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W. Ratcliff II

Publications and source records attributed to W. Ratcliff II.

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Electric-field Induced Reversible Switching of the Magnetic Easy-axis in Co/BiFeO3/SrRuO3/SrTiO3 Heterostructures

Electric-field (E-field) control of magnetism enabled by multiferroics has the potential to revolutionize the landscape of present memory devices plagued with high energy dissipation. To date, this E-field controlled multiferroic scheme at room temperature has only been demonstrated using BiFeO3 (BFO) films grown on DyScO3 (refs 1 and 2), a unique and expensive substrate, which gives rise to a particular ferroelectric domain pattern in BFO. Here, we demonstrate reversible E-field-induced switching of the magnetic state of the Co layer in Co/BFO (001) thin film heterostructures fabricated on SrTiO3 substrates. The angular dependence of the coercivity and the remanent magnetization of the Co layer indicates that its easy axis reversibly switches by 45° back and forth between the (100) and the (110) crystallographic directions of SrTiO3 as a result of alternating application of positive and negative voltage pulses on BFO. The coercivity of the Co layer exhibits a hysteretic behavior between two states as a function of voltage. To explain the observation, we have also measured the exact canting angle of the antiferromagnetic G-type domain in BFO films for the first time using neutron diffraction. These results suggest a pathway to integrating BFO-based devices on Si wafers for implementing low power consumption and non-volatile magnetoelectronic devices.

cond-mat.mtrl-sci

Temperature-dependent properties of the magnetic order in single-crystal BiFeO3

We report neutron diffraction and magnetization studies of the magnetic order in multiferroic BiFeO3. In ferroelectric monodomain single crystals, there are three magnetic cycloidal domains with propagation vectors equivalent by crystallographic symmetry. The cycloid period slowly grows with increasing temperature. The magnetic domain populations do not change with temperature except in the close vicinity of the N¶eel temperature, at which, in addition, a small jump in magneti- zation is observed. No evidence for the spin-reorientation transitions proposed in previous Raman and dielectric studies is found. The magnetic cycloid is slightly anharmonic for T=5 K. The an- harmonicity is much smaller than previously reported in NMR studies. At room temperature, a circular cycloid is observed, within errors. We argue that the observed anharmonicity provides important clues for understanding electromagnons in BiFeO3.

cond-mat.str-el

Interplay between Fe and Nd magnetism in NdFeAsO single crystals

The structural and magnetic phase transitions have been studied on NdFeAsO single crystals by neutron and x-ray diffraction complemented by resistivity and specific heat measurements. Two low-temperature phase transitions have been observed in addition to the tetragonal-to-orthorhombic transition at T_S = 142 K and the onset of antiferromagnetic (AFM) Fe order below T_N = 137 K. The Fe moments order AFM in the well-known stripe-like structure in the (ab) plane, but change from AFM to ferromagnetic (FM) arrangement along the c direction below T* = 15 K accompanied by the onset of Nd AFM order below T_Nd = 6 K with this same AFM configuration. The iron magnetic order-order transition in NdFeAsO accentuates the Nd-Fe interaction and the delicate balance of c-axis exchange couplings that results in AFM in LaFeAsO and FM in CeFeAsO and PrFeAsO.

cond-mat.supr-con

Magnetic form factor of SrFe$_2$As$_2$

Neutron diffraction measurements have been carried out to investigate the magnetic form factor of the parent SrFe2As2 system of the iron-based superconductors. The general feature is that the form factor is approximately isotropic in wave vector, indicating that multiple d-orbitals of the iron atoms are occupied as expected based on band theory. Inversion of the diffraction data suggests that there is some elongation of the spin density toward the As atoms. We have also extended the diffraction measurements to investigate a possible jump in the c-axis lattice parameter at the structural phase transition, but find no detectable change within the experimental uncertainties.

cond-mat.supr-con

3:1 magnetization plateau and suppression of ferroelectric polarization in an Ising chain multiferroic

