arXiv subjects

N. A. Spaldin

Publications and source records attributed to N. A. Spaldin.

At least 19 recordsLinked to original sources

arXiv2024

Non-relativistic ferromagnetotriakontadipolar order and spin splitting in hematite

We show that hematite, $α$-Fe$_2$O$_3$, below its Morin transition, has a ferroic ordering of rank-5 magnetic triakontadipoles on the Fe ions. In the absence of spin-orbit coupling, these are the lowest-order ferroically aligned magnetic multipoles, and they give rise to the $g$-wave non-relativistic spin splitting in hematite. We find that the ferroically ordered magnetic triakontadipoles result from the simultaneous antiferroic ordering of the charge hexadecapoles and the magnetic dipoles, providing a route to manipulating the magnitude and the sign of the magnetic triakontadipoles as well as the spin splitting. Furthermore, we find that both the ferroic ordering of the magnetic triakontadipoles and many of the spin-split features persist in the weak ferromagnetic phase above the Morin transition temperature.

cond-mat.str-el↗

arXiv2024

Depth-resolved profile of the interfacial ferromagnetism in $CaMnO_{3}/CaRuO_{3}$ superlattices

Emergent magnetic phenomena at interfaces represent a frontier in materials science, pivotal for advancing technologies in spintronics and magnetic storage. In this letter, we utilize a suite of advanced X-ray spectroscopic and scattering techniques to investigate emergent interfacial ferromagnetism in oxide superlattices comprised of antiferromagnetic CaMnO3 and paramagnetic CaRuO3. Our findings challenge prior theoretical models by demonstrating that the ferromagnetism extends beyond the interfacial layer into multiple unit cells of CaMnO3 and exhibits an asymmetric profile. Complementary density functional calculations reveal that the interfacial ferromagnetism is driven by the double exchange mechanism, facilitated by charge transfer from Ru to Mn ions. Additionally, defect chemistry, particularly the presence of oxygen vacancies, likely plays a crucial role in modifying the magnetic moments at the interface, leading to the observed asymmetry between the top and bottom CaMnO3 interfacial magnetic layers. Our findings underscore the potential of manipulating interfacial ferromagnetism through point defect engineering.

cond-mat.mtrl-sci↗

arXiv2021

Local Electronic Structure and Dynamics of Muon-Polaron Complexes in Fe$_2$O$_3$

We perform detailed muon spin rotation ($μ$SR) measurements in the classic antiferromagnet Fe$_2$O$_3$ and explain the spectra by considering dynamic population and dissociation of charge-neutral muon-polaron complexes. We show that charge-neutral muon states in Fe$_2$O$_3$, despite lacking the signatures typical of charge-neutral muonium centers in nonmagnetic materials, have a significant impact on the measured $μ$SR frequencies and relaxation rates. Our identification of such polaronic muon centers in Fe$_2$O$_3$ suggests that isolated hydrogen (H) impurities form analogous complexes, and that H interstitials may be a source of charge carrier density in Fe$_2$O$_3$.

cond-mat.mtrl-sci↗

arXiv2020

Manifestion of structural Higgs and Goldstone modes in the hexagonal manganites

Structural phase transitions described by Mexican hat potentials should in principle exhibit aspects of Higgs and Goldstone physics. Here, we investigate the relationship between the phonons that soften at such structural phase transitions and the Higgs- and Goldstone-boson analogues associated with the crystallographic Mexican hat potential. We show that, with the exception of systems containing only one atom type, the usual Higgs and Goldstone modes are represented by a combination of several phonon modes, with the lowest energy phonons of the relevant symmetry having substantial contribution. Taking the hexagonal manganites as a model system, we identify these modes using Landau theory, and predict the temperature dependence of their frequencies using parameters obtained from density functional theory. Separately, we calculate the additional temperature dependence of all phonon mode frequencies arising from thermal expansion within the quasi-harmonic approximation. We predict that Higgs-mode softening will dominate the low-frequency vibrational spectrum of InMnO$_3$ between zero kelvin and room-temperature, whereas the behavior of ErMnO$_3$ will be dominated by lattice expansion effects. We present temperature-dependent Raman scattering data that support our predictions, in particular confirming the existence of the Higgs mode in InMnO$_3$.

cond-mat.mtrl-sci↗

arXiv2019

Observation of a charge-neutral muon-polaron complex in antiferromagnetic Cr$_2$O$_3$

