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H. Alloul

Publications and source records attributed to H. Alloul.

At least 37 records · Page 2Linked to original sources

Incidence of the Tomonaga-Luttinger liquid state on the NMR spin lattice relaxation in Carbon Nanotubes

We report 13C nuclear magnetic resonance measurements on single wall carbon nanotube (SWCNT) bundles. The temperature dependence of the nuclear spin-lattice relaxation rate, 1/T1, exhibits a power-law variation, as expected for a Tomonage-Luttinger liquid (TLL). The observed exponent is smaller than that expected for the two band TLL model. A departure from the power law is observed only at low T, where thermal and electronic Zeeman energy merge. Extrapolation to zero magnetic field indicates gapless spin excitations. The wide T range on which power-law behavior is observed suggests that SWCNT is so far the best realization of a one-dimensional quantum metal.

cond-mat.str-el↗

Phase segregation in NaxCoO2 for large Na contents

We have investigated a set of sodium cobaltates (NaxCoO2) samples with various sodium content (0.67 \le x \le 0.75) using Nuclear Quadrupole Resonance (NQR). The four different stable phases and an intermediate one have been recognized. The NQR spectra of 59Co allowed us to clearly differentiate the pure phase samples which could be easily distinguished from multi-phase samples. Moreover, we have found that keeping samples at room temperature in contact with humid air leads to destruction of the phase purity and loss of sodium content. The high sodium content sample evolves progressively into a mixture of the detected stable phases until it reaches the x=2/3 composition which appears to be the most stable phase in this part of phase diagram.

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Hall effect and resistivity study of the magnetic transition, carrier content and Fermi liquid behavior in Ba(Fe(1-x) Cox)2As2

The negative Hall constant R_H measured all over the phase diagram of Ba(Fe(1-x)Cox)2As2 allows us to show that electron carriers always dominate the transport properties. The evolution of R_H with x at low doping (x<2%) indicates that important band structure changes happen for x<2% prior to the emergence of superconductivity. For higher x, an change of the electron concentration with T is required to explain the low T variations of R_H, while the electron scattering rate displays the T^2 law expected for a Fermi liquid. The T=0 residual scattering is affected by Co disorder in the magnetic phase, but is rather dominated by incipient disorder in the paramagnetic state.

cond-mat.supr-con↗

NQR and X-ray investigation of the structure of Na$_{2/3}$CoO$_{2}$ compound

We have synthesized various samples of the $x=2/3$ phase of sodium cobaltate Na$_{x}$CoO$_{2}$ and performed X-ray powder diffractions spectra to compare the diffraction with the structure proposed previously from NMR/NQR experiments [H. Alloul \emph{et al.}, EPL \textbf{85}, 47006 (2009)]. Rietveld analysis of the data are found in perfect agreement with those, and confirm the concentration x=2/3 obtained in the synthesis procedure. They even give indications on the atomic displacements of Na inside the unit cell. The detailed NQR data allow us to identify the NQR transitions and electric field gradient (EFG) parameters for 4 cobalt sites and 3 Na sites. The spin-lattice and spin-spin relaxation rates are found much smaller for the non-magnetic Co$^{3+}$ sites than for the magnetic sites on which the holes are delocalized. The atomic ordering of the Na layers is therefore at the source of this ordered distribution of cobalt charges. The method used here to resolve the Na ordering and the subsequent Co charge order can be used valuably for other concentrations of Na.

