Study of : pronounced differences between the and ground states

We present electrical resistivity and specific heat measurements of alloys on the Rh rich side of the phase diagram of the Ce(Rh_1-xPd_x)₂Si₂ system. We compare these results with those obtained at intermediate and low Rh concentrations. The analysis of the concentration and temperature dependence of the entropy and of the scaling behaviour of C _el ( T ) and ρ( T ) clearly confirm a separation of the magnetic phase diagram into two regions: the region x ≤0.3, showing a concentration independent characteristic temperature for the 4 f-electrons with T ₀ ≈ 45 K, while for x > 0.3, T₀ decreases to T ₀ ( x = 1) ≈ 15 K. At low Pd-content, T_N decreases very rapidly from T _N = 36 K in pure CeRh₂Si₂ to T _N = 18 K at x = 0.1. With higher Pd concentration T_N stabilizes at T _N ≈ 15 K whereas the magnitude of the anomalies in C _el ( T ) and in the susceptibility around T_N are further reduced and disappear at x ≈ 0.3. This differs from the behavior found on the Pd-rich side, where T_N decreases continuously to zero with increasing Rh content. The pronounced differences observed between both phase boundaries and the drastic effect of doping on the Rh rich side suggest an itinerant character in CeRh₂ Si₂, in contrast with the localized character of CePd₂Si₂. Further evidence for the itinerant character of CeRh₂Si₂ is given by the ρ( T ) dependence observed for x ≤0.3, which scales with ρ( T ) of the prototype itinerant compound YCo₂. Received 31 December 2001 / Received in final form 6 July 2002 Published online 19 December 2002 RID="a" ID="a"e-mail: berisso@cab.cnea.gov.ar     

Moment-volume instabilities in alloys with compositions around the C14 laves phase

We measured the thermal expansion and the specific heat of Ti_xFe_100-x alloys with x = 30.5, 32.5 and 35, all with hexagonal C14 laves phase structure (MgZn₂) like TiFe₂, and determine the temperature dependence of the magnetic contributions to the thermal expansion and the specific heat c_mag. For fixed composition and c mag ( T ) show the same type of behavior, demonstrating that both anomalies are of the same microscopic nature. They originate from moment-volume fluctuations (antiferromagnetic Invar-effect) as a comparison with total energy calculations as a function of atomic volume and moment for TiFe₂ reveals. Received: 26 January 1998 / Accepted: 17 April 1998     

Low temperature Kondo reduction of quadrupolar and magnetic moments in the YbCuAl series

We present measurements in the YbCu_5-xAl_x series, down to the 50 mK range, using ¹⁷⁰Yb M?ssbauer absorption spectroscopy and magnetisation measurements. In this series, the hybridisation between the Yb 4 f electrons and the conduction electrons is known to decrease as the Al content x increases. We apply the variational solution of the impurity Kondo problem to the interpretation of our data. We show that the Kondo temperature can be derived from the measured 4 f quadrupole moment and, for the magnetically ordered compounds (), we obtain the exchange energy as a function of the Al content. Our findings are in general agreement with Doniach's model describing the onset of magnetic ordering according to the relative values of the Kondo and exchange energy scales. Received 16 April 1998     

Ground-state properties of LiV2O4 and Li1-xZnx(V1-yTiy)2O4

We present susceptibility, microwave resistivity, NMR and heat-capacity results for Li_1-xZn_x(V_1-yTi_y)₂O₄ with 0 ? x ? 0.3 and 0 ? y ? 0.3. For all doping levels the susceptibility curves can be fitted with a Curie-Weiss law. The paramagnetic Curie-Weiss temperatures remain negative with an average value close to that of the pure compound Θ≈ - 36 K. Spin-glass anomalies are observed in the susceptibility, heat-capacity and NMR measurements for both type of dopants. From the temperature dependence of the spin-lattice relaxation rate we found critical-dynamic behavior in the Zn doped compounds at the freezing temperatures. For the Ti-doped samples two successive freezing transitions into disordered low-temperature states can be detected. The temperature dependence of the heat capacity for Zn-doped compounds does not resemble that of canonical spin glasses and only a small fraction of the total vanadium entropy is frozen at the spin-glass transitions. For pure LiV₂O₄ the spin-glass transition is completely suppressed. The temperature dependence of the heat capacity for LiV₂O₄ can be described using a nuclear Schottky contribution and the non-Fermi liquid model, appropriate for a system close to a spin-glass quantum critical point. Finally an ( x / y , T )-phase diagram for the low-doping regime is presented. Received 16 March 2001 and Received in final form 30 October 2001     