We report a comprehensive muon spin rotation ($μ$SR) study of the prototypical magnetoelectric antiferromagnet Cr$_2$O$_3$. We find the positively charged muon ($μ^+$) occupies several distinct interstitial sites, and displays a rich dynamic behavior involving local hopping, thermally activated site transitions and the formation of a charge-neutral complex composed of a muon and an electron polaron. The discovery of such a complex has implications for the interpretation of $μ$SR spectra in a wide range of magnetic oxides, and opens a route to study the dopant characteristics of interstitial hydrogen impurities in such materials. We address implications arising from implanting a $μ^+$ into a linear magnetoelectric, and discuss the challenges of observing a local magnetoelectric effect generated by the charge of the muon.

cond-mat.mtrl-sci↗

arXiv2019

Dynamic multiferroicity of a ferroelectric quantum critical point

Quantum matter hosts a large variety of phases, some coexisting, some competing; when two or more orders occur together, they are often entangled and cannot be separated. Dynamical multiferroicity, where fluctuations of electric dipoles lead to magnetisation, is an example where the two orders are impossible to disentangle. Here we demonstrate elevated magnetic response of a ferroelectric near the ferroelectric quantum critical point (FE QCP) since magnetic fluctuations are entangled with ferroelectric fluctuations. We thus suggest that any ferroelectric quantum critical point is an \textit{inherent} multiferroic quantum critical point. We calculate the magnetic susceptibility near the FE QCP and find a region with enhanced magnetic signatures that appears near the FE QCP, and controlled by the tuning parameter of the ferroelectric phase. The effect is small but observable - we propose quantum paraelectric strontium titanate as a candidate material where the magnitude of the induced magnetic moments can be $\sim 5 \times 10^{-7} μ_{B}$ per unit cell near the FE QCP.

cond-mat.str-el↗

arXiv2019

Ultrafast transient increase of oxygen octahedral rotations in a perovskite

The ability to control the structure of a crystalline solid on ultrafast timescales bears enormous potential for information storage and manipulation or generating new functional states of matter [1]. In many materials where the ultrafast control of crystalline structures has been explored, optical excitation pushes materials towards their less ordered high temperature phase [2{9] as electronically driven ordered phases melt and possible concomitant structural modifications relax. Nonetheless, for a few select materials it has been shown that photoexcitation can slightly enhance the amplitude of an electronic ordering phenomenon (i.e. its electronic order parameter) [9{13]. Here we show via femtosecond hard X-ray diffraction that photodoping of the perovskite EuTiO3 transiently increases the order parameter associated with a purely structural [14] phase transition represented by the antiferrodistortive rotation of the oxygen octahedra. This can be understood from an ultrafast charge-transfer induced reduction of the Goldschmidt tolerance factor [15], which is a fundamental control parameter for the properties of perovskites

cond-mat.str-el↗

arXiv2019

Search for the magnetic monopole at a magnetoelectric surface

We show, by solving Maxwell's equations, that an electric charge on the surface of a slab of a linear magnetoelectric material generates an image magnetic monopole below the surface provided that the magnetoelectric has a diagonal component in its magnetoelectric response. The image monopole, in turn, generates an ideal monopolar magnetic field outside of the slab. Using realistic values of the electric- and magnetic- field susceptibilties, we calculate the magnitude of the effect for the prototypical magnetoelectric material Cr$_2$O$_3$. We use low energy muon spin rotation to measure the strength of the magnetic field generated by charged muons as a function of their distance from the surface of a Cr$_2$O$_3$ films, and show that the results are consistent with the existence of the monopole. We discuss other possible routes to detecting the monopolar field, and show that, while the predicted monopolar field generated by Cr$_2$O$_3$ is above the detection limit for standard magnetic force microscopy, detection of the field using this technique is prevented by surface charging effects.

cond-mat.mtrl-sci↗

arXiv2018

Magnetophononics: ultrafast spin control through the lattice

Using a combination of first-principles and magnetization-dynamics calculations, we study the effect of the intense optical excitation of phonons on the magnetic behavior in insulating magnetic materials. Taking the prototypical magnetoelectric \CrO\ as our model system, we show that excitation of a polar mode at 17 THz causes a pronounced modification of the magnetic exchange interactions through a change in the average Cr-Cr distance. In particular, the quasi-static deformation induced by nonlinear phononic coupling yields a structure with a modified magnetic state, which persists for the duration of the phonon excitation. In addition, our time-dependent magnetization dynamics computations show that systematic modulation of the magnetic exchange interaction by the phonon excitation modifies the magnetization dynamics. This temporal modulation of the magnetic exchange interaction strengths using phonons provides a new route to creating non-equilibrium magnetic states and suggests new avenues for fast manipulation of spin arrangements and dynamics.