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Na ordering imprints a metallic kagome lattice onto the Co planes of Na2/3CoO2

We report $^{23}$Na and $^{59}$Co nuclear magnetic (NMR) and quadrupolar resonance (NQR) studies for the $x=2/3$ phase of the lamellar oxide Na$_{x}$CoO$_{2}$, which allowed us to establish reliably the atomic order of the Na layers and their stacking between the CoO$_{2}$ slabs. We evidence that the Na$^{+}$ order stabilizes filled non magnetic Co$^{3+}$ ions on 25% of the cobalt sites arranged in a triangular sublattice. The transferred holes are delocalized on the 75% complementary cobalt sites which unexpectedly display a planar cobalt kagomé structure. These experimental results resolve a puzzling issue by precluding localized moments pictures for the magnetic properties. They establish that the quasi ferromagnetic properties result from a narrow band connecting a frustrated arrangement of atomic orbitals, and open the route to unravel through similar studies the electronic properties of the diverse ordered phases of sodium cobaltates.

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Spin correlations and cobalt charge states: A new phase diagram of sodium cobaltates

Using 23Na NMR measurements on sodium cobaltates at intermediate dopings (0.44<=x<=0.62), we establish the qualitative change of behavior of the local magnetic susceptibility at x*=0.63-0.65, from a low x Pauli-like regime to the high x Curie-Weiss regime. For 0.5<=x<=0.62, the presence of a maximum T* in the temperature dependence of the susceptibility shows the existence of an x-dependent energy scale. T_1 relaxation measurements establish the predominantly antiferromagnetic character of spin correlations for x x*. It is suggested that at a given x the ferromagnetic correlations might dominate the antiferromagnetic ones above T*. From 59Co NMR data, it is shown that moving towards higher x away from x=0.5 results in the progressive appearance of nonmagnetic Co3+ sites, breaking the homogeneity of Co states encountered for x<=0.5. The main features of the NMR-detected 59Co quadrupolar effects, together with indications from the powder x-ray diffraction data, lead us to sketch a possible structural origin for the Co3+ sites. In light of this ensemble of new experimental observations, a new phase diagram is proposed, taking into account the systematic presence of correlations and their x-dependence.

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Na atomic order, Co charge disproportionation and magnetism in Na$_{x}$CoO$_{2}$ for large Na contents

We have synthesized and characterized four different stable phases of Na ordered Na$_{x}$CoO$_{2}$, for $0.65<x<0.8$. Above 100 K they display similar Curie-Weiss susceptibilities as well as ferromagnetic $q=0$ spin fluctuations in the CoO$_{2}$ planes revealed by $^{23}$Na NMR data. In all phases from $^{59}$Co NMR data we display evidences that the Co disproportionate already above 300 K into non magnetic Co$^{3+}$ and magnetic $\approx $Co$^{3.5+}$ sites on which holes delocalize. This allows us to understand that metallic magnetism is favored for these large Na contents. Below 100 K the phases differentiate, and a magnetic order sets in only for $x\gtrsim 0.75$ at $T_{N}=$22 K. We suggest that the charge order also governs the low $T$ energy scales and transverse couplings.

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Disorder, Metal-Insulator crossover and Phase diagram in high-Tc cuprates

We have studied the influence of disorder induced by electron irradiation on the normal state resistivities $ρ(T)$ of optimally and underdoped YBa2CuOx single crystals, using pulsed magnetic fields up to 60T to completely restore the normal state. We evidence that point defect disorder induces low T upturns of rho(T) which saturate in some cases at low T in large applied fields as would be expected for a Kondo-like magnetic response. Moreover the magnitude of the upturns is related to the residual resistivity, that is to the concentration of defects and/or their nanoscale morphology. These upturns are found quantitatively identical to those reported in lower Tc cuprates, which establishes the importance of disorder in these supposedly pure compounds. We therefore propose a realistic phase diagram of the cuprates, including disorder, in which the superconducting state might reach the antiferromagnetic phase in the clean limit.

