CeFe$_2$ is a geometrically frustrated ferromagnet that lies close to an instability at which a subtle change in the lattice symmetry couples to a transition to antiferromagnetism. We use x-ray diffraction, diamond-anvil-cell techniques, and numerical simulation to identify the ground states and to quantitatively illustrate effects of competing magnetic energy scales and geometrical frustration on the magnetic phase diagram. Comparison of phase transitions under both chemical substitution and applied pressure suggests a general solution to the physics of pyrochlore rare earth inter-metallic magnets.
Impact of geometrical frustration on charge transport near the Mott transition in pyrochlore (Y$_{1-x}$Cd$_{x}$)$_{2}$Mo$_{2}$O$_{7}$
为了探索阻挫晶格强关联电子系统中的新的自旋-电荷耦合现象,研究了烧绿石结构空穴掺杂自旋玻璃(Mott)绝缘体(Y $_{1-x}$ Cd $_{x}$)$_{2}$ Mo $_{2}$ O $_{7}$的电荷输运和动力学.在空穴掺杂导致自旋玻璃态消失的同时,出现了具有强重整化电子质量的扩散金属输运,这种输运没有长程自旋有序,这是由几何阻挫引起的强反铁磁自旋涨落引起的.
We investigate the effect of partial replacement of extended 5d Ir4+ sites by localized 3d Cr3+ moments on the magnetocaloric properties of Y2Ir2O7 (YIO) pyrochlore iridates. We find that Y2Ir2-xCrxO7 (YICO) undergoes cluster glass transition, possibly due to RKKY like interaction between localized Cr3+ moments occupying random sites in the pyrochlore network, mediated by 5d Ir conduction electrons. The coexistence of ferromagnetic and antiferromagnetic clusters give rise to the conventional and inverse magnetocaloric effect (MCE). We observe significant enhancement of conventional as well as …
We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parameterize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualit…
采用完全相对论密度泛函理论结合在位排斥(U)方法研究了钼系高温超导体A2 Mo 2 O 7的电子和磁性,重点研究了自旋玻璃绝缘材料Y2 Mo 2 O 7.我们发现在大U绝缘区,系统的不同磁态之间存在着特殊的能量竞争。传统的海森堡反铁磁交换作用的几何阻挫模型不能解释这种磁竞争。通过对广义自旋模型的分析,我们发现有效自旋相互作用不同于简单的海森堡形式,在自旋空间中具有强的各向异性。我们还发现,它们引起激烈的竞争之间的反铁磁态和铁磁态。磁相互作用的复杂形式表明了轨道自由度的关键作用。通过对一个三轨道哈伯德模型的分析,阐明了在4d 2电子组态中,磁竞争通过自旋-轨道相互作用与轨道阻挫密切相关.结果挑战了传统的自旋玻璃行为的图片,属性的起源纯粹的反铁磁交换相互作用的几何挫折。
The gadolinium pyrochlores, Gd$_2B_2$O$_7$, are amongst the best realizations of antiferromagnetically coupled Heisenberg spins on a pyrochlore lattice. We present a magnetic characterization of Gd$_2$Pt$_2$O$_7$, a unique member of this family. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements show that Gd$_2$Pt$_2$O$_7$ undergoes an antiferromagnetic ordering transition at $T_N = 1.6$ K. This transition is strongly first order, as indicated by the sharpness of the heat capacity anomaly, thermal hysteresis in the magnetic susceptibility, and a non-divergent relaxat…
The crystal structures and magnetic properties of three previously unreported A2B2F7 pyrochlore materials, NaSrMn2F7, NaCaFe2F7, and NaSrFe2F7 are presented. In these compounds, either S=2 Fe2+ or S=5/2 Mn2+ is on the B site, while nonmagnetic Na and Ca (Na and Sr) are disordered on the A site. The materials, which were grown as crystals via the floating zone method, display high effective magnetic moments and large Curie-Weiss thetas. Despite these characteristics, freezing of the magnetic spins, characterized by peaks in the susceptibility or specific heat, is not observed until low temperat…
We consider the structure of anisotropic exchange interactions in ytterbium-based insulating rare-earth magnets built from edge-sharing octahedra. We argue the features of trivalent ytterbium and this structural configuration allow for a qualitative determination of the different anisotropic exchange regimes that may manifest in such compounds. The validity of such super-exchange calculations is tested through comparison to the well-characterized breathing pyrochlore compound Ba$_3$Yb$_2$Zn$_5$O$_{11}$. With this in hand, we then consider application to three-dimensional pyrochlore spinels as …
