4 K) incommensurate magnetic order on the quasi-face-centered-cubic (FCC) lattices of the monoclinic double perovskites La$_2$NaRuO$_6$ and La$_2$NaOsO$_6$ respectively. Incommensurate magnetic order on the FCC lattice has not been predicted by mean field theory, but may arise via a delicate balance of inequivalent nearest neighbour and next nearest neighbour exchange interactions. In the Ru system with long-range order, inelastic neutron scattering also reveals a spin gap $Δ$ $\sim$ 2.75 meV. Magnetic anisotropy is generally minimized in the more familiar octahedrally-coordinated $3d^3$ systems, so the large gap observed for La$_2$NaRuO$_6$ may result from the significantly enhanced value of spin-orbit coupling in this $4d^3$ material.

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Magnetic ordering with reduced cerium moments in hole-doped CeOs2Al10

The lightly hole-doped system CeOs1.94Re0.06Al10 has been studied by muon spin relaxation and neutron diffraction measurements. A long-range antiferromagnetic ordering of the Ce-sublattice with substantially reduced value of the magnetic moment 0.18(1) μ_B has been found below T_N = 21 K. Similar to the undoped parent compound, the magnetic ground state of CeOs1.94Re0.06Al10 preserves the anomalous direction of the ordered moments along the c-axis. The obtained result reveals the crucial difference between electron- and hole-doping effects on the magnetic ordering in CeOs2Al10. The former suppresses the anisotropic c-f hybridization and promotes localized Ce moments. On the contrary, the latter increases the hybridization and shifts the system towards delocalized non-magnetic state.

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Crystal field states in a Quantum Spin Ice]{Crystal field states of Pr$^{3+}$ in the candidate quantum spin ice Pr$_{2}$Sn$_{2}$O$_{7}$

Neutron time-of-flight spectroscopy has been employed to study the crystal-field splitting of Pr$^{3+}$ in the pyrochlore stannate Pr$_{2}$Sn$_{2}$O$_{7}$. The crystal field has been parameterized from a profile fit to the observed neutron spectrum. The single-ion ground state is a well isolated non-Kramers doublet of $Γ_3^+$ symmetry with a large Ising-like anisotropy, $χ_{zz} /χ_\perp \approx 60$ at 10 K, but with a significant admixture of terms $| M_J \neq \pm J >$ which can give rise to quantum zero-point fluctuations. This magnetic state satisfies the requirements for quantum spin ice behavior.

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Electron doping evolution of the magnetic excitations in BaFe2-xNixAs2

We use inelastic neutron scattering (INS) spectroscopy to study the magnetic excitations spectra throughout the Brioullion zone in electron-doped iron pnictide superconductors BaFe$_{2-x}$Ni$_{x}$As$_{2}$ with $x=0.096,0.15,0.18$. While the $x=0.096$ sample is near optimal superconductivity with $T_c=20$ K and has coexisting static incommensurate magnetic order, the $x=0.15,0.18$ samples are electron-overdoped with reduced $T_c$ of 14 K and 8 K, respectively, and have no static antiferromagnetic (AF) order. In previous INS work on undoped ($x=0$) and electron optimally doped ($x=0.1$) samples, the effect of electron-doping was found to modify spin waves in the parent compound BaFe$_2$As$_2$ below $\sim$100 meV and induce a neutron spin resonance at the commensurate AF ordering wave vector that couples with superconductivity. While the new data collected on the $x=0.096$ sample confirms the overall features of the earlier work, our careful temperature dependent study of the resonance reveals that the resonance suddenly changes its $Q$-width below $T_c$ similar to that of the optimally hole-doped iron pnictides Ba$_{0.67}$K$_{0.33}$Fe$_2$As$_2$. In addition, we establish the dispersion of the resonance and find it to change from commensurate to transversely incommensurate with increasing energy. Upon further electron-doping to overdoped iron pnictides with $x=0.15$ and 0.18, the resonance becomes weaker and transversely incommensurate at all energies, while spin excitations above $\sim$100 meV are still not much affected. Our absolute spin excitation intensity measurements throughout the Brillouin zone for $x=0.096,0.15,0.18$ confirm the notion that the low-energy spin excitation coupling with itinerant electron is important for superconductivity in these materials, even though the high-energy spin excitations are weakly doping dependent.

