An NMR approach to the superconducting regime of the spin ladder compound Sr2Ca12Cu24O41

⁶³Cu-NMR experiments of Knight shift and relaxation time T₁ have been performed on the two-leg spin ladders of a Sr₂Ca₁₂Cu₂₄O₄₁ single crystal at several pressures up to the critical pressure for the stabilization of a superconducting ground state. The data confirm the onset of low-lying spin excitations at observed previously [Science 279, 345 (1998)] and reveal a marked decrease of the spin gap under pressures above 20 kbar although a significant fraction of the spin excitations remains gapped at kbar. A comparison between NMR and transport data under pressure suggests that the depression of the spin gap can be ascribed to an increase in the interladder exchange coupling, possibly mediated by the ladder-chain interaction along the b-direction. Received 21 October 1999     

Mechanical detection of nuclear spin relaxation in a micron-size crystal

A room temperature nuclear magnetic resonance force microscope (MRFM), fitted in a 1 tesla electromagnet, has been used to measure the nuclear spin relaxation of ¹H in a micron-size (70 ng) crystal of ammonium sulfate. NMR sequences, combining both pulsed and continuous wave radio-frequency fields, have allowed us to measure mechanically T₂ and T₁, the transverse and longitudinal spin relaxation times. Because two spin species with different T₁ values are measured in our 7 μm thick crystal, magnetic resonance imaging of their spatial distribution inside the sample section have been performed. To understand quantitatively the measured signal, we carefully study the influence of spin-lattice relaxation and non-adiabaticity of the continuous-wave sequence on the intensity and time dependence of the detected signal. Received 23 February 2000     

Dynamical properties of low-dimensional and spin-Peierls systems

Properties of low-dimensional spin-Peierls systems are described by using a one-dimensional S =1/2 antiferromagnetic Heisenberg chain linearly coupled to a single phonon mode of wave vector (whose contribution is expected to be dominant). By exact diagonalizations of small rings with up to 24 sites supplemented by a finite size scaling analysis, static and dynamical properties are investigated. Numerical evidences are given for a spontaneous discrete symmetry breaking towards a spin gapped phase with a frozen lattice dimerization. Special emphasis is put on the comparative study of the two inorganic spin-Peierls compounds CuGeO₃ and NaV₂O₅ and the model parameters are determined from a fit of the experimental spin gaps. We predict that the spin-phonon coupling is 2 or 3 times larger in NaV₂O₅ than in CuGeO₃. Inelastic neutron scattering spectra are calculated and similar results are found in the single phonon mode approximation and in the model including a static dimerization. In particular, the magnon S =1 branch is clearly separated from the continuum of triplet excitations by a finite gap. Received: 30 July 1997 / Revised: 16 September 1997 / Accepted: 10 October 1997     

Model glasses coupled to two different heat baths

In a p-spin interaction spherical spin-glass model both the spins and the couplings are allowed to change with time. The spins are coupled to a heat bath with temperature T, while the coupling constants are coupled to a bath having temperature T_J. In an adiabatic limit (where relaxation time of the couplings is much larger that of the spins) we construct a generalized two-temperature thermodynamics. It involves entropies of the spins and the coupling constants. The application for spin-glass systems leads to a standard replica theory with a non-vanishing number of replicas, n=T/T _J . For p>2 there occur at low temperatures two different glassy phases, depending on the value of n. The obtained first-order transitions have positive latent heat, and positive discontinuity of the total entropy. This is an essentially non-equilibrium effect. The dynamical phase transition exists only for n<1. For p=2 correlation of the disorder (leading to a non-zero n) removes the known marginal stability of the spin glass phase. If the observation time is very large there occurs no finite-temperature spin glass phase. In this case there are analogies with the non-equilibrium (aging) dynamics. A generalized fluctuation-dissipation relation is derived. Received 12 July 1999 and Received in final form 8 December 1999     

Dynamic triggering of a spin-transition by a pulsed magnetic field

We report the first study of the effect of a high pulsed magnetic field on a spin transition complex in the solid state. The high spin fraction was determined by optical reflectivity. Sizeable effects are observed for the well-known spin transition solid Fe(Phen)₂(NCS)₂. In the hysteresis loop temperature range, an increase in the HS fraction is obtained, with an irreversible (reversible) character in the ascending (descending) branch of the loop. The time dependence of the HS fraction provides information on the kinetics of the spin-crossover process at the spin transition. Received 23 February 1999 and Received in final form 8 June 1999     

High field ESR measurements of spin gap system MCu2(PO4)2

Submillimeter and millimeter wave ESR measurements of spin gap systems SrCu₂(PO₄)₂ and PbCu₂(PO₄)₂, which have four kinds of dimers, have been performed to investigate the magnetic properties of spin gap systems using the pulsed magnetic field up to 35T. The observed ESR spectra of powder sample SrCu₂(PO₄)₂ show sharp and single peak in the temperature range from 4.2 to 80 K. The anisotropy of the g-values turned out to be very small compared to the usual anisotropic powder spectra of copper compounds. The dynamical properties will be discussed from the temperature dependence measurements.     

