Frustrated three dimensional quantum magnets are notoriously impervious to theoretical analysis. Here we use a combination of three computational methods to investigate the three dimensional pyrochlore $S=1/2$ quantum antiferromagnet, an archetypical frustrated magnet, at finite temperature, $T$: canonical typicality for a finite cluster of $2\times 2 \times 2$ unit cells (i.e. $32$ sites), a finite-$T$ matrix product state method on a larger cluster with $48$ sites, and the numerical linked cluster expansion (NLCE) using clusters up to $25$ lattice sites, which include non-trivial hexagonal and octagonal loops. We focus on thermodynamic properties (energy, specific heat capacity, entropy, susceptibility, magnetisation) next to the static structure factor. We find a pronounced maximum in the specific heat at $T = 0.57 J$, which is stable across finite size clusters and converged in the series expansion. This is well-separated from a residual amount of spectral weight of $0.47 k_B \ln 2$ per spin which has not been released even at $T\approx0.25 J$, the limit of convergence of our results. This is a large value compared to a number of highly frustrated models and materials, such as spin ice or the kagome $S=1/2$ Heisenberg antiferromagnet. We also find a non-monotonic dependence on $T$ of the magnetisation at low magnetic fields, reflecting the dominantly non-magnetic character of the low-energy spectral weight. A detailed comparison of our results to measurements for the $S=1$ material NaCaNi$_2$F$_7$ yields rough agreement of the functional form of the specific heat maximum, which in turn differs from the sharper maximum of the heat capacity of the spin ice material Dy$_2$Ti$_2$O$_7$, all of which are yet qualitatively distinct from conventional, unfrustrated magnets.
This short note documents some of the pyrochlore magnetization plateaus resulting from the arguments of Pal & Lal that were not mentioned in arxiv:1902.06475v1. These are (layered) "Kagome"-like plateaus that are commensurate with the pyrochlore lattice, including an exact wavefunction for the $\frac{m}{m_s} = \frac{5}{6}$ plateau state.
We investigate the zero- and finite-temperature properties of the bond-random $s=1/2$ Heisenberg antiferromagnet on the pyrochlore lattice by the exact diagonalization and the Hams--de Raedt methods. We find that the randomness induces the gapless quantum spin liquid (QSL) state, the random-singlet state. Implications to recent experiments on the mixed-anion pyrochlore-lattice antiferromagnet Lu$_2$Mo$_2$O$_5$N$_2$ exhibiting gapless QSL behaviors are discussed.
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…
We use the rotation-invariant Green's function method (RGM) and the high-temperature expansion (HTE) to study the thermodynamic properties of the spin-$S$ Heisenberg ferromagnet on the pyrochlore lattice. We examine the excitation spectra as well as various thermodynamic quantities, such as the order parameter (magnetization), the uniform static susceptibility, the correlation length, the spin-spin correlations, and the specific heat, as well as the static and dynamic structure factors. We discuss the influence of the spin quantum number $S$ on the temperature dependence of these quantities. W…
We study the low-temperature physics of the $SU(2)$-symmetric spin-$1/2$ Heisenberg antiferromagnet on a pyrochlore lattice and find fingerprint evidence for the thermal spin-ice state in this frustrated quantum magnet. Our conclusions are based on the results of bold diagrammatic Monte Carlo simulations, with good convergence of the skeleton series down to the temperature $T/J=1/6$. The identification of the spin-ice state is done through a remarkably accurate microscopic correspondence for the static structure factor between the quantum Heisenberg, classical Heisenberg, and Ising models at a…