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Neutron scattering and muon spin relaxation measurements of the non-centrosymmetric antiferromagnet CeCoGe3

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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The Hour-Glass Magnetic Spectrum Arising from a Striped, Cluster Spin Glass Ground State in La1.75Sr0.25CoO4

We report inelastic neutron scattering results that reveal an hour-glass magnetic excitation spectrum in La1.75Sr0.25CoO4. The magnetic spectrum is similar to that observed previously in La1.67Sr0.33CoO4, but the spectral features are broader. We show that the spectrum of La1.75Sr0.25CoO4 can be modeled by the spin dynamics of a system with a disordered cluster spin glass ground state. Bulk magnetization measurements are presented which support the proposed glassy ground state. The observations reiterate the importance of quasi-one-dimensional magnetic correlations and disorder for the hour-glass spectrum, and suggest that disordered spin and charge stripes exist at lower doping in La2-xSrxCoO4 than previously thought.

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Negative magnetostrictive magnetoelectric coupling of BiFeO3

How the magnetoelectric coupling actually occurs on a microscopic level in multiferroic BiFeO3 is not well known. By using the high-resolution single crystal neutron diffraction techniques, we have determined the electric polarization of each individual elements of BiFeO3, and concluded that the magnetostrictive coupling suppresses the electric polarization at the Fe site below TN. This negative magnetoelectric coupling appears to outweigh the spin current contributions arising from the cycloid spin structure, which should produce a positive magnetoelectric coupling.

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Change of magnetic ground state by light electron-doping in CeOs2Al10

The effect of Ir substitution for Os in CeOs2Al10, with an unusually high Neel temperature of T~28.5K, has been studied by high-resolution neutron diffraction and magnetization measurements. A small amount of Ir (~ 8%) results in a pronounced change of the magnetic structure of the Ce-sublattice. The new magnetic ground state is controlled by the single ion anisotropy and implies antiferromagnetic arrangement of the Ce-moments along the a-axis, as expected from the anisotropy of the paramagnetic susceptibility. The value of the ordered moments, 0.92(1) mu_B, is substantially bigger than in the undoped compound, whereas the transition temperature is reduced down to 21K. A comparison of the observed phenomena with the recently studied CeRu1.9Rh0.1Al10 system, exhibiting similar behaviour [A. Kondo et al., J. Phys. Soc. Jpn. 82, 054709 (2013)], strongly suggests the electron doping as the main origin of the ground state changes. This provides a new way of exploring the anomalous magnetic properties of the Ce(Ru/Os)2Al10 compounds.

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Competing 4f-electron dynamics in Ce(Ru1-xFex)2Al10 (x=0 to 1): magnetic ordering emerging from the Kondo semiconducting state

We have carried out muon spin relaxation (muSR), neutron diffraction and inelastic neutron scattering (INS) investigations on polycrystalline samples of Ce(Ru1-xFex)2Al10 (x=0, 0.3, 0.5, 0.8 and 1) to investigate the nature of the ground state (magnetic ordered versus paramagnetic) and the origin of the spin gap formation as evident from the bulk measurements in the end members. Our zero-field muSR spectra clearly reveal coherent two-frequency oscillations at low temperature in x=0, 0.3 and 0.5 samples, which confirms the long-range magnetic ordering of the Ce-moment with TN=27, 26 and 21 K respectively. On the other hand the muSR spectra of x=0.8 and x=1 down to 1.4 K and 0.045 K, respectively exhibit a temperature independent Kubo-Toyabe term confirming a paramagnetic ground state. The long-range magnetic ordering in x=0.5 below 21 K has been confirmed through the neutron diffraction study. INS measurements of x=0 clearly reveal the presence of a sharp inelastic excitation near 8 meV between 5 K and 26 K, due to an opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. Interestingly, at 4.5 K the spin gap excitation broadens in x=0.3 and exhibits two clear peaks at 8.4(3) and 12.0(5) meV in x=0.5. In the x=0.8 sample, which remains paramagnetic down to 1.2 K, there is a clear signature of a spin gap of 10-12 meV at 7 K, with a strong Q-dependent intensity. Evidence of a spin gap of 12.5(5) meV has also been found in x=1. The observation of a spin gap in the paramagnetic samples (x=0.8 and 1) is an interesting finding in this study and it challenges our understanding of the origin of the semiconducting gap in CeT2Al10 (T=Ru and Os) compounds in terms of hybridization gap opening only a small part of the Fermi surface, gapped spin waves, or a spin-dimer gap.