Crossing of specific heat curves in some correlated fermion systems

Specific heat versus temperature curves for various pressures, or magnetic fields (or some other external control parameter) have been seen to cross at a point or in a very small range of temperatures in many correlated fermion systems. We show that this behavior is related to the possibility of existence of a quantum critical point. Vicinity to a quantum critical point in these systems leads to a crossover from quantum to classical fluctuation regime at some temperature . The temperature at which the curves cross turns out to be near this crossover temperature. We have discussed the case of the normal phase of liquid Helium three and the heavy fermion systems CeAl₃ and UBe₁₃ in detail within the spin fluctuation theory, a theory which inherently contains a low energy scale which can be identified with . When the crossover scale is a homogeneous function of these control parameters there is always crossing at a point. We also mention other theories exhibiting a low energy scale near a quantum critical point and discuss this phenomenon in those theories. Received 25 June 1999     

Quantum fluctuations and ground state of weakly interacting helix spin chains in a magnetic field

Ferromagnetic spin chains of a hexagonal lattice coupled by a weak antiferromagnetic interaction J₁ develop a helix arrangement if the intrachain antiferromagnetic NNN exchange J₂ is sufficiently large. We show that the classical minimum energy spin configuration is an umbrella when an external magnetic field is applied. The scenario is dramatically changed by quantum fluctuations. Indeed we find that the zero point motion forces the spins in a plane containing the magnetic field so that classical expectation is deceptive for our model. Our result is obtained by controlled expansion in the low field-long wavelength modulation limit. Received: 9 September 1997 / Revised: 15 October 1997 / Accepted: 17 November 1997     

First and second order ferromagnetic transition at in a 1D itinerant system

We consider a modified version of the one-dimensional Hubbard model, the t ₁ - t ₂ Hubbard chain, which includes an additional next-nearest-neighbor hopping. It has been shown that at weak coupling this model has a Luttinger liquid phase or a spin liquid phase depending upon the ratio of t₂ to t₁. Additionally if the on-site interaction U is large enough, the ground state is fully polarized. Using exact diagonalization and the density-matrix renormalization group, we show that the transition to the ferromagnetic phase is either of first or second order depending on whether the Luttinger liquid or spin liquid is being destabilized. Since we work at T =0, the second order transition is a quantum magnetic critical point. Received 21 July 1999     

The magnetism for NN AFM ground state in Fe-based superconductor: Sr1−xKxFe2As2

The crystal structure, magnetism properties, and density of states for FeAs layered compound SrFe₂As₂ have been investigated by using the density functional theory (DFT) method. The magnetism under a checkerboard nearest neighbor anti-ferromagnetic (NN AFM) and ferromagnetic (FM) order ground-state have been analyzed with substitution for Sr with K ion in Sr_1−xK_xFe₂As₂. The results indicate that the distortion of FeAs tetrahedrons is sensitive to the electron doping concentration. The system magnetism was suppressed by K doping in NN-AFM ground state instead of FM. The density of states at Fermi level N(E_F) under NN AFM ground state would be regarded as a driving force for the increased T_c of Sr_1−xK_xFe₂As₂ system as observed experimentally. Our calculation reflects that NN AFM type spin fluctuation may still exist in the Sr_1−xK_xFe₂As₂ system and it may be an origin of strong spin fluctuation in this system besides the spin density wave (SDW) states.     

Antiferromagnetic resonance and high magnetic field properties of NaNiO2

Magnetisation measurements up to 23 T and submillimeter wave ESR in the frequency region 48-380 GHz have been performed on NaNiO₂ powders at low temperature. Also typical spectra above the Néel temperature are shown. At 4 K the magnetisation shows a spin-flop transition at 1.8 T and saturation at 10 T. /Ni confirms the low spin state of the Ni³⁺ ions. The susceptibility exhibits a maximum at K with and K. NaNiO₂ is an A-type antiferromagnet: we derive K and K for the interactions between Ni ions within and between adjacent layers, respectively. The AFMR spectra yield an energy gap of 52.5 GHz, in agreement with the spin-flop value derived from the magnetisation. The anisotropy of the g factor observed at 100 K with can be attributed to the Jahn-Teller effect for Ni³⁺ ions in the low spin state, which stabilises the occupation. We finally comment on the isomorphic controversial Li_1-xNi_1+xO₂ compound. Received 9 March 2000 and Received in final form 13 July 2000.     

