Ordre magnétique à q=0 dans les cuprates supraconducteurs à haute température critique

This work is motivated by the study of the intra-unit-cell magnetic order in cuprate high temperature superconductors. It has been already reported in four cuprate families by using polarized neutron scattering, and it is well documented in a wide hole doping range. This order develops below Tmag, which matches the pseudo-gap temperature T*. This magnetic phase could be induced by the staggered orbital magnetism within the unit cell as proposed in the loop current model. This intra-unit-cell magnetic order indicates that time reversal symmetry is broken, but translation invariance is preserved. Experimentally, the goal is not only to systematically verify the existence of this intra-unit-cell magnetic order, but also to seize its nature. We particularly focused on two bilayer systems, YBa2Cu3O6+x and Bi2Sr2CaCu2O8+x. First, we revealed the persistence of the intra-unit-cell magnetic order at relatively high Tmag, near optimal doping. Compared to samples with a lower hole doping level, the magnetic intensity is strongly reduced. We demonstrated that this is due to finite magnetic correlation lengths. Moreover, we determined the associated magnetic structure factor along c, which displays a unique sharp decreasing. It is consistent with a model in which the sum of two anapoles within the bilayer is pointing along b*. Besides, below Tmag, we confirmed the existence of a tilt of the magnetic moment. However, we showed that at high temperature an Ising-like response along the c-axis is recovered. Finally, we proved that the magnetic signal associated to the intra-unit-cell magnetic order is still increasing in the superconducting state.Cette thèse a pour motivation l'étude de l'ordre magnétique à q=0 dans les cuprates supraconducteurs à haute température critique. Cet ordre a déjà été reporté dans quatre familles de cuprates grâce à la diffusion de neutrons polarisés. Il est établi, sur une large gamme de dopage en trous, que cet ordre se développe à partir d'une température Tmag comparable à la température d'apparition de la phase de pseudo-gap T*. Ces observations sont compatibles avec un modèle de boucles de courant, qui induisent des moments magnétiques orbitaux. Les symétries mises en jeu sont la brisure par renversement du temps et l'invariance par translation. D'un point de vue expérimental, il s'agit non seulement de vérifier systématiquement l'existence de cet ordre magnétique, mais également de saisir sa nature. Nous nous sommes particulièrement intéressés à l'étude de deux systèmes bicouches, YBa2Cu3O6+x et Bi2Sr2CaCu2O8+x. Dans un premier temps, nous avons montré la persistance de l'ordre magnétique à q=0 pour une valeur de Tmag relativement élevée, dans des échantillons proches du dopage optimal. Toutefois, l'intensité magnétique associée est fortement réduite. Nous avons montré que ceci était en fait dû à la présence de domaines de taille finie, l'ordre est à courte portée. Aussi, nous avons déterminé le facteur de structure le long de l'axe c, il présente une décroissance rapide unique. Dans le cadre des boucles de courant, une possible modélisation consisterait en une résultante de deux anapoles pointant le long de b* au sein de la bicouche. D'autre part, nous avons confirmé l'existence d'un moment magnétique incliné sous Tmag. Nous avons cependant mis en évidence un caractère Ising le long de l'axe c à haute température. Enfin, nous avons prouvé que le signal associé à l'ordre magnétique à q=0 continue d'augmenter dans l'état supraconducteur

Microscopic versus Macroscopic Glass Transitions and Relevant Length Scales in Mixtures of Industrial Interest

We have combined X-ray diffraction, neutron diffraction with polarization analysis, small-angle neutron scattering (SANS), neutron elastic fixed window scans (EFWS), and differential scanning calorimetry (DSC) to investigate polymeric blends of industrial interest composed by isotopically labeled styrene–butadiene rubber (SBR) and polystyrene (PS) oligomers of size smaller than the Kuhn length. The EFWS are sensitive to the onset of liquid-like motions across the calorimetric glass transition, allowing the selective determination of the “microscopic” effective glass transitions of the components. These are compared with the “macroscopic” counterparts disentangled by the analysis of the DSC results in terms of a model based on the effects of thermally driven concentration fluctuations and self-concentration. At the microscopic level, the mixtures are dynamically heterogeneous for blends with intermediate concentrations or rich in PS, while the sample with highest content of the fast SBR component looks as dynamically homogeneous. Moreover, the combination of SANS and DSC has allowed determining the relevant length scale for the α-relaxation through its loss of equilibrium to be ≈30 Å. This is compared with the different characteristic length scales that can be identified in these complex mixtures from structural, thermodynamical, and dynamical points of view because of the combined approach followed. We also discuss the sources of the non-Gaussian effects observed for the atomic displacements and the applicability of a Lindemann-like criterion in these materials.We thank Marc Couty for fruitful discussions and Karine Vernay (Michelin Advanced Research) for dSBR synthesis. The authors acknowledge Grant PID2021-123438NB-I00 funded by MCIN/AEI/10.13039/501100011033 and by “ERDF A way of making Europe”, as well as financial support of Eusko Jaurlaritza (code: IT1566-22) and from the IKUR Strategy under the collaboration agreement between Ikerbasque Foundation and the Materials Physics Center on behalf of the Department of Education of the Basque Government. We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI)