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Another dimension: investigations of molecular magnetism using muon-spin relaxation

We review examples of muon-spin relaxation measurements on molecule-based magnetic coordination polymers, classified by their magnetic dimensionality. These include the one-dimensional s=1/2 spin chain Cu(pyz)(NO3)2 and the two-dimensional s=1/2 layered material [Cu(HF2)(pyz)2]BF4. We also describe some of the more exotic ground states that may become accessible in the future given the ability to tune the interaction strengths of our materials through crystal engineering.

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Field-induced long-range magnetic order in the spin-singlet ground state system YbAl3C3: Neutron diffraction study

The $4f$-electron system YbAl$_3$C$_3$ with a non-magnetic spin-dimer ground state has been studied by neutron diffraction in an applied magnetic field. A long-range magnetic order involving both ferromagnetic and antiferromagnetic components has been revealed above the critical field H$_C\sim $ 6T at temperature T=0.05K. The magnetic structure indicates that the geometrical frustration of the prototype hexagonal lattice is not fully relieved in the low-temperature orthorhombic phase. The suppression of magnetic ordering by the remanent frustration is the key factor stabilizing the non-magnetic singlet ground state in zero field. Temperature dependent measurements in the applied field H=12T revealed that the long-range ordering persists up to temperatures significantly higher than the spin gap indicating that this phase is not directly related to the singlet-triplet excitation. Combining our neutron diffraction results with the previously published phase diagram, we support the existence of an intermediate disordered phase as the first excitation from the non-magnetic singlet ground state. Based on our results, we propose YbAl$_3$C$_3$ as a new material for studying the quantum phase transitions of heavy-fermion metals under the influence of geometrical frustration.

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Electron doping evolution of the anisotropic spin excitations in BaFe2-xNixAs2

We use inelastic neutron scattering to systematically investigate the Ni-doping evolution of the low-energy spin excitations in BaFe2-xNixAs2 spanning from underdoped antiferromagnet to overdoped superconductor (0.03< x < 0.18). In the undoped state, the low-energy (<80 meV) spin waves of BaFe2As2 form transversely elongated ellipses in the [H, K] plane of the reciprocal space. Upon Ni-doping, the c-axis magnetic exchange coupling is rapidly suppressed and the momentum distribution of spin excitations in the [H, K] plane is enlarged in both the transverse and longitudinal directions with respect to the in-plane AF ordering wave vector of the parent compound. As a function of increasing Ni-doping x, the spin excitation widths increase linearly but with a larger rate along the transverse direction. These results are in general agreement with calculations of dynamic susceptibility based on the random phase approximation (RPA) in an itinerant electron picture. For samples near optimal superconductivity at x= 0.1, a neutron spin resonance appears in the superconducting state. Upon further increasing the electron-doping to decrease the superconducting transition temperature Tc, the intensity of the low-energy magnetic scattering decreases and vanishes concurrently with vanishing superconductivity in the overdoped side of the superconducting dome. Comparing with the low-energy spin excitations centered at commensurate AF positions for underdoped and optimally doped materials (x<0.1), spin excitations in the over-doped side (x=0.15) form transversely incommensurate spin excitations, consistent with the RPA calculation. Therefore, the itinerant electron approach provides a reasonable description to the low-energy AF spin excitations in BaFe2-xNixAs2.

