A frustrated system is one whose symmetry precludes the possibility that every pairwise interaction (“bond”) in the system can be satisfied at the same time. Such systems are common in all areas of physical and biological science. In the most extreme cases, they can have a disordered ground state with “macroscopic” degeneracy; that is, one that comprises a huge number of equivalent states of the same energy. Pauling9s description of the low-temperature proton disorder in water ice was perhaps the first recognition of this phenomenon and remains the paradigm. In recent years, a new class of magnetic substance has been characterized, in which the disorder of the magnetic moments at low temperatures is precisely analogous to the proton disorder in water ice. These substances, known as spin ice materials, are perhaps the “cleanest” examples of such highly frustrated systems yet discovered. They offer an unparalleled opportunity for the study of frustration in magnetic systems at both an experimental and a theoretical level. This article describes the essential physics of spin ice, as it is currently understood, and identifies new avenues for future research on related materials and models.

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Spin ice state in frustrated magnetic pyrochlore materials.

Within the past 20 years or so, there has occurred an explosion of interest in the magnetic behavior of pyrochlore oxides of the type $A_{2}^{3+}$$B_{2}^{4+}$O$_{7}$ where $A$ is a rare-earth ion and $B$ is usually a transition metal. Both the $A$ and $B$ sites form a network of corner-sharing tetrahedra which is the quintessential framework for a geometrically frustrated magnet. In these systems the natural tendency to form long range ordered ground states in accord with the Third Law is frustrated, resulting in some novel short range ordered alternatives such as spin glasses, spin ices and spin liquids and much new physics. This article attempts to review the myriad of properties found in pyrochlore oxides, mainly from a materials perspective, but with an appropriate theoretical context.

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Magnetic Pyrochlore Oxides

The current state of efforts to understand the phenomenon of geometric magnetic frustration is described in the context of several key materials. All are transition metal oxides which crystallize with magnetic lattices which are geometrically or topologically prone to frustration such as those based on triangles or tetrahedra which share corners, edges or faces. These include the anhydrous alums, jarosites, pyrochlores, spinels, magnetoplumbites, garnets, ordered NaCl and other structure types. Special attention is paid to materials which do not undergo long range ordering at the lowest temperatures but instead form exotic ground states such as spin glasses, spin liquids and spin ices, and to S = 1/2 based materials.

Geometrically frustrated magnetic materials

The spin ice materials, including Ho2Ti2O7 and Dy2Ti2O7, are rare-earth pyrochlore magnets which, at low temperatures, enter a constrained paramagnetic state with an emergent gauge freedom. Spin ices provide one of very few experimentally realized examples of fractionalization because their elementary excitations can be regarded as magnetic monopoles and, over some temperature range, spin ice materials are best described as liquids of these emergent charges. In the presence of quantum fluctuations, one can obtain, in principle, a quantum spin liquid descended from the classical spin ice state characterized by emergent photon-like excitations. Whereas in classical spin ices the excitations are akin to electrostatic charges with a mutual Coulomb interaction, in the quantum spin liquid these charges interact through a dynamic and emergent electromagnetic field. In this review, we describe the latest developments in the study of such a quantum spin ice, focusing on the spin liquid phenomenology and the kinds of materials where such a phase might be found.

https://iopscience.iop.org/article/10.1088/0034-4885/77/5/056501/pdf

Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets

The large degeneracy of states resulting from the geometrical frustration of competing interactions is an essential ingredient of important problems in fields as diverse as magnetism, protein folding and neural networks. As first explained by Pauling, geometrical frustration of proton positions is also responsible for the unusual low-temperature thermodynamics of ice and its measured 'ground state' entropy. Recent work has shown that the geometrical frustration of ice is mimicked by Dy2Ti2O7, a site-ordered magnetic material in which the spins reside on a lattice of corner-sharing tetrahedra where they form an unusual magnetic ground state known as 'spin ice'. Here we identify a cooperative spin-freezing transition leading to the spin-ice ground state in Dy2Ti2O7. This transition is associated with a very narrow range of relaxation times, and represents a new form of spin-freezing. The dynamics are analogous to those associated with the freezing of protons in ice, and they provide a means through which to study glass-like behaviour and the consequences of frustration in the limit of low disorder.

How ‘spin ice’ freezes

Neutron time-of-flight spectroscopy has been employed to study the crystal-field interaction in the pyrochlore titanate Ho2Ti2O7. The crystal-field parameters and corresponding energy-level scheme have been determined from a profile fit to the observed neutron spectra. The ground state is a well separated Eg doublet with a strong Ising-like anisotropy, which can give rise to frustration in the pyrochlore lattice. Using the crystal-field parameters determined for the Ho compound as an estimate of the crystal-field potential in other pyrochlore magnets, we also find the Ising type behavior for Dy. In contrast, the almost planar anisotropy found for Er and Yb prevents frustration, because of the continuous range of possible spin orientations in this case.

https://digital.library.unt.edu/ark:/67531/metadc711960/m2/1/high_res_d/750480.pdf

Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7

We study the sawtooth lattice of a coupled spin 1/2 Heisenberg system, a variant of the railroad-trestle lattice. The ground state of this system is twofold degenerate with periodic boundary conditions and supports kink-antikink excitations, which are distinct in this case, unlike the railroad-trestle lattice. The resulting low-temperature thermodynamics is compared with the recently discovered delafossites ${\mathrm{YCuO}}_{2.5}$. \textcopyright{} 1996 the American Physical Society.

B. S. Shastry

Papers

Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7

Quantum solitons in the sawtooth lattice