Magnetism and ferroelectricity are essential to many forms of current technology, and the quest for multiferroic materials, where these two phenomena are intimately coupled, is of great technological and fundamental importance. Ferroelectricity and magnetism tend to be mutually exclusive and interact weakly with each other when they coexist. The exciting new development is the discovery that even a weak magnetoelectric interaction can lead to spectacular cross-coupling effects when it induces electric polarization in a magnetically ordered state. Such magnetic ferroelectricity, showing an unprecedented sensitivity to ap plied magnetic fields, occurs in 'frustrated magnets' with competing interactions between spins and complex magnetic orders. We summarize key experimental findings and the current theoretical understanding of these phenomena, which have great potential for tuneable multifunctional devices.

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Multiferroics: a magnetic twist for ferroelectricity

Multiferroics, defined for those multifunctional materials in which two or more kinds of fundamental ferroicities coexist, have become one of the hottest topics of condensed matter physics and materials science in recent years. The coexistence of several order parameters in multiferroics brings out novel physical phenomena and offers possibilities for new device functions. The revival of research activities on multiferroics is evidenced by some novel discoveries and concepts, both experimentally and theoretically. In this review, we outline some of the progressive milestones in this stimulating field, especially for those single-phase multiferroics where magnetism and ferroelectricity coexist. First, we highlight the physical concepts of multiferroicity and the current challenges to integrate the magnetism and ferroelectricity into a single-phase system. Subsequently, we summarize various strategies used to combine the two types of order. Special attention is paid to three novel mechanisms for multiferroicity generation: (1) the ferroelectricity induced by the spin orders such as spiral and E-phase antiferromagnetic spin orders, which break the spatial inversion symmetry; (2) the ferroelectricity originating from the charge-ordered states; and (3) the ferrotoroidic system. Then, we address the elementary excitations such as electromagnons, and the application potentials of multiferroics. Finally, open questions and future research opportunities are proposed.

Multiferroicity: the coupling between magnetic and polarization orders

Quantum impurity models describe an atom or molecule embedded in a host material with which it can exchange electrons. They are basic to nanoscience as representations of quantum dots and molecular conductors and play an increasingly important role in the theory of "correlated electron" materials as auxiliary problems whose solution gives the "dynamical mean field" approximation to the self energy and local correlation functions. These applications require a method of solution which provides access to both high and low energy scales and is effective for wide classes of physically realistic models. The continuous-time quantum Monte Carlo algorithms reviewed in this article meet this challenge. We present derivations and descriptions of the algorithms in enough detail to allow other workers to write their own implementations, discuss the strengths and weaknesses of the methods, summarize the problems to which the new methods have been successfully applied and outline prospects for future applications.

Continuous-time Monte Carlo methods for quantum impurity models

This article discusses fluctuating order in a quantum disordered phase proximate to a quantum critical point, with particular emphasis on fluctuating stripe order. Optimal strategies are derived for extracting information concerning such local order from experiments, with emphasis on neutron scattering and scanning tunneling microscopy. These ideas are tested by application to two model systems---an exactly solvable one-dimensional (1D) electron gas with an impurity, and a weakly interacting 2D electron gas. Experiments on the cuprate high-temperature superconductors which can be analyzed using these strategies are extensively reviewed. The authors adduce evidence that stripe correlations are widespread in the cuprates. They compare and contrast the advantages of two limiting perspectives on the high-temperature superconductor: weak coupling, in which correlation effects are treated as a perturbation on an underlying metallic (although renormalized) Fermi-liquid state, and strong coupling, in which the magnetism is associated with well-defined localized spins, and stripes are viewed as a form of micro phase separation. The authors present quantitative indicators that the latter view better accounts for the observed stripe phenomena in the cuprates.

How to detect fluctuating stripes in the high-temperature superconductors

Resonant Inelastic X-ray Scattering (RIXS)
 is an X-ray in, X-ray out technique that enables one to study the 
dispersion of excitations in solids. In this thesis, we investigated how
 various elementary excitations of transition metal oxides show up in 
RIXS spectra.