cond-mat.supr-con↗

Magnetic and transport properties of Pr2Pt3Si5

We have investigated the magnetic and transport properties of a polycrystalline Pr2Pt3Si5 sample through the dc and ac magnetic susceptibilities, electrical resistivity, and specific heat measurements. The Rietveld refinement of the powder X-ray diffraction data reveals that Pr2Pt3Si5 crystallizes in the U2Co3Si5-type orthorhombic structure (space group Ibam). Both the dc and ac magnetic susceptibility data measured at low fields exhibit sharp anomaly near 15 K. In contrast, the specific heat data exhibit only a broad anomaly implying no long range magnetic order down to 2 K. The broad Schottky-type anomaly in low temperature specific heat data is interpreted in terms of crystal electric field (CEF) effect, and a CEF-split singlet ground state is inferred. The absence of the long range order is attributed to the presence of nonmagnetic singlet ground state of the Pr3+ ion. The electrical resistivity data exhibit metallic behavior and are well described by the Bloch-Grüniesen-Mott relation.

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Evolution of quantum criticality in the system CeNi9Ge4

The heavy fermion system CeNi9Ge4 exhibits a paramagnetic ground state with remarkable features such as: a record value of the electronic specific heat coefficient in systems with a paramagnetic ground state, γ= C/T \simeq 5.5 J/molK^2 at 80 mK, a temperature-dependent Sommerfeld-Wilson ratio, R=χ/γ, below 1 K and an approximate single ion scaling of the 4f-magnetic specific heat and susceptibility. These features are related to a rather small Kondo energy scale of a few Kelvin in combination with a quasi-quartet crystal field ground state. Tuning the system towards long range magnetic order is accomplished by replacing a few at.% of Ni by Cu or Co. Specific heat, susceptibility and resistivity studies reveal T_N \sim 0.2 K for CeNi8CuGe4 and T_N \sim 1 K for CeNi8CoGe4. To gain insight whether the transition from the paramagnetic NFL state to the magnetically ordered ground state is connected with a heavy fermion quantum critical point we performed specific heat and ac susceptibility studies and utilized the μSR technique and quasi-elastic neutron scattering.

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Muon spin relaxation and neutron diffraction investigations of quadrupolar and magnetically ordered states of YbRu2Ge2

The magnetic and quadrupolar ordered states of polycrystalline YbRu2Ge2 have been investigated using zero-field muon spin relaxation (μSR) and neutron diffraction measurements. Specific heat measurements show three successive phase transitions, with decreasing temperature from a paramagnetic to a quadrupolar state at T0 ~ 10 K, from the quadrupolar to a magnetic state at T1 ~ 6.5 K and a possible change in the magnetic ground state at T2 ~ 5.5 K. Clear evidence for the magnetic transition below 7 K (spectrum at 8 K reveals paramagnetic state) and a likely change in the magnetic structure near 5.8 K is observed in the zero-field μSR measurements. The μSR data, however, do not reveal any signature of magnetic order in the temperature range 8 - 45 K. This result is further supported by neutron diffraction measurements, where clear magnetic Bragg peaks have been observed below 8 K, but not above it. Below 8 K, the magnetic Bragg peaks can be characterized by an incommensurate antiferromagnetic ordering with the propagation vector q = [0.352, 0, 0] and the magnetic moment 2.9(3) μB of Yb along the b-axis. These results are discussed in terms of quadrupolar ordered and magnetically ordered states.

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Molecular spin-orbit excitations in the J_eff = 1/2 frustrated spinel GeCo$_2$O$_4$

We describe powder and single-crystal inelastic neutron scattering experiments on a spinel-type antiferromagnet GeCo$_2$O$_4$, represented by an effective total angular momentum J_eff = 1/2. Several types of non-dispersive short-range magnetic excitations were discovered. The scattering intensity maps in $\vec{Q}$ space are well reproduced by dynamical structure factor analyses using molecular model Hamiltonians. The results of analyses strongly suggest that the molecular excitations below T_N arise from a hidden molecular-singlet ground state, in which ferromagnetic subunits are antiferromagnetically coupled. The quasielastic excitations above T_N are interpreted as its precursor. A combination of frustration and J_eff = 1/2 might induce these quantum phenomena.

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