Jahn-Teller distortion and magnetoresistance in electron doped Sr1-xCexMnO3 (x = 0.1, 0.2, 0.3 and 0.4)

Neutron and electron diffraction, electrical transport and magnetic measurements have been carried out on a newly synthesized electron doped Sr_1-xCe _x MnO₃ (x = 0.1, 0.2, 0.3 and 0.4) system. For x=0.1, while cooling, it undergoes a first-order metal-insulator transition at 315 K which is associated with a structural transition from cubic (Pm3m) to tetragonal (I4/mcm) due to Jahn-Teller ordering () which stabilizes a chain like (C-type) antiferromagnetic ground state with . The antiferromagnetic insulator state is insensitive to an applied magnetic field of 7 T. With increase of x, while the nuclear structure at room temperature for x=0.2 and 0.3 remains tetragonal, for x=0.4 it becomes orthorhombic (Imma) where the doping electrons seem to occupy mainly the d _x2-y2 symmetry. Further, the JT distortion and the antiferromagnetic interactions decrease with doping and a small negative magnetoresistance appears for . Magnetic measurements show that the dilution of antiferromagnetic interaction results into a spin glass like behaviour at low temperature for the samples with x=0.3 and 0.4. This behaviour is in contrast with the CMR properties of calcium based electron doped systems and hole doped manganites. The stability of C-type antiferromagnetic ordering in the electron doped system with large A-site cationic size may be responsible for the absence of double exchange ferromagnetism and CMR effect. Received 10 September 1999     

AC susceptibility enhancement studies in magnetic systems

Enhancement of AC susceptibility has been observed for typical ferromagnets (Gd), reentrant spin glasses like (Fe_1.5Mn_1.5Si) and canted spin systems (Ce(Fe_0.96Al_0.04)₂). The data have been interpreted with the help of a simulation model based on dry friction-like pinning of domain walls for systems having ferromagnetic domain structures. A strong pinning mechanism appears in the reentrant spin glass like and canted spin systems at low temperatures in addition to the intrinsic one in the ferromagnetic phase. The temperature variation of the pinning potential has been given qualitatively for the reentrant spin glass like systems.     

Heat capacities of the electron acceptor 7,7,8,8-tetracyano- quinodimethane (TCNQ) and its radical-ion salt NH4(TCNQ) showing spin-Peierls transition

Heat capacities of the electron acceptor 7,7,8,8-tetracyanoquinodimethane (TCNQ) and its radical-ion salt NH₄-TCNQ have been measured at temperatures in the 12-350 K range by adiabatic calorimetry. A λ-type heat capacity anomaly arising from a spin-Peierls (SP) transition was found at 301.3 K in NH₄-TCNQ. The enthalpy and entropy of transition are Δ_trsH=(667±7) J mol⁻¹ and Δ_trsS=(2.19±0.02) J K⁻¹ mol⁻¹, respectively. The SP transition is characterized by a cooperative coupling between the spin and the phonon systems. By assuming a uniform one-dimensional antiferromagnetic (AF) Heisenberg chains consisting of quantum spin (S=1/2) in the high-temperature phase and an alternating AF nonuniform chains in the low-temperature phase, we estimated the magnetic contribution to the entropy as Δ_trsS_mag=0.61 J K⁻¹ mol⁻¹ and the lattice contribution as Δ_trsS_lat=1.58 J K⁻¹ mol⁻¹. Although the total magnetic entropy expected for the present compound is R ln 2 (=5.76 J K⁻¹ mol⁻¹), a majority of the magnetic entropy (∼4.6 J K⁻¹ mol⁻¹) persists in the high-temperature phase as a short-range-order effect. The present thermodynamic investigation quantitatively revealed the roles played by the spin and the phonon at the SP transition. Standard thermodynamic functions of both compounds have also been determined.     