Relationship between resistivity and specific heat in a canonical non-magnetic heavy fermion alloy system: UPt5-xAu x

A comprehensive study of the relationship between the electronic specific heat coefficient () and the temperature square coefficient (A) of the electrical resistivity for a single, cubic, heavy fermion alloy system, UPt_5-xAu_x is presented. In this alloy system, whose low temperature properties are consistent with the Fermi-liquid behavior, varies by more than a factor of 10 while the corresponding A coefficient changes by a factor larger than 200. A tracks changes in fairly well, but , postulated to have a universal value for heavy fermions, is not constant and varies from about 10^-6 (x = 0, 0.5) to 10^-5 cm (mol K/mJ)² (x > 1.1), thus from a value typical of transition metals to that characteristic of other heavy fermion compounds. We have found a correlation between and magnetic characteristics such as the paramagnetic Curie-Weiss temperature and the low temperature magnetic susceptibility divided by . Received 29 January 1999     

On the 240 K anomaly in the magnetic properties of LiNiO2

In this work, results of X-band ESR spectroscopy, ac-magnetic susceptibility and X-ray powder diffraction measurements on Li_1-xNi _1+x O₂ (x = 0.02 and x = 0.07) are presented and discussed. While the susceptibility of the compound with x = 0.02 is shown to follow a Curie-Weiss law, with a Weiss temperature of the order of 30 K, the compound with x = 0.07 is found to order ferromagnetically below K. However, an additional anomaly is observed in the magnetic properties of this latter compound at around 240 K. We attribute this anomaly to the presence of macroscopic Ni-rich regions which order ferrimagnetically below this temperature. This phenomenon is different from the bulk ferromagnetism that occurs at much lower temperatures, and allows us to discard earlier suggestions proposed in the literature in which the 240 K anomaly has been considered as denoting an intrinsic phenomenon. Received 14 May 1999 and Received in final form 5 August 1999     

Thermodynamic properties of the spin-1/2 antiferromagnetic ladder under magnetic field

Specific heat (C_V) measurements in the spin-1/2 Cu₂(C₂H₁₂N₂)₂Cl₄ system under a magnetic field up to H =8.25 T are reported and compared to the results of numerical calculations based on the 2-leg antiferromagnetic Heisenberg ladder. While the temperature dependences of both the susceptibility and the low-field specific heat are accurately reproduced by this model, deviations are observed above the critical field H_C1 at which the spin gap closes. In this Quantum High Field phase, the contribution of the low-energy quantum fluctuations are stronger than in the Heisenberg ladder model. We argue that this enhancement can be attributed to dynamical lattice fluctuations. Finally, we show that such a Heisenberg ladder, for H > H C1, is unstable, when coupled to the 3D lattice, against a lattice distortion. These results provide an alternative explanation for the observed low temperature ( K-0.8 K) phase (previously interpreted as a 3D magnetic ordering) as a new type of incommensurate gapped state. Received: 23 July 1998 / Accepted: 24 August 1998     

Investigations of the sublattice magnetizations M(T) in antiferromagnets with fourth-order exchange interactions: EuSrTe

