arXiv subjects

G. Lawes

Publications and source records attributed to G. Lawes.

At least 19 recordsLinked to original sources

arXiv2014

Magnetostructural and magnetocaloric properties of bulk LaCrO3 system

We studied the magnetic properties of bulk LaCrO3; a GdFeO3-type distorted perovskite, with a predominant antiferromagnetic phase transition at ~ 290 K. The bulk LaCrO3 exhibits intrinsic weak ferromagnetism at room temperature, which may arise due to the tilting of CrO6 octahedra, resulting in a non-zero net magnetic moment, as confirmed from the magnetization measurements. A broad magnetically-induced entropy change (-ΔS) is observed with the maximum at 290 K, close to room temperature in LaCrO3 system.

cond-mat.str-el↗

arXiv2010

Magnetic structure and magnetoelectric coupling in bulk and thin film FeVO$_4$

We have investigated the magnetoelectric and magnetodielectric response in FeVO$_4$, which exhibits a change in magnetic structure coincident with ferroelectric ordering at $T_{N2}$$\approx$15 K. Using symmetry considerations, we construct a model for the possible magnetoelectric coupling in this system, and present a discussion of the allowed spin structures in FeVO$_4$. Based on this model, in which the spontaneous polarization is caused by a trilinear spin-phonon interaction, we experimentally explore the magnetoelectric coupling in FeVO$_4$ thin films through measurements of the electric field induced shift of the multiferroic phase transition temperature, which exhibits an increase of 0.25 K in an applied field of 4 MV/m. The strong spin-charge coupling in \fvo\, is also reflected in the significant magnetodielectric shift, which is present in the paramagnetic phase due to a quartic spin-phonon interaction and shows a marked enhancement with the onset of magnetic order which we attribute to the trilinear spin-phonon interaction. We observe a clear magnetic field induced dielectric anomaly at lower temperatures, distinct from the sharp peak associated with the multiferroic transition, which we tentatively assign to a spin reorientation cross-over. We also present a magnetoelectric phase diagram for FeVO$_4$.

cond-mat.mtrl-sci↗

arXiv2009

Suppression of multiferroic order in hexagonal YMn1-xInxO3 ceramics

We have investigated the effects of substituting In for Mn on the antiferromagnetic phase transition in YMnO3 using magnetic, dielectric, and specific heat measurements. We prepared a set of isostructural phase pure hexagonal YMn$_{1-x}$In$_{x}$O$_{3}$ samples having x=0 to x=0.9, which exhibit a systematic decrease of the antiferromagnetic ordering temperature with increasing In content. The multiferroic phase, which develops below TN, appears to be completely suppressed for x$\geq$0.5 in the temperature range investigated, which can be attributed solely to the dilution of magnetic interactions as the crystal structure remains hexagonal. Similar to previous reports, we find an enhancement of the magnetocapacitive coupling on dilution with non-magnetic ions.

cond-mat.mtrl-sci↗

arXiv2009

Coupled magnetic and ferroelectric domains in multiferroic Ni3V2O8

Electric control of multiferroic domains is demonstrated through polarized magnetic neutron diffraction. Cooling to the cycloidal multiferroic phase of Ni3V2O8 in an electric field (E) causes the incommensurate Bragg reflections to become neutron spin polarizing, the sense of neutron polarization reversing with E. Quantitative analysis indicates the E-treated sample has handedness that can be reversed by E. We further show close association between cycloidal and ferroelectric domains through E-driven spin and electric polarization hysteresis. We suggest that definite cycloidal handedness is achieved through magneto-elastically induced Dzyaloshinskii-Moriya interactions.

cond-mat.str-el↗

arXiv2009

Magnetically tunable dielectric materials

The coupling between localized spins and phonons can lead to shifts in the dielectric constant of insulating materials at magnetic ordering transitions. Studies on isostructural SeCuO3 (ferromagnetic) and TeCuO3 (antiferromagnetic) illustrate how the q-dependent spin-spin correlation function couples to phonon frequencies leading to a shift in the dielectric constant. A model is discussed for this spin-phonon coupling. The magnetodielectric coupling in multiferroic materials can be very large at a ferroelectric transition temperature. This coupling is investigated in the recently identified multiferroic Ni3V2O8.