Enhancement of the anomalous Hall effect and spin glass behavior in the bilayered manganite La2−2xSr1+2xMn2O7

The Hall resistivity and magnetization have been investigated in the ferromagnetic state of the bilayered manganite La_2−2xSr_1+2xMn₂O₇ (x=0.36). The Hall resistivity shows an increase in both the ordinary and anomalous Hall coefficients at low temperatures below 50 K, a region in which experimental evidence for the spin glass state has been found in a low magnetic field of 1 mT. The origin of the anomalous behavior of the Hall resistivity relevant to magnetic states may lie in the intrinsic microscopic inhomogeneity in a quasi-two-dimensional electron system.     

Spin-ordering in S = 1 anisotropic Heisenberg models with nondiagonal spin exchange

The properties of S = 1 anisotropic Heisenberg models with nondiagonal exchange between axial and planar spin components are investigated using Monte Carlo techniques. The quantum nature is taken into account in a semi-classical approximation. The ordering of the spins when applying an external field with axial and planar components is discussed. It is argued that the quantum nature of the spins and the nondiagonal exchange may explain the peculiar shape of the magnetic specific heat of FeBr₂ as well as the weakly first-order phase transition observed in the same compound when a tilted field is applied. Received 24 January 1999     

Dynamics of photoinduced reactions at oxide surfaces

This report summarizes our work on UV-laser induced desorption of small molecules and atoms from transition metal oxides. The systems presented serve as examples for a simple photochemical reaction, the fission of the molecule surface bond. State resolved detection methods were used to record the final state distributions of the desorbing neutral molecules. Detailed results on the systems NO/NiO(1 1 1) and CO/Cr₂O₃ (0 0 0 1) are presented. The experiments include investigations on stereodynamic aspects like the angular distributions of the desorbing molecules and, in the case of CO desorption, the rotational alignment with respect to the surface normal. Large desorption cross sections of (6 ± 1) · 10^–17 cm² for NO and (3.5 ± 1) · 10^–17 cm² for CO have been found for the desorption at 6.4 eV. The wavelength dependence indicates that the primary excitation step is substrate induced. The final state distributions show a high degree of translational, rotational and vibrational excitation and are clearly nonthermal of origin. The results are consistent with the formation of a negative ion intermediate state of the adsorbate. This observation is supported from a comparison to former results on NO/NiO(1 0 0) for which extensive ab initio calculations including electronically excited states exist. A spin state dependence of the vibrational excitation of NO could only be observed for NO/NiO(1 1 1) and is absent for NO/NiO(1 0 0). We attribute this observation to a spin state dependent coupling of the desorbing molecule to the surface in case the spin lattice orientation of the surface shows a preferential orientation. In the (111) plane the spin orientation is parallel within neighbour nickel ions while it is alternating in the (1 0 0) plane. For both systems studied the velocity component parallel to the surface is constant leading to a strong peaking along the surface normal for the fast molecules. The change from a preferred helicopter rotation (angular momentum vector aligned parallel to the surface normal) to a cartwheel motion (angular momentum vector aligned perpendicular to the surface normal) with increasing rotational excitation for desorption of the flat lying CO is consistent with a change of bonding geometry during the desorption process.     

Analysis of the first electron-removal states of using polarization dependent angle-resolved photoelectron spectroscopy

The first electron-removal states of the layered cuprate Ba₂Cu₃O₄Cl₂ were measured using angle-resolved photoelectron spectroscopy. The symmetry and energy-momentum relations of the lowest-lying states were determined and interpreted in terms of the motion of a single hole in the two different planar Cu-O subsystems of the Cu₃O₄ plane. One subsystem is antiferromagnetic as in the undoped parent compounds of the high-temperature superconductors and the other is paramagnetic and corresponds to the strongly overdoped case. The data are compared to theoretical results on hole dynamics in two-dimensional antiferromagnetic or paramagnetic spin backgrounds. The lineshape, symmetry and dispersion of the first electron-removal states of Ba₂Cu₃O₄Cl₂ can be described in terms of Zhang-Rice singlets within a single band model. The photohole lifetime in the paramagnetic subsystem of the Cu₃O₄ plane is much smaller than with an antiferromagnetic spin background. Received 19 March 1999 and Received in final form 15 August 1999     

NMR relaxation at low temperature in one dimensional antiferromagnets: Comparison between S = 12 and S = 52

The proton spin-lattice relaxation time T₁ has been measured at low temperatures in spin $\text{5}\text{2}$ (CH₃)₄NMnCl₃ (TMMC) and spin $\text{1}\text{2}$ CuCl₂2NC₅H₅ (CuPC). The two systems have very different temperature dependences which we attribute to the different spin values.