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Resonant Inelastic X-ray Scattering Studies of Elementary Excitations

${\mathrm{TbMnO}}_{3}$ is an orthorhombic insulator where incommensurate spin order for temperature ${T}_{N}l41\text{ }\text{ }\mathrm{K}$ is accompanied by ferroelectric order for $Tl28\text{ }\text{ }\mathrm{K}$. To understand this, we establish the magnetic structure above and below the ferroelectric transition using neutron diffraction. In the paraelectric phase, the spin structure is incommensurate and longitudinally modulated. In the ferroelectric phase, however, there is a transverse incommensurate spiral. We show that the spiral breaks spatial inversion symmetry and can account for magnetoelectricity in ${\mathrm{TbMnO}}_{3}$.

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Magnetic inversion symmetry breaking and ferroelectricity in TbMnO3

High-transition-temperature (high-T(c)) superconductivity develops near antiferromagnetic phases, and it is possible that magnetic excitations contribute to the superconducting pairing mechanism. To assess the role of antiferromagnetism, it is essential to understand the doping and temperature dependence of the two-dimensional antiferromagnetic spin correlations. The phase diagram is asymmetric with respect to electron and hole doping, and for the comparatively less-studied electron-doped materials, the antiferromagnetic phase extends much further with doping and appears to overlap with the superconducting phase. The archetypal electron-doped compound Nd2-xCexCuO4+/-delta (NCCO) shows bulk superconductivity above x approximately 0.13 (refs 3, 4), while evidence for antiferromagnetic order has been found up to x approximately 0.17 (refs 2, 5, 6). Here we report inelastic magnetic neutron-scattering measurements that point to the distinct possibility that genuine long-range antiferromagnetism and superconductivity do not coexist. The data reveal a magnetic quantum critical point where superconductivity first appears, consistent with an exotic quantum phase transition between the two phases. We also demonstrate that the pseudogap phenomenon in the electron-doped materials, which is associated with pronounced charge anomalies, arises from a build-up of spin correlations, in agreement with recent theoretical proposals.

Spin correlations in the electron-doped high-transition-temperature superconductor Nd2-xCexCuO4+/-delta.

Hexagonal HoMnO3 is a frustrated antiferromagnet (T(N)=72 K) ferroelectric (T(C)=875 K) in which these two order parameters are coupled. Our neutron measurements of the spin-wave dispersion for the S=2 Mn3+ on the layered triangular lattice are well described by a two-dimensional nearest-neighbor Heisenberg exchange J=2.44 meV, and an anisotropy D that is 0.28 meV above the spin-reorientation transition at 40 K and 0.38 meV below. For H parallel c the magnetic structures and phase diagram have been determined, and reveal additional transitions below 8 K where the ferroelectrically displaced Ho3+ ions are ordered magnetically.

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Magnetic order and spin dynamics in ferroelectric HoMnO3.

The study of randomness in low-dimensional quantum antiferromagnets is at the forefront of research in the field of strongly correlated electron systems, yet there have been relatively few experimental model systems. Complementary neutron scattering and numerical experiments demonstrate that the spin-diluted Heisenberg antiferromagnet La2Cu1– z (Zn,Mg) z O4is an excellent model material for square-lattice site percolation in the extreme quantum limit of spin one-half. Measurements of the ordered moment and spin correlations provide important quantitative information for tests of theories for this complex quantum-impurity problem.

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Owen Vajk

Papers

Magnetic inversion symmetry breaking and ferroelectricity in TbMnO3

Spin correlations in the electron-doped high-transition-temperature superconductor Nd2-xCexCuO4+/-delta.

Magnetic order and spin dynamics in ferroelectric HoMnO3.

Quantum Impurities in the Two-Dimensional Spin One-Half Heisenberg Antiferromagnet

Crystal Growth and Characterization of the Model High‐Temperature Superconductor HgBa2CuO4+δ