cond-mat.supr-con↗

Defects in correlated metals and superconductors

In materials with strong local Coulomb interactions, simple defects such as atomic substitutions strongly affect both macroscopic and local properties of the system. A nonmagnetic impurity, for instance, is seen to induce magnetism nearby. Even without disorder, models of such correlated systems are generally not soluble in 2 or 3 dimensions, and so few exact results are known for the properties of such impurities. Nevertheless, some simple physical ideas have emerged from experiments and approximate theories. Here, we first review what we can learn about this problem from 1D antiferromagnetically correlated systems. We then discuss experiments on the high Tc cuprate normal state which probe the effect of impurities on local charge and spin degrees of freedom, and compare with theories of single impurities in correlated hosts, as well as phenomenological effective Kondo descriptions. Subsequently, we review theories of impurities in d-wave superconductors including residual quasiparticle interactions, and compare with experiments in the superconducting state. We argue that existing data exhibit a remarkable similarity to impurity-induced magnetism in the 1D case, implying the importance of electronic correlations for the understanding of these phenomena, and suggesting that impurities may provide excellent probes of the still poorly understood ground state of the cuprates.

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Influence of charge order on the magnetic properties of Na$_{x}$CoO$_{2}$ for $x>0.65$

We have synthesized and characterized the four different stable phases of Na ordered Na$_{x}$CoO$_{2}$, for $0.65<x\lesssim 0.75$. Above 100K they display similar Curie-Weiss spin susceptibilities as well as ferromagnetic $q=0$ spin fluctuations in the CoO$_{2}$ planes revealed respectively by $^{23}$Na NMR shift and spin lattice $T_{1}$ data. The Co disproportionate already above 300K into Co$^{3+}$ and $\approx $Co$^{3.5+}$ in all phases, which allows us to understand that magnetism is favoured. Below 100K the paramagnetic properties become quite distinct, and a 3D magnetic order sets in only for $x=0.75$, so that charge order has a subtle incidence on the low $T$ energy scales and transverse magnetic couplings.

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Total suppression of superconductivity by high magnetic fields in YBa2 Cu3O6.6

We have studied in fields up to 60T the variation of the transverse magnetoresistance (MR) of underdoped YBCO6.6 crystals either pure or with Tc reduced down to 3.5K by electron irradiation. We evidence that the normal state MR is restored above a threshold field H'c(T), which is found to vanish at T'c>>Tc. In the pure YBCO6.6 sample a 50 Tesla field is already required to completely suppress the superconducting fluctuations at Tc. While disorder does not depress the pseudogap temperature, it reduces drastically the phase coherence established at Tc and weakly H'c(0), T'c and the onset Tnu of the Nernst signal which are more characteristic of the 2D local pairing.

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NMR study of the magnetic and metal-insulator transitions in Na0.5CoO2: a nesting scenario

Co and Na NMR are used to probe the local susceptibility and charge state of the two Co sites of the Na-ordered orthorhombic Na0.5CoO2. Above T_N=86K, both sites display a similar T-dependence of the spin shift, suggesting that there is no charge segregation into Co3+ and Co4+ sites. Below T_N, the magnetic long range commensurate order found is only slightly affected by the metal-insulator transition (MIT) at T_MIT=51K. Furthermore, the electric field gradient at the Co site does not change at these transitions, indicating the absence of charge ordering. All these observations can be explained by successive SDW induced by two nestings of the Fermi Surface specific to the x=0.5 Na-ordering.

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Impurity induced Local Magnetism and Density of States in the superconducting state of YBa2Cu3O7

Oxygen NMR is used to probe the local influence of nonmagnetic Zn and magnetic Ni impurities in the superconducting state of optimally doped high Tc YBa2Cu3O7. Zn and Ni induce a staggered paramagnetic polarization, similar to that evidenced above Tc, with a typical extension xi=3 cell units for Zn and xi>=3 for Ni. In addition, Zn is observed to induce a local density of states near the Fermi Energy in its neighbourhood, which also decays over about 3 cell units. Its magnitude decreases sharply with increasing temperature. This allows direct comparison with the STM observations done in BiSCO.

