Density-functional characterization of the multiferroicity in spin spiral chain cuprates

The ferroelectricity of the spiral magnets LiCu2O2 and LiCuVO4 was examined by calculating the electric polarizations of their spin spiral states on the basis of density-functional theory with spin-orbit coupling. Our work unambiguously reveals that spin-orbit coupling is responsible for the ferroelectricity with the primary contribution from the spin-orbit coupling on the Cu sites, but the asymmetric density distribution responsible for the electric polarization occurs mainly around the O atoms. The electric polarization is calculated to be much greater for the ab-plane than for the bc-plane spin spiral. The observed spin-spiral plane is found to be consistent with the observed direction of the electric polarization for LiCuVO4, but inconsistent for LiCu2O2.     

Magnetic ground state and transition of a quantum multiferroic LiCu2O2

Based on resonant soft x-ray magnetic scattering, we report that LiCu2O2 exhibits a large interchain coupling which suppresses quantum fluctuations along spin chains, and a quasi-2D short-range magnetic order prevails at temperatures above the magnetic transition. These observations unravel the fact that the ground state of LiCu2O2 possesses long-range 2D-like incommensurate magnetic order rather than being a gapped spin liquid as expected from the nature of quantum spin-1/2 chains. In addition, the spin coupling along the c axis is found to be essential for inducing electric polarization.     

Correlation between spin helicity and an electric polarization vector in quantum-spin chain magnet LiCu2O2

Measurements of polarized neutron scattering were performed on a S=1/2 chain multiferroic LiCu2O2. In the ferroelectric ground state with the spontaneous polarization along the c axis, the existence of transverse spiral spin component in the bc plane was confirmed. When the direction of electric polarization is reversed, the vector spin chirality as defined by C_(ij)=S_(i)xS_(j) (i and j being the neighboring spin sites) is observed to be reversed, indicating that the spin-current model or the inverse Dzyaloshinskii-Moriya mechanism is applicable even to this e_(g)-electron quantum-spin system. Differential scattering intensity of polarized neutrons shows a large discrepancy from that expected for the classical-spin bc-cycloidal structure, implying the effect of large quantum fluctuation.     

Theory of magnetic switching of ferroelectricity in spiral magnets

We propose a microscopic theory for magnetic switching of electric polarization (P) in the spin-spiral multiferroics by taking TbMnO3 and DyMnO3 as examples. We reproduce their phase diagrams under a magnetic field Hex by Monte Carlo simulation of an accurate spin model and reveal that competition among the Dzyaloshinskii-Moriya interaction, spin anisotropy, and spin exchange is controlled by the applied Hex, resulting in magnetic transitions accompanied by reorientation or vanishing of P. We also discuss the relevance of the proposed mechanisms to many other multiferroics such as LiCu2O2, MnWO4, and Ni3V2O4.     

Ferroelectricity in an s=1/2 chain cuprate

We report our discovery of ferroelectricity in the spiral-magnetic state in the quantum quasi-one-dimensional (1D) S=1/2 magnet of LiCu2O2. Electric polarization (P) emerges along the c direction below the spiral-magnetic order temperature, but changes from the c to a axis when magnetic fields (H) are applied along the b direction. We also found that P(c) increases with H(c), and P(a) appears with H(a). LiCu2O2 in zero field appears to be the first ferroelectric cuprate and also a prototypical example of the "1D spiral-magnetic ferroelectrics." However, the unexpected behavior in H may demonstrate the complexity of the ordered spin configuration, inherent in the 1D S=1/2 magnet of LiCu2O2.     

Competition between helimagnetism and commensurate quantum spin correlations in LiCu2O2

Neutron diffraction and bulk measurements are used to determine the nature of the low-temperature ordered state in LiCu2O2, a S=1/2 spin-chain compound with competing interactions. The spin structure is found to be helimagnetic, with a propagation vector (0.5,zeta,0), zeta=0.174. The nearest-neighbor exchange constant and frustration ratio are estimated to be J(1)=5.8 meV and J(2)/J(1)=0.29, respectively. For idealized quantum spin chains, these parameter values would signify a gapped spin-liquid ground state with commensurate spin correlations. The observed temperature dependence of the magnetic propagation vector in LiCu2O2 is attributed to a competition between incommensurate helimagnetism in the classical spin model and commensurability in the quantum case. It is also proposed that long-range ordering in LiCu2O2 is facilitated by intrinsic nonstoichiometry.     

