Evidence for impurity-induced frustration in La2CuO4

Zero-field muon spin rotation and magnetization measurements were performed in La2Cu{1-x}MxO4, for 0<x< 0.12, where Cu2+ is replaced either by M=Zn2+ or by M=Mg2+ spinless impurity. It is shown that while the doping dependence of the sublattice magnetization (M(x)) is nearly the same for both compounds, the N\'eel temperature (T_N(x)) decreases unambiguously more rapidly in the Zn-doped compound. This difference, not taken into account within a simple dilution model, is associated with the frustration induced by the Zn2+ impurity onto the Cu2+ antiferromagnetic lattice. In fact, from T_N(x) and M(x) the spin stiffness is derived and found to be reduced by Zn doping more significantly than expected within a dilution model. The effect of the structural modifications induced by doping on the exchange coupling is also discussed.Comment: 4 pages, 4 figure

Antiferro-quadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7

We present an experimental study of the quantum spin ice candidate pyrochlore coumpound \przr\ by means of magnetization measurements, specific heat and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the $[111]$ and $[1\bar{1}0]$ directions, ${\bf k}=0$ field induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for $H \parallel [1\bar{1}0]$, the ordered moment appears on the so called $\alpha$ chains only. The spin excitation spectrum is essentially {\it inelastic} and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For $H \parallel [1\bar{1}0]$ (at least up to 2.5 T), we find that a well defined mode forms from this broad response, whose energy increases with $H$, in the same way as the temperature of the specific heat anomaly. We finally discuss these results in the light of mean field calculations and propose a new interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those new interactions. We then propose a range of acceptable parameters for \przr\, that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice like excitations

Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb2+x_{2+x}Ti2−x_{2-x}O7+y_{7+y}

While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.Comment: Main text: 7 pages, 3 figures ; Supplemental Material: 6 pages, 2 figure

Observation of low energy dispersive modes in un- derdoped (La, Nd) 2−x Sr x CuO 4

We find excitations lower in energy than known phonon modes in underdoped La$_{2-x}$Sr$_x$CuO$_{4+\delta}$ (x=0.08), with both inelastic X-Ray scattering (IXS) and inelastic neutron scattering (INS). A non dispersive excitation at 9 meV is identified and is also seen by INS in (La,Nd)$_{2-x}$Sr$_x$CuO$_{4+\delta}$, with 40$\%$ Nd substitution. INS also identifies a still lower energy dispersive mode at low q in the Nd free sample. These modes are clearly distinct from the longitudinal acoustic phonon and correspond in energy to the Zone Centre modes measured by optical spectroscopy and associated with stripe dynamics

Systèmes magnétiques dilués à base d'oxydes

version 12-12-2006Following the report of a new kind of room temperature ferromagnetism in thin films of titanium oxide doped with cobalt, the research of analogous properties in bulk SrTiO3-based perovskite was considered. Solid solutions of SrTi(1-x)M(x)O(3-d) (M = Co, Fe ; 0.01 less or equal to x less or equal to 0.50) were prepared by substitution of cobalt or iron fot titanium; the oxygen stoechiometry was modified for some of these compositions by thermal treatment under low oxygen pressure. The magnetic properties of the two systems under study are very similar. All the compositions have a paramagnetic behavior; only in highly doped samples (x higher or equal to o.35) a transition to a spin glass state is show. A small ferromagnetic component was detected at low temperature in these high doped samples and associated with some ferromagnetic exchange interactions that can exist in the systems. In the weakly doped samples (x=0.01 and 0.02) a different small ferromagnetic signal was detected at room temperature; his evolution with the dopant concentration and oxygen stoechiometry was studied. The results suggest that the dopant may not be at the origin of the observed ferromagnetism. The highly doped samples show a semiconductor behavior with unexpected temperature dependence.Suite aux travaux ayant mis en évidence une forme de ferromagnétisme inhabituelle à température ambiante dans des couches minces d'oxyde de titane dopées au cobalt, la recherche de comportement analogue dans des matériaux massifs à base de pérovskite SrTiO3 a été entreprise. En substituant le titane par le cobalt ou le fer, des solutions solides SrTi(1-x)M(x)O(3-d) (M = Co, Fe ; 0.01 plus petit ou égal à x plus petit ou égal à 0.50) ont été préparées ; de plus, la stœchiométrie en oxygène de certaines compositions a été modifiée par traitement sous faible pression partielle d'oxygène. Les propriétés magnétiques de ces deux systèmes sont très ressemblantes. Un comportement paramagnétique est mis en évidence dans toutes les compositions, seuls les échantillons fortement dopés (x plus grand ou égal à 0.35) présentent une transition vers un état verre de spin. Une composante ferromagnétique a été mise en évidence à basse température dans ces échantillons à forte concentration en dopant et associée aux échanges ferromagnétiques qui peuvent exister dans ces systèmes. Dans les échantillons faiblement dopés (x=0.01 et 0.02) une composante ferromagnétique très faible a été observée à la température ambiante ; son évolution avec la concentration en dopant ainsi qu'avec la stœchiométrie en oxygène des composés a été étudiée. Les résultats obtenus suggèrent que le dopant pourrait ne pas être à l'origine de ce ferromagnétisme. Les compositions les plus riches en fer ou en cobalt ont un comportement semi-conducteur présentant une dépendance en température inattendue