The Raman spectroscopy and AC and DC magnetization of Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$ have been investigated. In Raman Spectroscopy, the systematic shift in all phonon modes with Eu content in Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$ confirms that Dy$^{3+}$ ion is substituted by Eu3+ ions. High concentration of Eu induces the dipolar exchange interactions and crystal-field interactions in Dy$_{2-x}$Eu$_x$Ti$_2$O$_7$. Rich Eu content samples (x=1.8 and 1.9) show the existence of wasp-waisted hysteresis loop and that can be attributed to the coexistence of dipolar field and anisotropy exchange interaction. AC su…
Frustration in spin system can give rise to unique ordered states and as a consequence several physical phenomena are expected such as multiferroics, high temperature superconductors and anomalous hall effect. Here we report the "new magnetic orders" induced by anisotropic spin exchanges on pyrochlore spinels as the interplay of spin orbit coupling and geometrical frustration. Due to complicated superexchange paths of B-site spinels, we claim that anisotropic interaction between next-nearest neighbors play an important role. Based on the systematic studies of generic spin model, we argue that …
The consequences of nonmagnetic-ion dilution for the pyrochlore family Y$_{2}$($M_{1-x}N_{x}$)$_{2}$O$_{7}$ ($M$ = magnetic ion, $N$ = nonmagnetic ion) have been investigated. As a first step, we experimentally examine the magnetic properties of Y$_{2}$CrSbO$_{7}$ ($x$ = 0.5), in which the magnetic sites (Cr$^{3+}$) are percolative. Although the effective Cr-Cr spin exchange is ferromagnetic, as evidenced by a positive Curie-Weiss temperature, $Θ_\mathrm{CW}$ = 20.1(6) K, our high-resolution neutron powder diffraction measurements detect no sign of magnetic long range order down to 2 K. In ord…
We consider the pyrochlore-lattice quantum Heisenberg ferromagnet and discuss the properties of this spin model at arbitrary temperatures. To this end, we use the Green's function technique within the random-phase (or Tyablikov) approximation as well as the linear spin-wave theory and quantum Monte Carlo simulations. We compare our results to the ones obtained recently by other methods to corroborate our findings. Finally, we contrast our results with the ones for the simple-cubic-lattice case: both lattices are identical at the mean-field level. We demonstrate that thermal fluctuations are mo…
Geometrically Frustrated Quadrupoles on the Pyrochlore Lattice and Generalized Spin Liquids
Max Planck Institute for the Physics of Complex Systems(马克斯·普朗克复杂系统物理研究所);Laboratoire Léon Brillouin, CEA, CNRS, Université Paris-Saclay(里昂·布里渊实验室,法国原子能和替代能源委员会,法国国家科学研究中心,巴黎萨克雷大学);Université Grenoble Alpes, CNRS, Institut Néel(格勒诺布尔阿尔卑斯大学,法国国家科学研究中心,尼尔研究所)
Three-dimensionally (3D) frustrated magnets generally exist in the magnetic diamond and pyrochlore lattices, in which quantum fluctuations suppress magnetic orders and generate highly entangled ground states (GS). LiYbSe2 in a previously unreported pyrochlore lattice was discovered from LiCl flux growth. Distinct from the quantum spin liquid (QSL) candidate NaYbSe2 hosting a perfect triangular lattice of Yb3+, LiYbSe2 crystallizes in the cubic pyrochlore structure with space group Fd-3m (No. 227). The Yb3+ ions in LiYbSe2 are arranged on a network of corner-sharing tetrahedra, which is particu…