We present the results of an exact diagonalization study of the spin-1/2 Heisenberg antiferromagnet on a two-dimensional version of the pyrochlore lattice, also known as the square lattice with crossings or the checkerboard lattice. Examining the low energy spectra for systems of up to 24 spins, we find that all clusters studied have non-degenerate ground states with total spin zero, and big energy gaps to states with higher total spin. We also find a large number of non-magnetic excitations at energies within this spin gap. Spin-spin and spin-Peierls correlation functions appear to be short-r…
Absent pinch points and emergent clusters: further neighbour interactions in the pyrochlore Heisenberg antiferromagnet
我们讨论的起源自旋相关性中子散射实验中观察到的顺磁相的一些挫折尖晶石化合物，最显着的ZnCr 2 O 4。这些相关性令人震惊，原因有二。首先，它们被解释为弱相互作用的六边形自旋簇形成的证据。其次，它们与最近邻海森堡烧绿石反铁磁体的计算结果非常不同，其中库仑相位相关产生尖锐的散射特征，称为夹点。使用大- $n$计算和蒙特卡罗模拟，我们表明，非常弱的进一步邻居交换相互作用可以占两个明显的形成集群和抑制的夹点。
Magnetic phase diagram of the antiferromagnetic pyrochlore Gd2Ti2O7
Gd 2 Ti 2 O 7是烧绿石晶格上的高度受抑的反铁磁体，除了海森堡交换之外，自旋还通过偶极-偶极力相互作用。本文报道了在三个不同方向的外加磁场作用下对Gd_2 Ti_2 O_7单晶进行的低温比热测量。测量结果显示，强烈的各向异性行为的Gd 2 Ti 2 O 7在磁场中，尽管明显缺乏一个显着的单离子各向异性的Gd 3+。给出了H//[111]、H//[110]和H//[112]的H-T相图。结果表明，进一步的理论工作超出了一个简单的平均场模型是必要的。
Field-Driven Transitions in the Dipolar Pyrochlore Antiferromagnet Gd$_2$Ti$_2$O$_7$
本文提出了偶极耦合的钛酸钆Gd $_2$ Ti $_2$ O $_7$焦绿石体系中磁场驱动跃迁的平均场论.低温中子散射产生的相，可以被看作是一个8亚晶格反铁磁体，其中长程有序矩和涨落矩共存。我们的理论给出了实现这样一个阶段的参数区域，并预测了其他几个阶段，它们之间的过渡由磁场以及温度驱动。我们发现了几个实例{ \em本地}无序参数描述的过渡。
In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature dependences of the magnetic susceptibility and heat capacity, and the magnetization curve are consistent with those of an $S$ = 5/2 pyrochlore lattice antiferromagnet with nearest-neighbor interactions of 2 …
We address the ground-state properties of the long-standing and much-studied three-dimensional quantum spin liquid candidate, the $S=\frac 1 2$ pyrochlore Heisenberg antiferromagnet. By using $SU(2)$ density-matrix renormalization group (DMRG), we are able to access cluster sizes of up to 128 spins. Our most striking finding is a robust spontaneous inversion symmetry breaking, reflected in an energy density difference between the two sublattices of tetrahedra, familiar as a starting point of earlier perturbative treatments. We also determine the ground-state energy, $E_0/N_\text{sites} = -0.49…
Valence bond crystal in a pyrochlore antiferromagnet with orbital degeneracy
本文讨论了三重轨道简并$S=1/2$磁性离子的烧绿石晶格的基态。我们推导出一个有效的自旋轨道哈密顿量，并表明轨道自由度可以调制自旋交换，消除无限自旋简并烧绿石结构的特点。由此产生的状态是自旋单重态二聚体的集合，由于它们的相对取向而具有残余简并性。后者被磁弹性相互作用提升，在自旋单态相空间中诱导，迫使四重态畸变。这种理论为在B-尖晶石MgTi $_2$ O $_4$中观察到的螺旋自旋单态模式提供了解释。
We address the long-standing problem of the microscopic origin of the richly diverse phenomena in the chromium breathing pyrochlore material family. Combining electronic structure and renormalization group techniques we resolve the magnetic interactions and analyze their reciprocal-space susceptibility. We show that the physics of these materials is principally governed by long-range Heisenberg Hamiltonian interactions, a hitherto unappreciated fact. Our calculations uncover that in these isostructural compounds, the choice of chalcogen triggers a proximity of the materials to classical spin l…
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 investigate the quantum Heisenberg model on the pyrochlore lattice for a generic spin $S$ in the presence of nearest-neighbor $J_{1}$ and second-nearest-neighbor $J_{2}$ exchange interactions. By employing the pseudofermion functional renormalization group method, we find, for $S=1/2$ and $S=1$, an extended quantum-spin-liquid phase centered around $J_{2}=0$, which is shown to be robust against the introduction of breathing anisotropy. The effects of temperature, quantum fluctuations, breathing anisotropies, and a $J_{2}$ coupling on the nature of the scattering profile, and the pinch point…