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Nernst effect and disorder in the normal state of high-T_{c} cuprates

We have studied the influence of disorder induced by electron irradiation on the Nernst effect in optimally and underdoped YBa2Cu3O(7-d) single crystals. The fluctuation regime above T_{c} expands significantly with disorder, indicating that the T_{c} decrease is partly due to the induced loss of phase coherence. In pure crystals the temperature extension of the Nernst signal is found to be narrow whatever the hole doping, contrary to data reported in the low-T_{c} cuprates families. Our results show that the presence of "intrinsic" disorder can explain the enhanced range of Nernst signal found in the pseudogap phase of the latter compounds.

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NMR Evidence for Gapped Spin Excitations in Metallic Carbon Nanotubes

We report on the spin dynamics of 13C isotope enriched inner-walls in double-wall carbon nanotubes (DWCNT) using 13C nuclear magnetic resonance (NMR). Contrary to expectations, we find that our data set implies that the spin-lattice relaxation time (T1) has the same temperature (T) and magnetic field (H) dependence for most of the innerwall nanotubes detected by NMR. In the high temperature regime (T > 150 K), we find that the T and H dependence of 1/T1T is consistent with a 1D metallic chain. For T < 150 K, we find a significant increase in 1/T1T with decreasing T, followed by a sharp drop below 20 K. The data clearly indicates the formation of a gap in the spin excitation spectrum, where the gap value 2 Delta = 40 K (= 3.7 meV) is H independent.

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Evidence of a single nonmagnetic Co3+ state in the Na1CoO2 cobaltate

Macroscopic magnetization, muon spin rotation (muSR), and NMR measurements were carried out to study magnetism in the Na1CoO2 cobaltate. Using SQUID measurements, Na1CoO2 is shown to have a bulk magnetic susceptibility much lower and flatter than that of NaxCoO2 with x=0.7-0.9. In fact, muSR yields a signal of mostly nonmagnetic origin, which is attributed to the x=1 phase. The intrinsic cobalt spin susceptibility corresponding to this x=1 phase is measured using Na NMR. It is indeed found to be almost zero, in agreement with a low-spin 3+ charge state of all cobalt atoms. This single state of Co ions in CoO2 planes is confirmed by Co NMR, whose determination of cobalt shift and quadrupolar parameters allows us to give a reference value of the Co3+ orbital shift in cobaltates.

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59Co NMR study of the Co states in superconducting and anhydrous cobaltates

$^{59}$Co NMR spectra in oriented powders of Na$_{0.35}$CoO$_{2}$ and in its hydrated superconducting phase (HSC) Na$_{0.35}$CoO$_{2}$,1.3H$_{2}$O reveal a single electronic Co state with identical $T$ independent NMR shift tensor. These phases differ markedly from Na$_{0.7}$CoO$_{2}$, in which we resolve 3 types of Co sites. The large T variation of their spin susceptibilities $χ^{s}$ and the anisotropy of the orbital susceptibility $χ^{orb}$ allow us to conclude that charge disproportionation occurs, in a non magnetic Co$^{3+}$ and two magnetic sites with about 0.3 and 0.7 holes in the $t_{2g}$ multiplet. The data are consistent with those for the single Co site in the anhydrous and HSC phase assuming the expected Co$^{3.65+}$ charge.

cond-mat.supr-con↗

Series of Bulk Magnetic Phase Transitions in NaxCoO2: a muSR study

Using muon spin rotation, well-defined bulk ~ 100% magnetic phases in NaxCoO2 are revealed. A novel magnetic phase is detected for x = 0.85 with the highest transition temperature ever observed for x >= 0.75. This stresses the diversity of x >=0.75 magnetic phases and the link between magnetic and structural degrees of freedom. For the charge-ordered x = 0.50 compound, a cascade of transitions is observed below 85 K. From a detailed analysis of our data, we conclude that the ordered moment varies continuously with temperature and suggest that the two secondary transitions at 48 K and 29 K correspond to a moderate reorientation of antiferromagnetically coupled moments.

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