Ferroelectric Ising chain magnet Ca$_3$Co$_{2-x}$Mn$_x$O$_6$ ($x\simeq$0.96) was studied in magnetic fields up to 33 T. Magnetization and neutron scattering measurements reveal successive metamagnetic transitions from the zero-field $\uparrow \uparrow \downarrow \downarrow$ spin configuration to the $\uparrow \uparrow \uparrow \downarrow$ state with a broad magnetization plateau, and then to the $\uparrow \uparrow \uparrow \uparrow$ state. The absence of hysteresis in these plateaus reveals an intriguing coupling between the intra-chain state and the three-dimensional geometrically frustrated magnetic system. Inversion symmetry, broken in the $\uparrow \uparrow \downarrow \downarrow$ state, is restored in the $\uparrow \uparrow \uparrow \downarrow$ state, leading to the complete suppression of the electric polarization driven by symmetric superexchange.

cond-mat.str-el

Singe ferroelectric and chiral magnetic domain of single-crystalline BiFeO$_3$ in an electric field

We report polarized neutron scattering and piezoresponse force microscopy studies of millimeter-sized single crystals of multiferroic BiFeO$_3$. The crystals, grown below the Curie temperature, consist of a single ferroelectric domain. Two unique electric polarization directions, as well as the populations of equivalent spiral magnetic domains, can be switched reversibly by an electric field. A ferroelectric monodomain with a single-$q$ single-helicity spin spiral can be obtained. This level of control, so far unachievable in thin films, makes single-crystal BiFeO$_3$ a promising object for multiferroics research.

cond-mat.mtrl-sci

Low energy spin waves and magnetic interactions in SrFe$_2$As$_2$

We report inelastic neutron scattering studies of magnetic excitations in antiferromagnetically ordered SrFe$_{2}$As$_{2}$ ($T_{N}=220$ K), the parent compound of the FeAs-based superconductors. At low temperatures (T=7 K), the spectrum of magnetic excitations $S(Q,\hbar ω)$ consists of a Bragg peak at the elastic position ($\hbar ω=0$ meV), a spin gap ($ Δ\leq 6.5$ meV), and sharp spin wave excitations at higher energies. Based on the observed dispersion relation, we estimate the effective magnetic exchange coupling using a Heisenberg model. On warming across $T_{N} $, the low temperature spin gap rapidly closes, with weak critical scattering and spin-spin correlations in the paramagnetic state. The antiferromagnetic order in SrFe$_{2}$As$_{2}$ is therefore consistent with a first order phase transition, similar to the structural lattice distortion.

cond-mat.supr-con

Spin and Lattice Structure of Single Crystal SrFe2As2

We use neutron scattering to study the spin and lattice structure on single crystals of SrFe2As2, the parent compound of the FeAs based superconductor (Sr,K)Fe2As2. We find that SrFe2As2 exhibits an abrupt structural phase transitions at 220K, where the structure changes from tetragonal with lattice parameters c > a = b to orthorhombic with c > a > b. At almost the same temperature, Fe spins in SrFe2As2 develop a collinear antiferromagnetic structure along the orthorhombic a-axis with spin direction parallel to this a-axis. These results are consistent with earlier work on the RFeAsO (R = rare earth elements) families of materials and on BaFe2As2, and therefore suggest that static antiferromagnetic order is ubiquitous for the parent compound of these FeAs-based high-transition temperature superconductors.

cond-mat.str-el

Magnetic Order versus superconductivity in the Iron-based layered La(O1-xFx)FeAs systems

