arXiv subjects

C. J. Fennie

Publications and source records attributed to C. J. Fennie.

16 recordsLinked to original sources

arXiv2019

Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca$_3$Ti$_2$O$_7$

Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90$^\circ$ ferroelectric) domain walls in the hybrid improper ferroelectric Ca$_3$Ti$_2$O$_7$. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.

cond-mat.mtrl-sci↗

arXiv2016

Strain Control of Fermiology and Many-Body Interactions in Two-Dimensional Ruthenates

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr$_2$RuO$_4$ and its isoelectronic counterpart Ba$_2$RuO$_4$ using oxide molecular beam epitaxy (MBE), \emph{in situ} angle-resolved photoemission spectroscopy (ARPES), and transport measurements. Near the topological transition of the $γ$ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.

cond-mat.supr-con↗

arXiv2015

Hierarchical spin-orbital polarisation of a giant Rashba system

The Rashba effect is one of the most striking manifestations of spin-orbit coupling in solids, and provides a cornerstone for the burgeoning field of semiconductor spintronics. It is typically assumed to manifest as a momentum-dependent splitting of a single initially spin-degenerate band into two branches with opposite spin polarisation. Here, combining polarisation-dependent and resonant angle-resolved photoemission measurements with density-functional theory calculations, we show that the two "spin-split" branches of the model giant Rashba system BiTeI additionally develop disparate orbital textures, each of which is coupled to a distinct spin configuration. This necessitates a re-interpretation of spin splitting in Rashba-like systems, and opens new possibilities for controlling spin polarisation through the orbital sector.

cond-mat.mtrl-sci↗

arXiv2015

Interplay of Spin-Orbit Interactions, Dimensionality, and Octahedral Rotations in Semimetallic SrIrO$_3$

We employ reactive molecular-beam epitaxy to synthesize the metastable perovskite SrIrO$_{3}$ and utilize {\it in situ} angle-resolved photoemission to reveal its electronic structure as an exotic narrow-band semimetal. We discover remarkably narrow bands which originate from a confluence of strong spin-orbit interactions, dimensionality, and both in- and out-of-plane IrO$_6$ octahedral rotations. The partial occupation of numerous bands with strongly mixed orbital characters signals the breakdown of the single-band Mott picture that characterizes its insulating two-dimensional counterpart, Sr$_{2}$IrO$_{4}$, illustrating the power of structure-property relations for manipulating the subtle balance between spin-orbit interactions and electron-electron interactions.

cond-mat.str-el↗

arXiv2014

Correlated vs. conventional insulating behavior in the Jeff=1/2 vs. 3/2 bands in the layered iridate Ba2IrO4

We employ molecular beam epitaxy to stabilize Ba2IrO4 thin films and utilize in situ angle-resolved photoemission spectroscopy to investigate the evolution of its electronic structure through the Neel temperature TN. Our measurements indicate that dispersions of the relativistic Jeff=1/2 and 3/2 bands exhibit an unusual dichotomy in their behavior through the Neel transition. Although the charge gap survives into the paramagnetic state, only the Jeff=1/2 state exhibits a strong temperature dependence and its gap softens with increasing temperature approaching TN, while the nearly fully occupied Jeff=3/2 state which remains nearby in energy exhibits negligible changes with temperature.

cond-mat.str-el↗

arXiv2013

Structural control of magnetic anisotropy in a strain driven multiferroic EuTiO3 thin film

Octahedral distortion plays a key role in engineering the physical properties of heterostructures composed of perovskite oxides. We observe a strong in-plane uniaxial magnetic anisotropy in a strain-enabled multiferroic EuTiO3 thin film epitaxially grown on a (110)o DyScO3 substrate. First principles calculations show that the magnetic anisotropy is closely correlated with the uniaxial TiO6 octahedral tilting and the ferroelectric polarization of the film, indicating potential strong magnetoelectric coupling in the strain-engineered multiferroic system.

cond-mat.mtrl-sci↗

arXiv2013

Topological Surface States and Superconductivity in [Tl$_4$](Tl$_{1-x}$Sn$_{x}$)Te$_3$ Perovskites