We present a neutron scattering study of the temperature and composition dependence of the MnO-type superstructure reflection intensities in the diamagnetically diluted antiferromagnetic compounds Eu_xSr_1-xTe. In these materials antiferromagnetic biquadratic and ferromagnetic three-spin interactions have been identified recently. These fourth-order non-Heisenberg interactions are able to create their own order parameter which is believed to govern the order of the transverse moment components and which, hence, is directed perpendicular to the common Heisenberg order parameter. The observed MnO-type diffraction intensities originate in the sublattice magnetizations, , of both order parameters. Due to the different composition dependencies for biquadratic interaction processes and three-spin interaction processes , the ferromagnetic three-spin interactions dominate for x > x c =0.85, while for x <0.85 the antiferromagnetic biquadratic interactions dominate. Associated with this sign change in the fourth-order interaction sum the transverse order parameter changes from the antiferromagnetic MnO type for x <0.85 to ferromagnetic for x >0.85. This is noticed as a sudden decrease of the low-temperature MnO scattering intensities at x c =0.85. Although susceptibility measurements reveal clearly a ferromagnetic component for x >0.85 no ferromagnetic Bragg intensities were observed in standard neutron scattering spectra using EuTe powder samples. We explain this by the competition of antiferromagnetic biquadratic and ferromagnetic three-spin interactions whereby a disturbed ferromagnetic superstructure may be generated which gives rise also to weak MnO-type diffraction lines. It is found that the resulting obeys a T² law until a temperature as large as 0.75T_N irrespective of the nature of the transverse order parameter. The T² law must, hence, be common to both types of order parameter showing that the fourth-order interactions re-define the spin dynamics of both completely. From the linear composition dependence of the normalized T² coefficient the existence of three-spin interactions is again confirmed. Received 23 July 1998 and Received in final form 12 October 1998     

On the T Bloch law in magnets with fourth-order exchange interaction

For the ferromagnets EuS and GdMg, in which fourth-order exchange interactions (i.e. biquadratic, three-spin and four-spin interactions) have been identified, the deviation of the spontaneous magnetization with respect to the T =0 value is shown to follow a T² law instead of the famous T3/2 law expected for a Heisenberg ferromagnet. Moreover, the observed T² law holds for temperatures as large as 0.8T_C and the extrapolated magnetization value for does not conform to ferromagnetic saturation. This is because the fourth-order exchange interactions generate a second order-parameter which is assumed to govern the order of the transverse moment components. These moment components have a finite expectation value for at the expense of the Heisenberg order parameter. Like the spontaneous magnetization, the critical field curves B c ( T ) of the metamagnet EuSe and the antiferromagnet EuTe also start decreasing with a T² term for . It is argued that the T² law is a consequence of the fourth-order exchange interactions. This is shown experimentally by a study of the critical field curves [0pt] pertinent to the longitudinal (Heisenberg) order-parameter in the diamagnetically diluted antiferromagnets Eu_xSr_1-xTe. In this solid solution series a particular composition of x c =0.85 exists at which the different fourth-order interaction processes compensate each other in the high temperature average. As a consequence, an Eu_xSr_1-xTe sample with x =0.85 meets the requirements of a Heisenberg antiferromagnet at least if a quantity is considered for which the high-temperature average over all fourth-order interactions is decisive. This seems to be the case for the critical field curve [0pt] which gives the phase boundary to the paramagnetic phase. In fact, a crossover from a T² to a T3/2 law is observed for [0pt] on approaching x_c. This, we believe, shows the frequently observed T² law is caused by the fourth-order interactions. Received 23 July 1998 and Received in final form 12 October 1998     

Anelastic relaxation and around the critical Sr content x = 0.02

Anelastic relaxation and ¹³⁹LaNQR relaxation rates in La_2–xSr_xCuO₄ for Sr content around 2 and 3 percent are discussed in terms of spin and lattice excitations and of the related ordering processes. It is argued how the phase diagram of La_2–xSr_xCuO₄ at the boundary between the antiferromagnetic (AF) and the spin-glass phase (x = 0.02) could be more complicate than previously thought, with a transition to a quasi-long range ordered state at K, as indicated by neutron scattering data. On the other hand, the ¹³⁹LaNQR spectra are compatible with a transition to an AF phase around K, in agreement with the phase diagram commonly accepted in literature. In this case the peaks in NQR and anelastic relaxation rates around 150 K and 80 K respectively in La_1.98Sr_0.02CuO₄, yield the first evidence of freezing process involving simultaneously lattice and spin excitations, possibly corresponding to motion of charged stripes. Received 18 May 2000 and Received in final form 11 July 2000     