cond-mat.mtrl-sci↗

arXiv2008

Ferromagnetism and spin polarized charge carriers in In$_{2}$O$_{3}$ thin films

We present evidence for spin polarized charge carriers in In$_2$O$_3$ films. Both In$_2$O$_3$ and Cr doped In$_2$O$_3$ films exhibit room temperature ferromagnetism after vacuum annealing, with a saturation moment of approximately 0.5 emu/cm$^3$. We used Point Contact Andreev Reflection measurements to directly determine the spin polarization, which was found to be approximately 50$\pm$5% for both compositions. These results are consistent with suggestions that the ferromagnetism observed in certain oxide semiconductors may be carrier mediated.

cond-mat.mtrl-sci↗

arXiv2007

Electric field control of magnetic phase transitions in Ni3V2O8

We report on the electric field control of magnetic phase transition temperatures in multiferroic Ni3V2O8 thin films. Using magnetization measurements, we find that the phase transition temperature to the canted antiferromagnetic state is suppressed by 0.2 K in an electric field of 30 MV/m, as compared to the unbiased sample. Dielectric measurements show that the transition temperature into the magnetic state associated with ferroelectric order increases by 0.2 K when the sample is biased at 25 MV/m. This electric field control of the magnetic transitions can be qualitatively understood using a mean field model incorporating a tri-linear coupling between the magnetic order parameters and spontaneous polarization.

cond-mat.mtrl-sci↗

arXiv2007

Ordered spin-ice state in the geometrically frustrated metallic-ferromagnet Sm2Mo2O7

The recent discovery of Spin-ice is a spectacular example of non-coplanar spin arrangements that can arise in the pyrochlore A2B2O7 structure. We present magnetic and thermodynamic studies on the metallic-ferromagnet pyrochlore Sm2Mo2O7. Our studies, carried out on oriented crystals, suggest that the Sm spins have an ordered spin-ice ground state below about T* = 15 K. The temperature- and field-evolution of the ordered spin-ice state are governed by an antiferromagnetic coupling between the Sm and Mo spins. We propose that as a consequence of a robust feature of this coupling, the tetrahedra aligned with the external field adopt a "1-in, 3-out" spin structure as opposed to "3-in, 1-out" in dipolar spin ices, as the field exceeds a critical value.

cond-mat.str-el↗

arXiv2007

Magnetodielectric coupling in Mn3O4

We have investigated the dielectric anomalies associated with spin ordering transitions in the tetragonal spinel Mn$_3$O$_4$, using thermodynamic, magnetic, and dielectric measurements. We find that two of the three magnetic ordering transitions in Mn$_3$O$_4$ lead to decreases in the temperature dependent dielectric constant at zero applied field. Applying a magnetic field to the polycrystalline sample leaves these two dielectric anomalies practically unchanged, but leads to an increase in the dielectric constant at the intermediate spin-ordering transition. We discuss possible origins for this magnetodielectric behavior in terms of spin-phonon coupling. Band structure calculations suggest that in its ferrimagnetic state, Mn$_3$O$_4$ corresponds to a semiconductor with no orbital degeneracy due to strong Jahn-Teller distortion.

cond-mat.mtrl-sci↗

arXiv2007

Direct transition from a disordered to a multiferroic phase on a triangular lattice

Competing interactions and geometric frustration provide favourable conditions for exotic states of matter. Such competition often causes multiple phase transitions as a function of temperature and can lead to magnetic structures that break inversion symmetry, thereby inducing ferroelectricity [1-4]. Although this phenomenon is understood phenomenologically [3-4], it is of great interest to have a conceptually simpler system in which ferroelectricity appears coincident with a single magnetic phase transition. Here we report the first such direct transition from a paramagnetic and paraelectric phase to an incommensurate multiferroic in the triangular lattice antiferromagnet RbFe(MoO4)2 (RFMO). A magnetic field extinguishes the electric polarization when the symmetry of the magnetic order changes and ferroelectricity is only observed when the magnetic structure has chirality and breaks inversion symmetry. Multiferroic behaviour in RFMO provides a theoretically tractable example of ferroelectricity from competing spin interactions. A Landau expansion of symmetry-allowed terms in the free energy demonstrates that the chiral magnetic order of the triangular lattice antiferromagnet gives rise to a pseudoelectric field, whose temperature dependence agrees with that observed experimentally.

cond-mat.mtrl-sci↗

arXiv2006

Optical Properties and Magnetic Field-Induced Phase Transitions in the Ferroelectric State of Ni$_3$V$_2$O$_8$