Materials with strong spin-orbit coupling have attracted attention following the prediction and subsequent discovery of strong two- and three-dimensional topological insulators in which a topological property of the bulk band structure of an insulator results in metallic surface states with Dirac-like dispersion. Here we report the discovery of Dirac-like surface states in the perovskite superconductor [Tl$_4$]TlTe$_3$ (Tl5Te3) and its non-superconducting tin-doped derivative, [Tl4](Tl$_{0.4}$Sn$_{0.6}$)Te$_3$, as observed by angle-resolved photoemission spectroscopy (ARPES). Density functional theory (DFT) calculations predict a single spin-orbit driven band parity inversion at the $Z$ point above the Fermi level of Tl5Te3, suggesting the surface states are protected by Z$_2$ topology. Calculations on [Tl$_4$]SnTe$_3$ show no parity inversions, implying that a topological transition from non-trivial to trivial must occur upon doping with tin, i.e., [Tl$_4$](Tl$_{1-x}$Sn$_{x}$)Te$_3$. Thus [Tl$_4$]{\it M}Te$_3$ perovskites are a possible new, non-trigonal class of Z$_2$ topological compounds. Additionally, as Tl5Te3 is a stoichiometric bulk superconductor, these perovskites are ideal materials in which to study the interplay between surface states and bulk superconductivity.

cond-mat.mtrl-sci↗

arXiv2012

Formation and consequences of heavy d-electron quasiparticles in Sr3Ru2O7

We report angle-resolved photoelectron spectroscopy measurements of the quantum critical metal Sr3Ru2O7 revealing itinerant Ru 4d-states confined over large parts of the Brillouin zone to an energy range of < 6 meV, nearly three orders of magnitude lower than the bare band width. We show that this energy scale agrees quantitatively with a characteristic thermodynamic energy scale associated with quantum criticality and illustrate how it arises from the hybridization of light and strongly renormalized, heavy quasiparticle bands. For the largest Fermi surface sheet we find a marked k-dependence of the renormalization and show that it correlates with the Ru 4d - O 2p hybridization.

cond-mat.str-el↗

arXiv2012

Reversible Control of Magnetic Interactions by Electric Field in a Single Phase Material

Intrinsic magnetoelectric coupling describes the interaction between magnetic and electric polarization through an inherent microscopic mechanism in a single phase material. This phenomenon has the potential to control the magnetic state of a material with an electric field, an enticing prospect for device engineering. We demonstrate 'giant' magnetoelectric cross-field control in a single phase rare earth titanate film. In bulk form, EuTiO3 is antiferromagnetic. However, both anti and ferromagnetic interactions coexist between different nearest neighbor europium ions. In thin epitaxial films, strain can be used to alter the relative strength of the magnetic exchange constants. Here, we not only show that moderate biaxial compression precipitates local magnetic competition, but also demonstrate that the application of an electric field at this strain state, switches the magnetic ground state. Using first principles density functional theory, we resolve the underlying microscopic mechanism resulting in the EuTiO3 G-type magnetic structure and illustrate how it is responsible for the 'giant' cross-field magnetoelectric effect.

cond-mat.mtrl-sci↗

arXiv2012

Magnetodielectric coupling and phonon properties of compressively strained EuTiO3 thin films deposited on LSAT

Compressively strained epitaxial (001) EuTiO3 thin films of tetragonal symmetry have been deposited on (001) (LaAlO3)_0.29-(SrAl_{1/2}Ta_{1/2}O3)_0.71 (LSAT) substrates by reactive molecular-beam epitaxy. Enhancement of the Neel temperature by 1 K with 0.9% compressive strain was revealed. The polar phonons ofthe films have been investigated as a function of temperature and magnetic field by means of infrared reflectance spectroscopy. All three infrared active phonons show strongly stiffened frequencies compared to bulk EuTiO3 in accordance with first principles calculations. The phonon frequencies exhibit gradual softening on cooling leading to an increase in static permittivity. A new polar phonon with frequency near the TO1 soft mode was detected below 150 K. The new mode coupled with the TO1 mode was assigned as the optical phonon from the Brillouin zone edge, which is activated in infrared spectra due to an antiferrodistortive phase transition and due to simultaneous presence of polar and/or magnetic nanoclusters. In the antiferromagnetic phase we have observed a remarkable softening of the lowest-frequency polar phonon under an applied magnetic field, which qualitatively agrees with first principles calculations. This demonstrates the strong spin-phonon coupling in EuTiO3, which is responsible for the pronounced dependence of its static permittivity on magnetic field in the antiferromagnetic phase.

cond-mat.mtrl-sci↗

arXiv2010

Atomic displacements in the "charge-ice" pyrochlore Bi2Ti2O7 studied by neutron total scattering

The oxide pyrochlore Bi$_2$Ti$_2$O$_6$O$^\prime$ is known to be associated with large displacements of Bi and O$^\prime$ atoms from their ideal crystallographic positions. Neutron total scattering, analyzed in both reciprocal and real space, is employed here to understand the nature of these displacements. Rietveld analysis and maximum entropy methods are used to produce an average picture of the structural non-ideality. Local structure is modeled via large-box reverse Monte Carlo simulations constrained simultaneously by the Bragg profile and real-space pair distribution function. Direct visualization and statistical analyses of these models show the precise nature of the static Bi and O$^\prime$ displacements. Correlations between neighboring Bi displacements are analyzed using coordinates from the large-box simulations. The framework of continuous symmetry measures has been applied to distributions of O$^\prime$Bi$_4$ tetrahedra to examine deviations from ideality. Bi displacements from ideal positions appear correlated over local length scales. The results are consistent with the idea that these nonmagnetic lone-pair containing pyrochlore compounds can be regarded as highly structurally frustrated systems.