cond-mat.str-el↗

arXiv2017

Strain and ferroelectric soft mode induced superconductivity in strontium titanate

We investigate the effects of strain on superconductivity with particular reference to SrTiO$_3$. Assuming that a ferroelectric mode that softens under tensile strain is responsible for the coupling, an increase in the critical temperature and range of carrier densities for superconductivity is predicted, while the peak of the superconducting dome shifts towards lower carrier densities. Using a Ginzburg-Landau approach in 2D, we find a linear dependence of the critical temperature on strain: if the couplings between the order parameter and strains in different directions differ while their sum is fixed, different behaviours under uniaxial and biaxial (uniform) strain can be understood.

cond-mat.supr-con↗

arXiv2017

Evidence of incoherent carriers associated with resonant impurity levels and their influence on superconductivity in the anomalous superconductor Pb$_{1-x}$Tl$_x$Te

We present a combined experimental and theoretical study of the evolution of the Fermi surface of the anomalous superconductor Pb$_{1-x}$Tl$_x$Te as a function of thallium concentration, drawing on a combination of magnetotransport measurements (Shubnikov de Haas oscillations and Hall coefficient), Angle Resolved Photoemission Spectroscopy (ARPES), and density functional theory (DFT) calculations of the electronic structure. Our results indicate that for Tl concentrations beyond a critical value the Fermi energy coincides with resonant impurity states in Pb$_{1-x}$Tl$_x$Te, and we rule out the presence of an additional valence band maximum at the Fermi energy. Through comparison to non-superconducting Pb$_{1-x}$Na$_x$Te we argue that the presence of these states at the Fermi energy provides the pairing interaction and thus also the anomalously high temperature superconductivity in this material.

cond-mat.supr-con↗

arXiv2017

Global formation of topological defects in the multiferroic hexagonal manganites

The spontaneous transformations associated with symmetry-breaking phase transitions generate domain structures and defects that may be topological in nature. The formation of these defects can be described according to the Kibble-Zurek mechanism, which provides a generic relation that applies from cosmological to interatomic lengthscales. Its verification is challenging, however, in particular at the cosmological scale where experiments are impractical. While it has been demonstrated for selected condensed-matter systems, major questions remain regarding e.g. its degree of universality. Here we develop a global Kibble-Zurek picture from the condensed-matter level. We show theoretically that a transition between two fluctuation regimes (Ginzburg and mean-field) can lead to an intermediate region with reversed scaling, and we verify experimentally this behavior for the structural transition in the series of multiferroic hexagonal manganites. Trends across the series allow us to identify additional intrinsic features of the defect formation beyond the original Kibble-Zurek paradigm.

cond-mat.mtrl-sci↗

arXiv2016

Fermi surface evolution of Na-doped PbTe studied through density functional theory calculations and Shubnikov-de Haas measurements

We present a combined experimental and theoretical study of the evolution of the low-temperature Fermi surface of lead telluride, PbTe, when holes are introduced through sodium substitution on the lead site. Our Shubnikov-de-Haas measurements for samples with carrier concentrations up to $9.4\times10^{19}$cm$^{-3}$ (0.62 Na atomic $\%$) show the qualitative features of the Fermi surface evolution (topology and effective mass) predicted by our density functional (DFT) calculations within the generalized gradient approximation (GGA): we obtain perfect ellipsoidal L-pockets at low and intermediate carrier concentrations, evolution away from ideal ellipsoidicity for the highest doping studied, and cyclotron effective masses increasing monotonically with doping level, implying deviations from perfect parabolicity throughout the whole band. Our measurements show, however, that standard DFT calculations underestimate the energy difference between the L-point and $Σ$-line valence band maxima, since our data are consistent with occupation of a single Fermi surface pocket over the entire doping range studied, whereas the calculations predict an occupation of the $Σ$-pockets at higher doping. Our results for low and intermediate compositions are consistent with a non-parabolic Kane-model dispersion, in which the L-pockets are ellipsoids of fixed anisotropy throughout the band, but the effective masses depend strongly on Fermi energy.

cond-mat.mtrl-sci↗

arXiv2015

Quasi-static magnetoelectric quadrupoles as the order parameter for the pseudo-gap phase in cuprate superconductors

We introduce a mechanism in which coupling between fluctuating spin magnetic dipole moments and polar optical phonons leads to a non-zero ferroic ordering of quasi-static magnetoelectric multipoles. Using first-principles calculations within the LSDA$+U$ method of density functional theory, we calculate the magnitude of the effect for the prototypical cuprate superconductor, HgBa$_2$CuO$_4$. We show that our proposed mechanism is consistent, to our knowledge, with all experimental data for the onset of the pseudo-gap phase and therefore propose the quasi-static magnetoelectric multipole as a possible pseudo-gap order parameter. Finally, we show that our mechanism embraces some key aspects of previous theoretical models, in particular the description of the pseudo-gap phase in terms of orbital currents.