We use a combination of optical spectra, first principles calculations, and energy dependent magneto-optical measurements to elucidate the electronic structure and to study the phase diagram of Ni$_3$V$_2$O$_8$. We find a remarkable interplay of magnetic field and optical properties that reveals additional high magnetic field phases and an unexpected electronic structure which we associate with the strong magneto-dielectric couplings in this material over a wide energy range. Specifically, we observed several prominent magneto-dielectric effects that derive from changes in crystal field environment around Ni spine and cross-tie centers. This effect is consistent with a field-induced modification of local structure. Symmetry-breaking effects are also evident with temperature. We find Ni$_3$V$_2$O$_8$ to be an intermediate gap, local moment band insulator. This electronic structure is particularly favorable for magneto-dielectric couplings, because the material is not subject to the spin charge separation characteristic of strongly correlated large gap Mott insulators, while at the same time remaining a magnetic insulator independent of the particular spin order and temperature.

cond-mat.str-el↗

arXiv2006

Observation of 300 K High Energy MagnetoDielectric Response in the Bilayer Manganite (La$_{0.4}$Pr$_{0.6}$)$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$

We observed a large HEMD effect in the bilayer manganite (La$_{0.4}$Pr$_{0.6}$)$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$, a direct consequence of field driven spin-glass insulator to ferromagnetic metal transition. The remnants of the transition can be used to achieve dielectric contrast at room temperature. This discovery suggests that electronic mechanisms such as the metal-insulator transition, charge ordering, and orbital ordering can be exploited to give substantial dielectric contrast in other materials.

cond-mat.mtrl-sci↗

arXiv2006

Complex magnetic order in the kagome staircase compound Co3V2O8

Co3V2O8 (CVO) has a geometrically frustrated magnetic lattice, a Kagome staircase. The crystal structure consists of two inequivalent Co sites, one-dimensional chains of Co(2) spine sites, linked by Co(1) cross-tie sites. Neutron powder diffraction has been used to solve the basic magnetic and crystal structures of this system, while polarized and unpolarized single crystal diffraction measurements have been used to reveal a variety of incommensurate phases, interspersed with lock-in transitions to commensurate phases. CVO initially orders magnetically at 11.3 K into an incommensurate, transversely polarized, spin density wave state, with wave vector k=(0,delta,0) with delta=0.55 and the spin direction along the a axis. Delta is found to decrease monotonically with decreasing temperature, and then it locks into a commensurate antiferromagnetic structure with delta=0.5 for 6.9<T<8.6 K. Below 6.9 K the magnetic structure becomes incommensurate again. Delta continues to decrease with decreasing temperature, and locks-in again at delta=1/3 over a narrow temperature range (6.2<T<6.5 K). The system then undergoes a strongly first order transition to the ferromagnetic ground state (delta=0) at Tc=6.2 K. A dielectric anomaly is observed around the ferromagnetic transition temperature of 6.2 K, demonstrating a significant spin-charge coupling present in CVO. A theory based on group theory analysis and a minimal Ising model with competing exchange interactions can explain the basic features of the magnetic ordering.

cond-mat.str-el↗

arXiv2006

Dielectric anomalies and spiral magnetic order in CoCr2O4

We have investigated the structural, magnetic, thermodynamic, and dielectric properties of polycrystalline CoCr$_2$O$_4$, an insulating spinel exhibiting both ferrimagnetic and spiral magnetic structures. Below $T_c$ = 94 K the sample develops long-range ferrimagnetic order, and we attribute a sharp phase transition at $T_N$ $\approx$ 25 K with the onset of long-range spiral magnetic order. Neutron measurements confirm that while the structure remains cubic at 80 K and at 11 K; there is complex magnetic ordering by 11 K. Density functional theory supports the view of a ferrimagnetic semiconductor with magnetic interactions consistent with non-collinear ordering. Capacitance measurements on CoCr$_2$O$_4$, show a sharp decrease in the dielectric constant at $T_N$, but also an anomaly showing thermal hysteresis falling between approximately $T$ = 50 K and $T$ = 57 K. We tentatively attribute the appearance of this higher temperature dielectric anomaly to the development of \textit{short-range} spiral magnetic order, and discuss these results in the context of utilizing dielectric spectroscopy to investigate non-collinear short-range magnetic structures.