cond-mat.mtrl-sci↗

arXiv2009

Coexistence of Weak Ferromagnetism and Ferroelectricity in the High Pressure LiNbO3-type Phase of FeTiO3

We report the magnetic and electrical characteristics of a polycrystalline specimen of FeTiO3 synthesized at high pressure that is isostructural with acentric LiNbO3 (LBO). Piezoresponse force microscopy, optical second harmonic generation, and magnetometry demonstrate that FeTiO3-II is ferroelectric at and below room temperature and weakly ferromagnetic below ~120 K. These results validate symmetry-based materials design criteria and first principles calculations of coexistence between ferroelectricity and weak ferromagnetism in a series of transition metal titanates crystallizing in the LBO structure. The high-pressure form of FeTiO3 stands out as a rare example of a ferroelectric exhibiting weak ferromagnetism generated by a Dzyaloshinskii-Moriya interaction.

cond-mat.mtrl-sci↗

arXiv2009

Strain-induced ferroelectricity in CaTiO$_3$ from first principles

First principles calculations are used to investigate the effects of epitaxial strain on the structure of the perovskite oxide CaTiO$_3$, with particular focus on the stabilization of a ferroelectric phase related to a polar instability hidden in the orthorhombic equilibrium bulk $Pbnm$ structure but found in previous first-principles studies of the ideal cubic perovskite high-symmetry reference structure. At 1.5% strain, we find an epitaxial orientation transition between the $ab$-$ePbnm$ phase, favored for compressive strains, and the $c$-$ePbnm$ phase. For larger tensile strains, a polar instability develops in the $c$-$ePbnm$ phase and an epitaxial-strain-induced ferroelectric phase is obtained with polarization along a $<$110$>$ direction with respect to the primitive perovskite lattice vectors of the square substrate.

cond-mat.mtrl-sci↗

arXiv2009

Broadband Dielectric Spectroscopy of Ruddlesden-Popper Sr$_{n+1}$Ti$_{n}$O$_{3n+1}$ ($n$ = 1, 2, 3) Thin Films

We explore the frequency-dependent relative permittivity of Ruddlesden-Popper series Sr(n+1)Ti(n)O(3n+1) (n =1,2,3) thin films as a function of temperature and dc electric field. Interdigitated capacitors and coplanar waveguides were used to extract the frequency response from 500 Hz to 40 GHz. At room temperature, the in-plane relative permittivities obtained for Sr(n+1)Ti(n)O(3n+1) (n =1,2,3) were 42+/-3, 54+/-3, and 77+/-2, respectively, and were independent of frequency. At low temperatures, permittivity increases and electric field tunability develops in Sr(4)Ti(3)O(10).

cond-mat.mtrl-sci↗

arXiv2008

Combinatorial discovery of a lead-free morphotropic phase boundary in a thin-film piezoelectric perovskite

We report on the discovery of a lead-free morphotropic phase boundary in Sm doped BiFeO3 with a simple perovskite structure using the combinatorial thin film strategy. The boundary is a rhombohedral to pseudo-orthorhombic structural transition which exhibits a ferroelectric (FE) to antiferroelectric (AFE) transition at approximately Bi0.86Sm0.14FeO3 with dielectric constant and out-of-plane piezoelectric coefficient comparable to those of epitaxial (001) oriented Pb(Zr,Ti)O3 (PZT) thin films at the MPB. The discovered composition may be a strong candidate of a Pb-free piezoelectric replacement of PZT.

cond-mat.mtrl-sci↗

arXiv2006

Broken parity and a chiral ground state in the frustrated magnet CdCr2O4

We present a model describing the lattice distortion and incommensurate magnetic order in the spinel CdCr2O4, a good realization of the Heisenberg "pyrochlore" antiferromagnet. The magnetic frustration is relieved through the spin-Peierls distortion of the lattice involving a phonon doublet with odd parity. The distortion stablizes a collinear magnetic order with the propagation wavevector q=2π(0,0,1). The lack of inversion symmetry makes the crystal structure chiral. The handedness is transferred to magnetic order by the relativistic spin-orbit coupling: the collinear state is twisted into a long spiral with the spins in the ac plane and q shifted to 2π(0,δ,1).

cond-mat.str-el↗