Charge ordering-disordering in the Th-doped CaMnO3

The structural transitions that appear in the manganites Ca_1-xTh_xMnO₃ versus temperature are studied in connection with their magnetic and transport properties, and compared to those of the Ca_1-xLn_xMnO₃ manganites. An orthorhombic to monoclinic transition is observed for low x values (;this structural distortion, also observed for Ln-doped oxides, is related to the magnetoresistance properties. For higher x values (), modulated commensurate and incommensurate phases are obtained at low temperature, with , b =2 a p and , which are related to Mn³⁺/Mn⁴⁺ charge ordering (CO) phenomena. T values, determined from electron diffraction, are in agreement with those determined from the M ( T ) curves. The low temperature electron microscopy shows that the CO in those oxides is more complex than in Ln-doped manganites. In particular, the destabilisation of CO and consequently of the antiferromagnetic interactions is evidenced as the thorium content increases which may explain the appearance of a spin-glass like behavior for higher x values not seen for Ca_1-xSm_xMnO₃ phases . Received 2 November 1998     

Soft modes and phonon interactions in studied by neutron scattering

The low frequency lattice dynamics and its relationship to the second order paraelectric-to-ferroelectric transition in Sn₂P₂S₆ is studied. The dispersion branches of the acoustic and lowest lying optical phonons in the a^*-c^* plane have been obtained in the ferroelectric phase, for x-polarized phonons. Close to the phase transition a considerable softening is found for the lowest optical mode (P_x), comparable to the behaviour observed in previous Raman investigations. As found previously in Sn₂P₂Se₆, a strong coupling between the TO(P_x) and TA(u_xz) phonons is observed, although, apparently, not strong enough to lead to an incommensurate phase. The soft TO(P_x) mode at the zone center is observed. The temperature dependence of its frequency and damping shows that the transition is not entirely displacive. At low temperatures an unusual apparent negative LO-TO splitting is observed which is shown to arise from the coupling of the x-polarized soft mode to the nearby z-polarized optical phonon. For comparison, the soft TO(P_x) dispersion in the a^*-b^* plane is measured in both the paraelectric and ferroelectric phases. Consistent frequency changes and LO-TO splitting are observed, revealing a significant interaction between the TA(u_yx) and LA(u_xx) acoustics branches and the TO and LO soft optic branches, respectively. In contrast, the nearby y-polarized optic branch shows almost no temperature dependence. Finally, the influence of piezoelectric effects on the limiting acoustic slopes in the ferroelectric phase is discussed. Received: 11 May 1998 / Revised and Accepted: 15 June 1998     

SR evidence of low frequency spin fluctuations in the AF phase of hole-doped NiO

μSR measurements in the antiferromagnetic (AF) phase of Ni_1-xLi_xO for are reported. While in pure NiO the muon longitudinal depolarization rate is found almost temperature independent, in the Li-doped compounds broad maxima around 130 K are observed. These maxima are associated with the progressive freezing of the spin fluctuations of S =1/2 defects induced by the localization of the extra-holes. From the temperature dependence of and the stretched exponential form of the depolarization, insights on the distribution of correlation times for the fluctuating field at the muon site are derived. Received: 27 April 1998 / Received in final form and Accepted: 21 August 1998     

Magnetic order in LaEuSrCuO studied [2pt] by Fe Mössbauer spectroscopy

⁵⁷Fe M?ssbauer effect studies of La_1.65Eu_0.20Sr_0.15CuO₄ doped with 0.5 at% ⁵⁷Fe performed in the temperature region 300 K > T > 4.2 K give an onset temperature for magnetic ordering of K. This temperature practically is the same as that found in Nd doped La_2-xSr_xCuO₄. It indicates that the magnetic ordering temperature in the LTT phase of rare earth (RE) doped La_2-xSr_xCuO₄ is independent of the RE moment. The direction of the ⁵⁷Fe magnetic moment in the magnetically ordered state is within the CuO₂ plane, while it has been found to be parallel to the c-axis in Nd doped La_2-xSr_xCuO₄. Received: 23 June 1998 / Accepted: 14 July 1998     