Magnetic field control of ferroelectric polarization and magnetization of LiCu_2O_2 compound

A spin model of LiCu2O2 compound with ground state of ellipsoidal helical structure is adopted. Taking into account the interchain coupling and exchange anisotropy, we investigate the magnetoelectric properties in a rotating magnetic field and perform the Monte Carlo simulation on a two-dimensional lattice. A prominent anisotropic response is observed in both the magnetization curve and the polarization curve, qualitatively coinciding with the behaviors that are detected in the experiment. In addition, the influences of the magnetic field with various magnitudes on polarization are also explored and analyzed in detail. As the magnetic field increases, a much smoother polarization of angle dependence is exhibited,indicating the strong correlation between the magnetic and ferroelectric orders.     

Chiral order and electromagnetic dynamics in one-dimensional multiferroic cuprates

We show by unbiased numerical calculations that the ferromagnetic nearest-neighbor exchange interaction stabilizes a vector spin chiral order against the quantum fluctuation in a frustrated spin-1/2 chain relevant to multiferroic cuprates, LiCu2O2 and LiCuVO4. Our realistic semiclassical analyses for LiCu2O2 resolve controversies on the helical magnetic structure and unveil the pseudo-Nambu-Goldstone modes as the origin of experimentally observed electromagnons.     

Optical nuclear spin polarization in quantum dots

Hyperfine interaction between electron spin and randomly oriented nuclear spins is a key issue of electron coherence for quantum information/computation. We propose an efficient way to establish high polarization of nuclear spins and reduce the intrinsic nuclear spin fluctuations. Here, we polarize the nuclear spins in semiconductor quantum dot(QD) by the coherent population trapping(CPT) and the electric dipole spin resonance(EDSR) induced by optical fields and ac electric fields. By tuning the optical fields, we can obtain a powerful cooling background based on CPT for nuclear spin polarization. The EDSR can enhance the spin flip–flop rate which may increase the cooling efficiency. With the help of CPT and EDSR, an enhancement of 1300 times of the electron coherence time can be obtained after a 10-ns preparation time.     

Stimulated polarization wave process in spin 3/2 chains

Stimulated wave of polarization, triggered by a flip of a single spin, presents a simple model of quantum amplification. Recently, it has been demonstrated that, in an idealized one-dimensional Ising spin 1/2 chain with nearest-neighbor interactions and realistic spin 1/2 chain including the natural dipole-dipole interactions, irradiated by a weak resonant transverse field, a wave of flipped spins can be triggered by a single spin flip. Here we focuse on control of polarization wave in chain of spin 3/2, where the nuclear quadrupole interaction is dominant. Results of simulations for 1D spin chains and rings with up to five spins are presented.     

Direct evidence for a dynamical ground state in the highly frustrated Tb(2)Sn(2)O(7) pyrochlore

mSR experiments have been performed on a powder sample of the "ordered spin ice" Tb(2)Sn(2)O(7) pyrochlore. At base temperature (T=35 mK), the muon relaxation is found to be of dynamical nature, which demonstrates that strong fluctuations persist below the ferromagnetic transition (T(C)=0.87 K). Hints of long-range ordering appear as oscillations of the muon polarization when an external field is applied and also as a hysteretic behavior below T(C). We propose that dynamics results from fluctuations of clusters of correlated spins with the ordered spin ice structure.     

Spin-lattice interaction in the quasi-one-dimensional helimagnet LiCu2O2

The field dependence of the electron spin resonance in a helimagnet LiCu2O2 was investigated for the first time. In the paramagnetic state, a broad resonance line was observed corresponding to a g factor of 2.3. In the critical regime, around the paramagnetic to helimagnetic phase transition the resonance broadens and shifts to higher frequencies. A narrow signal is recovered at a low temperature, corresponding to a spin gap of 1.4 meV in zero field. A comprehensive model of the magnons is presented, using exchange parameters from neutron scattering [T. Masuda Phys. Rev. B 72, 014405 (2005)10.1103/PhysRevB.72.014405] and the spin anisotropy determined here. The role of the quantum fluctuations is discussed.     

On the nuclear magnetoelectric resonance in tetragonal KNbO3

The magnetic response of a KNbO₃ crystal due to the nuclear spin precession resulting from the excitation of nuclear spins by an alternating electric field has been investigated theoretically. The converse effect, i.e., the emergence of an alternating electrical polarization as a result of the magnetic excitation of nuclear spins, has also been considered.     