cond-mat.supr-con↗

arXiv2015

Magnetoelectro-elastic control of magnetism in an artificial multiferroic

We study the coexistence of strain- and charge-mediated magnetoelectric coupling in a cobalt (0-7 nm) wedge on ferroelectric [Pb(Mg$_{1/3}$/Nb$_{2/3}$)O$_{3}$]$_{0.68}$-[PbTiO$_{3}$]$_{0.32}$ (011) using surface-sensitive x-ray magnetic circular dichroism spectroscopy at the Co L$_{3,2}$ edges. Three distinct electric field driven remanent magnetization states can be set in the Co film at room temperature. Ab-initio density functional theory calculations unravel the relative contributions of both strain and charge to the observed magnetic anisotropy changes illustrating magnetoelectro-elastic coupling at artificial multiferroic interfaces.

cond-mat.mtrl-sci↗

arXiv2015

A Bespoke Single-Band Hubbard Model Material

The Hubbard model, which augments independent-electron band theory with a single parameter to describe electron-electron correlations, is widely regarded to be the `standard model' of condensed matter physics. The model has been remarkably successful at addressing a range of correlation effects in solids, but beyond one dimension its solution is intractable. Much current research aims, therefore, at finding appropriate approximations to the Hubbard model phase diagram. Here we take the new approach of using ab initio electronic structure methods to design a material whose Hamiltonian is that of the single-band Hubbard model. Solution of the Hubbard model will then be available through measurement of the material's properties. After identifying an appropriate crystal class and several appropriate chemistries, we use density functional theory and dynamical mean-field theory to screen for the desired electronic band structure and metal-insulator transition. We then explore the most promising candidates for structural stability and suitability for doping and propose specific materials for subsequent synthesis. Finally, we identify a regime -- that should manifest in our bespoke material -- in which the single-band Hubbard model on a triangular lattice exhibits exotic d-wave superconductivity.

cond-mat.str-el↗

arXiv2015

Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5

THz-frequency optical pulses can resonantly drive selected vibrational modes in solids and deform their crystal structure. In complex oxides, this method has been used to melt electronic orders, drive insulator to metal transitions or induce superconductivity. Strikingly, coherent interlayer transport strongly reminiscent of superconductivity can be transiently induced up to room temperature in YBa2Cu3O6+x. By combining femtosecond X-ray diffraction and ab initio density functional theory calculations, we determine here the crystal structure of this exotic non-equilibrium state. We find that nonlinear lattice excitation in normal-state YBa2Cu3O6+x at 100 K causes a staggered dilation/contraction of the Cu-O2 intra/inter- bilayer distances, accompanied by anisotropic changes in the in-plane O-Cu-O bond buckling. Density functional theory calculations indicate that these motions cause dramatic changes in the electronic structure. Amongst these, the enhancement in the dx2-y2 character of the in-plane electronic structure is likely to favor superconductivity.

cond-mat.supr-con↗

arXiv2015

Incommensurate magnetic structure, Fe/Cu chemical disorder and magnetic interactions in the high-temperature multiferroic YBaCuFeO5

Motivated by the recent observations of incommensurate magnetic order and electric polarization in YBaCuFeO5 up to temperatures TN2 as high as 230K [1,2] we report here for the first time a model for the incommensurate magnetic structure of this material that we complement with ab-initio calculations of the magnetic exchange parameters. Using neutron powder diffraction we show that the appearance of polarization below TN2 is accompanied by the replacement of the high temperature collinear magnetic order by a circular inclined spiral with propagation vector ki=(1/2, 1/2, 1/2+-q). Moreover, we find that the polarization approximately scales with the modulus of the magnetic modulation vector q down to the lowest temperature investigated (T=3K). Further, we observe occupational Fe/Cu disorder in the FeO5-CuO5 bipyramids, although a preferential occupation of such units by Fe-Cu pairs is supported by the observed magnetic order and by density functional calculations. We calculate exchange coupling constants for different Fe/Cu distributions and show that, for those containing Fe-Cu dimers, the resulting magnetic order is compatible with the experimentally observed collinear magnetic structure (kc=(1/2, 1/2, 1/2), TN2 > T > TN1 = 440K). Based on these results we discuss possible origins for the incommensurate modulation and its coupling with ferroelectricity.

cond-mat.str-el↗