In frustrated magnetic systems, geometric constraints or the competition amongst interactions introduce extremely high degeneracy and prevent the system from readily selecting a low-temperature ground state. The most frustrated known spin arrangement is on the pyrochlore lattice, but nearly all magnetic pyrochlores have unquenched orbital angular momentum, constraining the spin directions through spin-orbit coupling. Pyrochlore Mn$_2$Sb$_2$O$_7$ is an extremely rare Heisenberg pyrochlore system, with directionally-unconstrained spins and low chemical disorder. We show that it undergoes a spin-…
Frustrated quantum magnets not only provide exotic ground states and unusual magnetic structures, but also support unconventional excitations in many cases. Using a physically relevant spin model for a breathing pyrochlore lattice, we discuss the presence of topological linear band crossings of magnons in antiferromagnets. These are the analogs of Weyl fermions in electronic systems, which we dub Weyl magnons. The bulk Weyl magnon implies the presence of chiral magnon surface states forming arcs at finite energy. We argue that such antiferromagnets present a unique example in which Weyl points…
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…
Tenth-order high-temperature expansion for the susceptibility and the specific heat of spin-s Heisenberg models with arbitrary exchange patterns: Application to pyrochlore and kagome magnets
We investigate the ground-state properties of the nearest-neighbor $S=1$ pyrochlore Heisenberg antiferromagnet using two complementary numerical methods, density-matrix renormalization group (DMRG) and pseudofermion functional renormalization group (PFFRG). Within DMRG, we are able to reliably study clusters with up to 48 spins by keeping 20 000 SU(2) states. The investigated 32-site and 48-site clusters both show indications of a robust $C_3$ rotation symmetry breaking of the ground-state spin correlations and the 48-site cluster additionally features inversion symmetry breaking. Our PFFRG an…
The magnetization processes of the spin-3/2 antiferromagnet LiInCr4O8 comprising a "breathing" pyrochlore lattice, which is an alternating array of small and large tetrahedra, are studied under ultrahigh magnetic fields of up to 130 T using state-of-the-art pulsed magnets. A half magnetization plateau is observed above 90 T to 130 T, suggesting that LiInCr4O8 has a strong spin-lattice coupling, similar to conventional chromium spinel oxides. The magnetization of LiGa0.125In0.875Cr4O8, in which the structural and magnetic transitions at low temperatures have been completely suppressed, shows a …
We theoretically investigate spin-lattice coupling (SLC) effects on the in-field ordering properties of classical Heisenberg antiferromagnets on the breathing pyrochlore lattice. Here, we use the two possible simplified models describing the effect of local lattice distortions on the spin ordering via the SLC, the bond-phonon and site-phonon models. It is found by means of Monte Carlo simulations that in both models, the $\frac{1}{2}$ plateau shows up in the magnetization curve being relatively robust against the breathing bond-alternation, although magnetic long-range orders (LRO's) are reali…
Our polycrystalline sample study on the Yb-based chalcogenide spinels $A$Yb$_2$$X_4$ ($A =$ Cd, Mg, $X =$ S, Se) has revealed frustrated magnetism due to the antiferromagnetically coupled Heisenberg spin on the pyrochlore lattice. Our crystal electric field analysis indicates the Yb ground state has nearly Heisenberg spins with a strong quantum character of the ground doublet. All the materials exhibit an antiferromagnetic order at 1.4-1.8 K, much lower temperature than the antiferromagnetic exchange coupling scale of $\sim 10$ K. The magnetic specific heat $C_{\rm M}$ shows a $T^{3}$ dependen…