In high-transition temperature (high-Tc) copper oxides, it is generally believed that antiferromagnetism plays a fundamental role in the superconducting mechanism because superconductivity occurs when mobile electrons or holes are doped into the antiferromagnetic parent compounds. The recent discovery of superconductivity in the rare-earth (R) iron-based oxide systems [RO1-xFxFeAs] has generated enormous interest because these materials are the first noncopper oxide superconductors with Tc exceeding 50 K. The parent (nonsuperconducting) LaOFeAs material is metallic but shows anomalies near 150 K in both resistivity and dc magnetic susceptibility. While optical conductivity and theoretical calculations suggest that LaOFeAs exhibits a spin-density-wave (SDW) instability that is suppressed with doping electrons to form superconductivity, there has been no direct evidence of the SDW order. Here we use neutron scattering to demonstrate that LaOFeAs undergoes an abrupt structural distortion below ~150 K, changing the symmetry from tetragonal (space group P4/nmm) to monoclinic (space group P112/n) at low temperatures, and then followed with the development of long range SDW-type antiferromagnetic order at ~134 K with a small moment but simple magnetic structure. Doping the system with flourine suppresses both the magnetic order and structural distortion in favor of superconductivity. Therefore, much like high-Tc copper oxides, the superconducting regime in these Fe-based materials occurs in close proximity to a long-range ordered antiferromagnetic ground state. Since the discovery of long

cond-mat.supr-con

Neel to Spin-Glass-like Phase Transition versus Dilution in Geometrically Frustrated ZnCr_{2-2x}Ga_{2x}O_4

ZnCr2O4 undergoes a first order spin-Peierls-like phase transition at 12.5 K from a cubic spin liquid phase to a tetragonal Neel state. Using powder diffraction and single crystal polarized neutron scattering, we determined the complex spin structure of the Neel phase. This phase consisted of several magnetic domains with different characteristic wave vectors. This indicates that the tetragonal phase of ZnCr2O4 is very close to a critical point surrounded by many different Neel states. We have also studied, using elastic and inelastic neutron scattering techniques, the effect of nonmagnetic dilution on magnetic correlations in ZnCr_{2-2x}Ga_{2x}O_4 (x=0.05 and 0.3). For x=0.05, the magnetic correlations do not change qualitatively from those in the pure material, except that the phase transition becomes second order. For x= 0.3, the spin-spin correlations become short range. Interestingly, the spatial correlations of the frozen spins in the x=0.3 material are the same as those of the fluctuating moments in the pure and the weakly diluted materials.

cond-mat.str-el

Probing spin correlations with phonons in the strongly frustrated magnet ZnCr2O4

The spin-lattice coupling plays an important role in strongly frustrated magnets. In ZnCr$_2$O$_4$, an excellent realization of the Heisenberg antiferromagnet on the ``pyrochlore'' network, a lattice distortion relieves the geometrical frustration through a spin-Peierls-like phase transition at $T_c = 12.5$ K. Conversely, spin correlations strongly influence the elastic properties of a frustrated magnet. By using infrared spectroscopy and published data on magnetic specific heat, we demonstrate that the frequency of an optical phonon triplet in ZnCr$_2$O$_4$ tracks the nearest-neighbor spin correlations above $T_c$. The splitting of the phonon triplet below $T_c$ provides a way to measure of the spin-Peierls order parameter.

cond-mat.str-el

Spin singlet formation in MgTi$_2$O$_4$: evidence of a helical dimerization pattern

The transition metal spinel MgTi$_2$O$_4$ undergoes a metal-insulator transition on cooling below $T_{M-I} = 260$ K. A sharp reduction of the magnetic susceptibility below $T_{M-I}$ suggests the onset of a magnetic singlet state. Using high-resolution synchrotron and neutron powder diffraction, we have solved the low-temperature crystal structure of MgTi$_2$O$_4$, which is found to contain dimers with short Ti-Ti distances (the locations of the spin singlets) alternating with long bonds to form helices. Band structure calculations based on hybrid exchange density functional theory show that, at low temperatures, MgTi$_2$O$_4$ is an orbitally ordered band insulator.

cond-mat

First-order nature of the ferromagnetic phase transition in (La-Ca)MnO_3 near optimal doping