The pyrochlore lattice is associated with several potential and actual spin liquid phases as a result of its strong geometric frustration. At finite temperature, these can exhibit an unusually broad cross-over regime to a conventional paramagnet. Here, we study this regime analytically by showing how a single-tetrahedron Hamiltonian can extrapolate beyond the first term of a high-temperature expansion and yield insights into the build-up of correlations. We discuss how this unusual behaviour is brought about by the structure of the eigenspaces of the coupling matrix. Further interesting behavi…
Magnetic transition, long-range order, and moment fluctuations in the pyrochlore iridate Eu2Ir2O7
μ子自旋旋转和弛豫实验中的烧绿石铱酸盐Eu 2 Ir 2 O 7产生一个明确的μ子自旋进动频率低于金属-绝缘体/反铁磁转变温度TM = 120 K,表示远程相称的磁秩序,从而排除了量子自旋液体和自旋玻璃样基态。动态μ子自旋弛豫速率在2 K和~TM之间与温度无关,并产生了非常长的Ir^{4+}自旋相关时间,表明低位自旋激发的奇异密度。类似的行为被发现在其他pyrophores和几何挫折系统,但也在unfrustrated iridate BaIrO 3。Eu 2 Ir 2 O 7可能只有微弱的阻挫;如果是这样的话,奇异性可能与小能隙绝缘态有关,而不是阻挫。
Nonequilibrium low temperature phase in pyrochlore iridate Y$_2$Ir$_2$O$_7$: Possibility of glass-like dynamics
几何阻挫效应和自旋轨道耦合效应共同影响着烧绿石基铱氧化物的性质。本文研究了烧绿石铱酸盐Y $_2$ Ir $_2$ O $_7$的结构、磁性、热力学和输运性质。磁化强度数据显示,在温度$T_{irr}$ $\sim$ 160 K附近出现磁不可逆性,然而,在低于$T_{irr}$的温度下没有观察到长程型铁磁有序的迹象。比热数据显示在$T_{irr}$上没有明显的异常,数据分析表明在费米能级上有相当大的态密度。随温度变化的X-射线衍射测量表明,在结构对称性没有变化到低温。另一方面,该材料显示出类似于玻璃态动力学的显著弛豫和老化行为。在这个高度绝缘的系统中的电子电荷输运被发现遵循幂律依赖与温度。该材料表现出负磁电阻效应,并用量子干涉效应解释了这一现象。
Structural properties of the geometrically frustrated pyrochlore Tb2Ti2O7
虽然理论上表现出最近邻反铁磁相互作用和几何挫折的材料在没有无序的情况下不应该磁有序,但很少有这样的系统被实验观察到。一个这样的系统似乎是烧绿石Tb 2 Ti 2 O 7。然而,以前的结构研究表明,Tb_2Ti_2O_7是一个不完美的烧绿石。为了澄清这种情况,我们进行了中子粉末衍射(NPD)和X射线吸收精细结构(XAFS)的样品上的测量,这些样品是相同的制备,显示没有磁序。NPD测量结果表明,Tb_2Ti_2O_7的长程有序结构在4.5 ~ 600 K之间没有发生结构转变。具体而言,每个部位的均方位移(u^2)遵循无偏移的德拜模型。在2%的上限内,没有观察到Tb/Ti位点互换的证据。同样,在标称烧绿石值的2%的上限内,没有观察到氧化学计量的过量或不足。Tb L3-和Ti K-边XAFS测量从20-300 K类似地表明一个良好有序的局部结构。考虑了结构的其他方面。我们得出结论,Tb 2 Ti 2 O 7具有,在实验误差范围内,一个理想的,无序的烧绿石晶格,从而使系统保持在一个动态的,受挫的自旋状态的最低观测温度。
Pyrochlore iridates and pyrochlore ices are two families of materials where novel quantum phenomena are intertwined with strong spin-orbit coupling, substantial electron correlation and geometrical frustration. Motivated by the puzzling experiments on two pyrochlore systems Pr2Ir2O7 and Yb2Ti2O7, we study the proximate Ising orders and the quantum phase transition out of quantum spin ice U(1) quantum spin liquid (QSL). We apply the electromagnetic duality of the compact quantum electrodynamics to analyze the "magnetic monopoles" condensation for U(1) QSL. The monopole condensation transition r…
The pyrochlore lattice involves corner sharing tetrahedra and the resulting geometric frustration is believed to suppress any antiferromagnetic order for Mott insulators on this structure. There are nevertheless short-range correlations which could be vital near the Mott-Hubbard insulator-metal transition. We use a static auxiliary-field-based Monte Carlo to study this problem in real space on reasonably large lattices. The method reduces to unrestricted Hartree-Fock at zero temperature but captures the key magnetic fluctuations at finite temperature. Our results reveal that increasing interac…
We predict magnetisation plateaux ground states for $S=1/2$ Heisenberg antiferromagnets on pyrochlore lattices by formulating arguments based on gauge and spin-parity transformations. We derive a twist operator appropriate to the pyrochlore lattice, and show that it is equivalent to a large gauge transformation. Invariance under this large gauge transformation indicates the sensitivity of the ground state to changes in boundary conditions. This leads to the formulation of an Oshikawa-Yamanaka-Affleck (OYA)-like criterion at finite external magnetic field, enabling the prediction of plateaux in…