Disentangling Component Dynamics in an All-Polymer Nanocomposite Based on Single-Chain Nanoparticles by Quasielastic Neutron Scattering

[EN] We have investigated an all-polymer nanocomposite (NC) consisting of single-chain nanoparticles (SCNPs) immersed in a matrix of linear chains of their precursors (25/75% composition in weight). The SCNPs were previously synthesized via "click" chemistry, which induces intramolecular cross-links in the individual macromolecules accompanied by a slight shift (5-8 K) of the glass transition temperature toward higher values and a broadening of the dynamic response with respect to the raw precursor material. The selective investigation of the dynamics of the NC components has been possible by using properly isotopically labeled materials and applying quasielastic neutron scattering techniques. Results have been analyzed in the momentum transfer range where the coherent scattering contribution is minimal, as determined by complementary neutron diffraction experiments with polarization analysis. We observe the development of dynamic heterogeneity in the intermediate scattering function of the NC components, which grows with increasing time. Local motions in the precursor matrix of the NC are accelerated with respect to the reference bulk behavior, while the displacements of SCNPs' hydrogens show enhanced deviations from Gaussian and exponential behavior compared with the pure melt of SCNPs. The resulting averaged behavior in the NC coincides with that of the pure precursor, in accordance with the macroscopic observations by differential scanning calorimetry (DSC) experiments.We acknowledge the Grant PGC2018-094548-B-I00 funded by MCIN/AEI/10.13039/501100011033 and by "ERDF A way of making Europe". We also acknowledge the financial support of Eusko Jaurlaritza, codes: IT-1175-19 and IT1566-22 and the Open Access funding provided by University of Basque Country

Structure, spin correlations and magnetism of the S=1/2S = 1/2 square-lattice antiferromagnet Sr2_2CuTe1−x_{1-x}Wx_xO6_6 (0≤x≤10 \leq x \leq 1)

Quantum spin liquids are highly entangled magnetic states with exotic properties. The $S = 1/2$ square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are physical realizations of this model, but have distinctly different types magnetic order and interactions due to a $d^{10}/d^0$ effect. Long-range magnetic order is suppressed in the solid solution Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ in a wide region of $x = 0.05-0.6$, where the ground state has been proposed to be a disorder-induced spin liquid. Here we show that the spin-liquid-like $x = 0.2$ and $x = 0.5$ samples have distinctly different local spin correlations, which suggests they have different ground states. Furthermore, the previously ignored interlayer coupling between the square-planes is likely to play a role in the suppression of magnetic order on the W-rich side at $x \approx 0.6$. These results highlight the complex magnetism of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ and hint at a new quantum critical point at $x \approx 0.3$.Comment: 19+8 pages, 6+8 figure

Structure, Spin Correlations, and Magnetism of the S = 1/2 Square-Lattice Antiferromagnet Sr2CuTe1-xWxO6 (0 ≤ x ≤ 1)

Quantum spin liquids are highly entangled magnetic states with exotic properties. The S = 1/2 square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr2CuTeO6 and Sr2CuWO6 are physical realizations of this model but have distinctly different types of magnetic order and interactions due to a d10/d0 effect. Long-range magnetic order is suppressed in the solid solution Sr2CuTe1-xWxO6 in a wide region of x = 0.05-0.6, where the ground state has been proposed to be a disorder-induced spin liquid. Here, we present a comprehensive neutron scattering study of this system. We show using polarized neutron scattering that the spin liquid-like x = 0.2 and x = 0.5 samples have distinctly different local spin correlations, which suggests that they have different ground states. Low-temperature neutron diffraction measurements of the magnetically ordered W-rich samples reveal magnetic phase separation, which suggests that the previously ignored interlayer coupling between the square planes plays a role in the suppression of magnetic order at x ≈ 0.6. These results highlight the complex magnetism of Sr2CuTe1-xWxO6 and hint at a new quantum critical point between 0.2 &lt; x &lt; 0.4.</p

Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr2_2Sn2_2O7_7

Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classical spin ice state with low-temperature spin freezing and emergent magnetic monopoles. Systems with smaller effective moments, such as Pr$^{3+}$-based pyrochlores, have been proposed as excellent candidates for hosting a "quantum spin ice" characterized by entanglement and a slew of exotic quasiparticle excitations. However, experimental evidence for a quantum spin ice state has remained elusive. Here, we show that the low-temperature magnetic properties of Pr$_2$Sn$_2$O$_7$ satisfy several important criteria for continued consideration as a quantum spin ice. We find that Pr$_2$Sn$_2$O$_7$ exhibits a partially spin-frozen ground state with a large volume fraction of dynamic magnetism. Our comprehensive bulk characterization and neutron scattering measurements enable us to map out the magnetic field-temperature phase diagram, producing results consistent with expectations for a ferromagnetic Ising pyrochlore. We identify key hallmarks of spin ice physics, and show that the application of small magnetic fields ($\mu_0 H_c \sim$0.75T) suppresses the spin ice state and induces a long-range ordered magnetic structure. Together, our work clarifies the current state of Pr$_2$Sn$_2$O$_7$ and encourages future studies aimed at exploring the potential for a quantum spin ice ground state in this system

Intra-unit-cell magnetic order in cuprate high temperature superconductors

Cette thèse a pour motivation l'étude de l'ordre magnétique à q=0 dans les cuprates supraconducteurs à haute température critique. Cet ordre a déjà été reporté dans quatre familles de cuprates grâce à la diffusion de neutrons polarisés. Il est établi, sur une large gamme de dopage en trous, que cet ordre se développe à partir d'une température Tmag comparable à la température d'apparition de la phase de pseudo-gap T*. Ces observations sont compatibles avec un modèle de boucles de courant, qui induisent des moments magnétiques orbitaux. Les symétries mises en jeu sont la brisure par renversement du temps et l'invariance par translation. D'un point de vue expérimental, il s'agit non seulement de vérifier systématiquement l'existence de cet ordre magnétique, mais également de saisir sa nature. Nous nous sommes particulièrement intéressés à l'étude de deux systèmes bicouches, YBa2Cu3O6+x et Bi2Sr2CaCu2O8+x. Dans un premier temps, nous avons montré la persistance de l'ordre magnétique à q=0 pour une valeur de Tmag relativement élevée, dans des échantillons proches du dopage optimal. Toutefois, l'intensité magnétique associée est fortement réduite. Nous avons montré que ceci était en fait dû à la présence de domaines de taille finie, l'ordre est à courte portée. Aussi, nous avons déterminé le facteur de structure le long de l'axe c, il présente une décroissance rapide unique. Dans le cadre des boucles de courant, une possible modélisation consisterait en une résultante de deux anapoles pointant le long de b* au sein de la bicouche. D'autre part, nous avons confirmé l'existence d'un moment magnétique incliné sous Tmag. Nous avons cependant mis en évidence un caractère Ising le long de l'axe c à haute température. Enfin, nous avons prouvé que le signal associé à l'ordre magnétique à q=0 continue d'augmenter dans l'état supraconducteur.This work is motivated by the study of the intra-unit-cell magnetic order in cuprate high temperature superconductors. It has been already reported in four cuprate families by using polarized neutron scattering, and it is well documented in a wide hole doping range. This order develops below Tmag, which matches the pseudo-gap temperature T*. This magnetic phase could be induced by the staggered orbital magnetism within the unit cell as proposed in the loop current model. This intra-unit-cell magnetic order indicates that time reversal symmetry is broken, but translation invariance is preserved. Experimentally, the goal is not only to systematically verify the existence of this intra-unit-cell magnetic order, but also to seize its nature. We particularly focused on two bilayer systems, YBa2Cu3O6+x and Bi2Sr2CaCu2O8+x. First, we revealed the persistence of the intra-unit-cell magnetic order at relatively high Tmag, near optimal doping. Compared to samples with a lower hole doping level, the magnetic intensity is strongly reduced. We demonstrated that this is due to finite magnetic correlation lengths. Moreover, we determined the associated magnetic structure factor along c, which displays a unique sharp decreasing. It is consistent with a model in which the sum of two anapoles within the bilayer is pointing along b*. Besides, below Tmag, we confirmed the existence of a tilt of the magnetic moment. However, we showed that at high temperature an Ising-like response along the c-axis is recovered. Finally, we proved that the magnetic signal associated to the intra-unit-cell magnetic order is still increasing in the superconducting state