cond-mat.mtrl-sci↗

arXiv2006

Positive and negative magnetocapacitance in magnetic nanoparticle systems

The dielectric properties of MnFe$_2$O$_4$ and $γ$-Fe$_2$O$_3$ magnetic nanoparticles embedded in insulating matrices were investigated. The samples showed frequency dependent dielectric anomalies coincident with the magnetic blocking temperature and significant magnetocapacitance above this blocking temperature, as large as 0.4% at H = 10kOe. For both samples the magnetic field induced change in dielectric constant was proportional to the square of the sample magnetization. These measurements suggest that the dielectric properties of magnetic nanoparticles are closely related to the disposition of magnetic moments in the system. As neither bulk gamma-Fe2O3 nor MnFe2O3 are magnetoelectric materials, this magnetodielectric coupling is believed to arise from extrinsic effects which are discussed in light of recent work relating magnetoresistive and magnetocapacitive behavior.

cond-mat.mtrl-sci↗

arXiv2005

Field dependence of magnetic ordering in Kagome-staircase compound Ni3V2O8

We present powder and single-crystal neutron diffraction and bulk measurements of the Kagome-staircase compound Ni3V2O8 (NVO) in fields up to 8.5T applied along the c-direction. (The Kagome plane is the a-c plane.) This system contains two types of Ni ions, which we call "spine" and "cross-tie". Our neutron measurements can be described with the paramagnetic space group Cmca for T < 15K and each observed magnetically ordered phase is characterized by the appropriate irreducible representation(s). Our zero-field measurements show that at T_PH=9.1K NVO undergoes a transition to an incommensurate order which is dominated by a longitudinally-modulated structure with the spine spins mainly parallel to the a-axis. Upon further cooling, a transition is induced at T_HL=6.3K to an elliptically polarized incommensurate structure with both spine and cross-tie moments in the a-b plane. At T_LC=4K the system undergoes a first-order phase transition, below which the magnetic structure is a commensurate antiferromagnet with the staggered magnetization primarily along the a-axis and a weak ferromagnetic moment along the c-axis. A specific heat peak at T_CC'=2.3K indicates an additional transition, which we were however not able to relate to a change of the magnetic structure. Neutron, specific heat, and magnetization measurements produce a comprehensive temperature-field phase diagram. The symmetries of the two incommensurate magnetic phases are consistent with the observation that only one phase has a spontaneous ferroelectric polarization. All the observed magnetic structures are explained theoretically using a simplified model Hamiltonian, involving competing nearest- and next-nearest-neighbor exchange interactions, spin anisotropy, Dzyaloshinskii-Moriya and pseudo-dipolar interactions.

cond-mat.str-el↗

arXiv2005

Ferroelectricity in Incommensurate Magnets

We review the phenomenology of coupled magnetic and electric order parameters for systems in which ferroelectric and incommensurate magnetic order occur simultaneously. We discuss the role that such materials might play in fabricating novel magnetoelectric devices. Then we briefly review the mean-field description of ferroelectricity and modulated magnetic ordering as a preliminary to analyzing the symmetry of the interaction between the spontaneous polarization and the order parameters describing long-range modulated magnetic ordering. As illustration we show how this formulation provides a phenomenological explanation for the observed phase transitions in Ni$_3$V$_2$O$_8$ and TbMnO$_3$ in which ferroelectric and magnetic order parameters simultaneously become nonzero at a single phase transition. In addition, this approach explains the fact that the spontaneous polarization only appears along a specific crystallographic direction. We analyze the symmetry of the strain dependence of the exchange tensor and show that it is consistent with the macroscopic symmetry analysis. We conclude with a brief discussion of how our approach might be relevant in understanding other systems with coupled magnetic and ferroelectric order, and more importantly, how these principles relate to the search for materials with larger magnetoelectric couplings at room temperature.

cond-mat.mtrl-sci↗

arXiv2005

Magnetically driven ferroelectric order in Ni$_3$V$_2$O$_8$

We show that for Ni$_3$V$_2$O$_8$ long-range ferroelectric and incommensurate magnetic order appear simultaneously in a single phase transition. The temperature and magnetic field dependence of the spontaneous polarization show a strong coupling between magnetic and ferroelectric orders. We determine the magnetic symmetry of this system by constraining the data to be consistent with Landau theory for continuous phase transitions. This phenomenological theory explains our observation the spontaneous polarization is restricted to lie along the crystal b axis and predicts that the magnitude should be proportional to a magnetic order parameter.

cond-mat.mtrl-sci↗