Ferroelectricity driven by the noncentrosymmetric magnetic ordering in multiferroic TbMn(2)O(5): a first-principles study

The ground state structural, electronic, and magnetic properties of multiferroic TbMn(2)O(5) are investigated via first-principles calculations. We show that the ferroelectricity in TbMn(2)O(5) is driven by the noncentrosymmetric magnetic ordering, without invoking the spin-orbit coupling and noncollinear spins. The intrinsic electric polarization in this compound is calculated to be 1187 nC cm(-2), an order of magnitude larger than previously thought.     

On the nuclear electric resonance in ferroelectric KNbO<Subscript>3</Subscript>

The pulse electric excitation of nuclear spins in the KNbO₃ crystal and the electric polarization response caused by the nuclear spin precession were theoretically studied. Equations for a 90-degree exciting pulse and the amplitude of the nuclear response are derived, and numerical evaluations are performed.     

Indirect magnetic exchange interaction mediated by bound Landau states in 2DES

The possibility of indirect exchange coupling mediated by Landau electrons bound to magnetic impurities in 2DES is studied here. The importance of the resonance scattering of the Landau electrons with the impurities is emphasized due to its spin selectivity which results in strong spin polarization of the localized Landau states. The bound Landau states act as mediators of the superexchange interaction resulting in an antiferromagnetic interaction between the nuclear spins of the impurities. The coupling constant, between these nuclear spins, J, is presented for the case of a weak scattering limit and found to depend strongly on the ratio of the impurity separation over the magnetic length. Possible applications of these results may include a long-range mechanism for coupling between two nuclear spins to be used as a qubits interaction with a spacing distance of the order of the magnetic length.     

Theory of the transition at 0.2 K in Ni-doped Bi2Sr2CaCu2O8

A theory is put forward that the electronic phase transition at 0.2 K in Ni-doped Bi2Sr2CaCu2O8 is a result of the formation of a spin density wave in the system of Ni impurities. The driving force for the transition is the exchange interaction between the impurity spins and the spins of the conduction electrons. This creates a small gap at two of the four nodes of the superconducting gap. The effect is to reduce the thermal conductivity by a factor of 2, as observed.     

Optical orientation of Mn2+ ions in GaAs in weak longitudinal magnetic fields

We report on optical orientation of Mn2+ ions in bulk GaAs subject to weak longitudinal magnetic fields (B≤100 mT). A manganese spin polarization of 25% is directly evaluated by using spin-flip Raman scattering. The dynamical Mn2+ polarization occurs due to the s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence reveals a nontrivial electron spin dynamics, where the oriented Mn2+ ions tend to stabilize the electron spins.     

Coherent Polarization Transfer Effects Are Crucial for Interpreting Low-Field CIDNP Data

In this work we demonstrate that low-field chemically induced dynamic nuclear polarization (CIDNP) is strongly affected by re-distribution of polarization, which is formed in the course of spin evolution in transient radical pairs, in diamagnetic reaction products. This phenomenon is of importance when the spins of the reaction product are coupled strongly meaning that spin–spin interactions between them are comparable to the differences in their Zeeman interactions with the external magnetic field. In this case, polarization transfer relies on a coherent mechanism; as a consequence, spins can acquire significant polarization even when they have no hyperfine coupling to the electron spins in the radical pairs, i.e., cannot be polarized directly by CIDNP. This is demonstrated by taking CIDNP of n-butylamine as an example: in this case only the α-CH₂ protons are polarized directly, which is confirmed by high-field CIDNP, whereas the β-CH₂, γ-CH₂ and δ-CH₃ protons get polarized only indirectly due to the transfer of polarization from the α-CH₂ protons. These results show that low-field CIDNP data should be interpreted with care to discriminate between the effects of spin evolution in transient radical pairs and in diamagnetic reaction products.     

Solid-state NMR spectroscopy using the lost I spin magnetization in polarization transfer experiments

A variation of the cross polarization (CP) experiment is discussed. The method requires two scans where the difference signal is equivalent to the I spin magnetization that is transferred to the S spins. The acquired signal is equivalent to F1 sum projection of a two-dimensional (2D) heteronuclear correlation experiment and is obtained by just two scans without the need to increment the indirect time domain t(1). Any polarization transfer method and any kind of spin manipulations during the t(1) incrementation period of a 2D NMR experiment can be applied. The method allows fast measurements of the CP transfer, particularly if various S spins signal overlap and is good for spectral editing of I spin signals with contact to S spins. Various examples for biomaterials are presented. Most importantly, this novel approach is ideal for detailed investigations of organic-mineral interfaces in bone, here demonstrated for O-phospho-l-serine as simple model compound.