Neutron scattering has been used to study the nature of the ferromagnetic transition in single crystals of La_0.7Ca_0.3MnO_3 and La_0.8Ca_0.2MnO_3, and polycrystalline samples of La_0.67Ca_0.33MnO_3 and La_5/8Ca_3/8MnO_3 where the naturally occurring O-16 can be replaced with the O-18 isotope. Small angle neutron scattering on the x=0.3 single crystal reveals a discontinuous change in the scattering at the Curie temperature for wave vectors below ~0.065 A^-1. Strong relaxation effects are observed for this domain scattering, for the magnetic order parameter, and for the quasielastic scattering, demonstrating that the transition is not continuous in nature. There is a large oxygen isotope effect observed for the T_C in the polycrystalline samples. For the optimally doped x=3/8 sample we observed T_C(O-16)=266.5 K and T_C(O-18)=261.5 K at 90% O-18 substitution. The temperature dependence of the spin-wave stiffness is found to be identical for the two samples despite changes in T_C. Hence, T_C is not solely determined by the magnetic subsystem, but instead the ferromagnetic phase is truncated by the formation of polarons which cause an abrupt transition to the paramagnetic, insulating state. Application of uniaxial stress in the x=0.3 single crystal sharply enhances the polaron scattering at room temperature. Measurements of the phonon density-of-states show only modest differences above and below T_C and between the two different isotopic samples.

cond-mat.str-el

Magnetic properties of the frustrated AFM spinel ZnCr_2O_4 and the spin-glass Zn_{1-x}Cd_xCr_2O_4 (x=0.05,0.10)

The $T$-dependence (2- 400 K) of the electron paramagnetic resonance (EPR), magnetic susceptibility, $χ(T)$, and specific heat, $C_{v}(T)$, of the $normal$ antiferromagnetic (AFM) spinel ZnCr$_{2}$O$_{4}$ and the spin-glass (SG) Zn$_{1-x}$Cd$_{x}$Cr$_{2}$O$_{4}$ ($x=0.05,0.10$) is reported. These systems behave as a strongly frustrated AFM and SG with $% T_{N}$ $ \approx T_{G}\approx 12$ K and -400 K $\gtrsim Θ_{CW}\gtrsim -500$ K. At high-$T$ the EPR intensity follows the $χ(T)$ and the $g$-value is $T$-independent. The linewidth broadens as the temperature is lowered, suggesting the existence of short range AFM correlations in the paramagnetic phase. For ZnCr$_{2}$O$_{4}$ the EPR intensity and $χ(T)$ decreases below 90 K and 50 K, respectively. These results are discussed in terms of nearest-neighbor Cr$^{3+}$ (S $=3/2$%) spin-coupled pairs with an exchange coupling of $| J/k| \approx $ 50 K. The appearance of small resonance modes for $T\lesssim 17$ K, the observation of a sharp drop in $χ(T)$ and a strong peak in $C_{v}(T)$ at $T_{N}=12$ K confirms, as previously reported, the existence of long range AFM correlations in the low-$T$ phase. A comparison with recent neutron diffraction experiments that found a near dispersionless excitation at 4.5 meV for $T\lesssim T_{N}$ and a continuous gapless spectrum for $T\gtrsim T_{N}$, is also given.

cond-mat.str-el

Local spin resonance and spin-Peierls-like phase transition in a geometrically frustrated antiferromagnet

Using inelastic magnetic neutron scattering we have discovered a localized spin resonance at 4.5 meV in the ordered phase of the geometrically frustrated cubic antiferromagnet $\rm ZnCr_2O_4$. The resonance develops abruptly from quantum critical fluctuations upon cooling through a first order transition to a co-planar antiferromagnet at $T_c=12.5(5)$ K. We argue that this transition is a three dimensional analogue of the spin-Peierls transition.

cond-mat.str-el