The kagome lattice is a paragon of geometrical frustration, long-studied for its association with novel ground-states including spin liquids (SLs). Many recently synthesized kagome materials feature rare-earth ions, which may be expected to exhibit highly anisotropic exchange interactions. The consequences of this combination of strong exchange anisotropy and extreme geometrical frustration are yet to be fully understood. Here, we establish a general picture of the interactions and resulting ground-states (GSs) arising from nearest neighbour exchange anisotropy on the kagome lattice. We determ…
The family of magnetic rare-earth pyrochlore oxides R2M2O7 plays host to a diverse array of exotic phenomena, driven by the interplay between geometrical frustration and spin-orbit interaction, which leads to anisotropy in both magnetic moments and their interactions. In this article we establish a general, symmetry--based theory of pyrochlore magnets with anisotropic exchange interactions. Starting from a very general model of nearest-neighbour exchange between Kramers ions, we find four distinct classical ordered states, all with q=0, competing with a variety of spin-liquids and unconvention…
Motivated by the proposal of a Weyl-semimetal phase in pyrochlore iridates, we consider a Hubbard-type model on the pyrochlore lattice. To shed light on the question as to why such a state has not been observed experimentally, its robustness is analyzed. On the one hand, we study the possible phases when the system is doped. Magnetic frustration favors several phases with magnetic and charge order that do not occur at half filling, including additional Weyl-semimetal states close to quarter filling. On the other hand, we search for density waves that break translational symmetry and destroy th…
Spin-lattice coupling in frustrated antiferromagnets
本文综述了自旋-晶格耦合在消除烧绿石反铁磁体,特别是尖晶石氧化物的几何阻挫中的作用机制。烧绿石晶格的组成单元四面体单元在晶格自由度与反铁磁性耦合时发生自旋驱动的Jahn-Teller不稳定性。通过限制我们的考虑,以保持平移对称性的晶格的扭曲,我们提出了一个一般的理论,集体自旋Jahn-Teller效应的烧绿石晶格。预测的晶格畸变之一打破了反转对称性,并产生了手性烧绿石晶格,其中受挫键形成具有一定手性的螺旋。手性通过自旋轨道耦合转移到自旋系统,导致长周期螺旋状态,如在尖晶石CdCr 2 O 4中观察到的。我们讨论了利用局域声子模的自旋-晶格耦合的显式模型,以及它们在其他阻挫磁体中的应用。
The two orbital Hubbard model, with the electrons additionally coupled to a complex magnetic background, arises in the pyrochlore molybdates. The background involves local moments Hund's coupled to the electrons, driving double exchange ferromagnetism, and antiferromagnetic (AF) tendency arising from competing superexchange. The key scales include the Hubbard repulsion and the superexchange, both of which can be tuned in these materials. They control the phase transition from a ferromagnetic metal to a spin glass metal and then to a spin glass (Mott) insulator. We provide a comprehensive descr…
Pyrochlore iridates A2Ir2O7 (A = rare earth elements, Y or Bi) hold great promise for realizing novel electronic and magnetic states owing to the interplay of spin-orbit coupling, electron correlation and geometrical frustration. A prominent example is the formation of all-in/all-out (AIAO)antiferromagnetic order in the Ir4+ sublattice that comprises of corner-sharing tetrahedra. Here we report on an unusual magnetic phenomenon, namely a cooling-field induced shift of magnetic hysteresis loop along magnetization axis, and its possible origin in pyrochlore iridates with non-magnetic Ir defects …