High-pressure study of the non-Fermi liquid material U 2 Pt 2 In

The effect of hydrostatic pressure ( p ? 1.8 GPa) on the non-Fermi liquid state of U₂Pt₂In is investigated by electrical resistivity measurements in the temperature interval 0.3-300 K. The experiments were carried out on single-crystals with the current along ( I || c ) and perpendicular ( I || a ) to the tetragonal axis. The pressure effect is strongly current-direction dependent. For I || a we observe a rapid recovery of the Fermi-liquid T²-term with pressure. A comparison of the data with the magnetotransport theory of Rosch provides evidence for the location of U₂Pt₂In at an antiferromagnetic quantum critical point. For I || c the resistivity increases under pressure, indicating the enhancement of an additional scattering mechanism. Received 2 March 2001 and Received in final form 29 June 2001     

Magnetic order and transport in the heavy-fermion system CeCuAu

We report on extensive elastic neutron scattering to determine the wave vector of the magnetic order in CeCu_6-xAu_x single crystals for x > 0.1. For all values of x investigated (0.2, 0.3, 0.5, 1.0) we find long-range incommensurate antiferromagnetic order with an ordering vector (0.625 0.275) for x =0.2, nearly unchanged for x =0.3, and (0.59) for x =0.5, staying roughly the same for x =1.0. In addition, short-range correlations are observed for x =0.2, reminiscent of those found previously for x =0.1. The ordered magnetic moment is found to increase rapidly for small x, and more slowly for the larger x values. The increase of the specific-heat anomaly at the ordering temperature with x is in qualitative accord with this behavior. Finally, data of the electrical resistivity for current flow along the three crystallographic directions are presented, showing a clear signature of the magnetic order. A theoretical interpretation of the interplay of magnetic order and transport in terms of (i) the partial suppression of the Kondo effect by the staggered magnetization and (ii) the anisotropic band structure induced by the staggered field is shown to account well for the data, provided the ordering vector is close to 2 k F, where k F is a typical Fermi momentum. Received: 20 February 1998 / Accepted: 17 April 1998     

Effective Hubbard model for Zn-doped CuO2 plane

In the framework of the cell-perturbation method for the original p-d model an effective two-band Hubbard model for the CuO₂ plane with Zn impurities is derived. Zn impurities are modelled by Wannir oxygen one-hole states at vacant Cu sites. The model is based on the results of band structure calculations carried out within the local-density approximation. Further reduction to an extended t-J model shows a large ferromagnetic superexchange interaction between the Cu spin with the nearest virtual oxygen spin in the Zn cell. Received 17 November 1998     

Electronic properties of CuO 2 -planes: A DMFT study

We study one-particle spectra and the electronic band-structure of a CuO ₂ -plane within the three-band Hubbard model. The Dynamical Mean-Field Theory (DMFT) is used to solve the many particle problem. The calculations show that the optical gap is given by excitations from the lower Hubbard band into the so called Zhang-Rice singlet band. The optical gap turns out to be considerably smaller than the bare charge transfer energy () for a typical set of parameters, which is in agreement with experiment. We also investigate the dependence of the shape of the Fermi surface on the different hopping parameters t CuO and t OO. A value t OO / t CuO >0 leads to a Fermi surface surrounding the M point. Received 21 September 1998 and Received in final form 8 June 1999     

Long and short range spin-spin interactions in ErBaCuO

Dipolar spin-spin interactions play a crucial role as for the magnetic order in the compounds of the RBa₂Cu₃O_6+x family, (R = Dy, Er, Nd). However, inelastic neutron scattering data observed in ErBa₂Cu₃O₇ can be explained only if exchange interactions in addition to dipolar ones are taken into account. Received: 12 January 1998 / Received in final form: 26 March 1998 / Accepted: 10 April 1998