Systèmes magnétiques dilués à base d'oxydes

Suite aux travaux ayant mis en évidence une forme de ferromagnétisme inhabituelle à température ambiante dans des couches minces d'oxyde de titane dopées au cobalt, la recherche de comportement analogue dans des matériaux massifs à base de pérovskite SrTiO3 a été entreprise. En substituant le titane par le cobalt ou le fer, des solutions solides SrTi(1-x)M(x)O(3-d) (M = Co, Fe ; 0.01 plus petit ou égal à x plus petit ou égal à 0.50) ont été préparées ; de plus, la stœchiométrie en oxygène de certaines compositions a été modifiée par traitement sous faible pression partielle d'oxygène. Les propriétés magnétiques de ces deux systèmes sont très ressemblantes. Un comportement paramagnétique est mis en évidence dans toutes les compositions, seuls les échantillons fortement dopés (x plus grand ou égal à 0.35) présentent une transition vers un état verre de spin. Une composante ferromagnétique a été mise en évidence à basse température dans ces échantillons à forte concentration en dopant et associée aux échanges ferromagnétiques qui peuvent exister dans ces systèmes. Dans les échantillons faiblement dopés (x=0.01 et 0.02) une composante ferromagnétique très faible a été observée à la température ambiante ; son évolution avec la concentration en dopant ainsi qu'avec la stœchiométrie en oxygène des composés a été étudiée. Les résultats obtenus suggèrent que le dopant pourrait ne pas être à l'origine de ce ferromagnétisme. Les compositions les plus riches en fer ou en cobalt ont un comportement semi-conducteur présentant une dépendance en température inattendue.Following the report of a new kind of room temperature ferromagnetism in thin films of titanium oxide doped with cobalt, the research of analogous properties in bulk SrTiO3-based perovskite was considered. Solid solutions of SrTi(1-x)M(x)O(3-d) (M = Co, Fe ; 0.01 less or equal to x less or equal to 0.50) were prepared by substitution of cobalt or iron fot titanium; the oxygen stoechiometry was modified for some of these compositions by thermal treatment under low oxygen pressure. The magnetic properties of the two systems under study are very similar. All the compositions have a paramagnetic behavior; only in highly doped samples (x higher or equal to o.35) a transition to a spin glass state is show. A small ferromagnetic component was detected at low temperature in these high doped samples and associated with some ferromagnetic exchange interactions that can exist in the systems. In the weakly doped samples (x=0.01 and 0.02) a different small ferromagnetic signal was detected at room temperature; his evolution with the dopant concentration and oxygen stoechiometry was studied. The results suggest that the dopant may not be at the origin of the observed ferromagnetism. The highly doped samples show a semiconductor behavior with unexpected temperature dependence.ORSAY-PARIS 11-BU Sciences (914712101) / SudocSudocFranceF

Zirconate Pyrochlore Frustrated Magnets: Crystal Growth by the Floating Zone Technique

This article reviews recent achievements on the crystal growth of a new series of pyrochlore oxides—lanthanide zirconates, which are frustrated magnets with exotic magnetic properties. Oxides of the type A 2 B 2 O 7 (where A = Rare Earth, B = Ti, Mo) have been successfully synthesised in single crystal form using the floating zone method. The main difficulty of employing this technique for the growth of rare earth zirconium oxides A 2 Zr 2 O 7 arises from the high melting point of these materials. This drawback has been recently overcome by the use of a high power Xenon arc lamp furnace for the growth of single crystals of Pr 2 Zr 2 O 7 . Subsequently, large, high quality single crystals of several members of the zirconate family of pyrochlore oxides A 2 Zr 2 O 7 (with A = La → Gd) have been grown by the floating zone technique. In this work, the authors give an overview of the crystal growth of lanthanide zirconates. The optimum conditions used for the floating zone growth of A 2 Zr 2 O 7 crystals are reported. The characterisation of the crystal boules and their crystal quality is also presented