arXiv subjects

S. W. Lovesey

Publications and source records attributed to S. W. Lovesey.

At least 37 records · Page 2Linked to original sources

arXiv2020

Diffraction by multipoles in a 5d2 rhenium double perovskite

A recent polarized neutron diffraction experiment on the 5d2 rhenium double perovskite Ba2YReO6 held at a low temperature uncovered weak magnetic diffraction peaks. Data analysis inferred a significantly reduced Re dipole moment, and long-range order compatible with an antiferromagnet, non-collinear motif. To interpret the experimental findings, we present a model wavefunction for Re ions derived from the crystal field potential, Coulomb interaction, and spin-orbit coupling that fully respects the symmetry of the low-temperature ordered state. It is used to calculate in analytic form all multipole moments visible in neutron and resonance enhanced x-ray diffraction. A minimal model consistent with available neutron diffraction data predicts significant multipolar moments up to the hexadecapole, and, in particular, a dominant charge-like quadrupole moment. Calculated diffraction patterns embrace single crystal x-ray diffraction at the Re L-edge, and renewed neutron diffraction, to probe the presumed underlying multipolar order.

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arXiv2020

Multipole Orders in a Chain Ferrate Na2FeSe

Fundamental block and staggered orders of magnetic Fe multipoles in Na2FeSe2 are classified by their symmetry and magnetoelectric properties. Our structure model incorporates ferromagnetic or antiferromagnetic coupling between chains. The ferrate salt is valued in studies of highly correlated electrons as the only iron selenide known to possess chain-like structural units hosting ferrous cations. Axial and polar (Dirac) multipoles are compulsory in the electronic structure since Fe ions exhibit enantiomorphic symmetry in the parent K2ZnO2-type compound. Calculated Bragg diffraction patterns for neutrons and x-rays reveal specific contributions from both multipole types.

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arXiv2020

Lone octupole and bulk magnetism in osmate 5d2 double perovskites

Cubic double perovskites that host heavy ions with total angular momentum J = 2 can exhibit a singular magnetic state epitomized by a lone octupole and bulk ferro-type magnetism. It exists in the Chen - Balents Hamiltonian with a quadrupole interaction and competing exchange forces between the ions. Our symmetry inspired analysis mirrors the Dzyaloshinskii - Man'ko theory of latent antiferromagnetic ordering, and a 3-k collinear structure. Experimental tests of the singular state include neutron and x-ray Bragg diffraction.

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arXiv2020

Magnetic multipoles and correlation shortage in pyrochlore cerium stannate

Cerium electronic multipoles in trigonal symmetry viewed in magnetic neutron diffraction are investigated. Analytic expressions for all the magnetic multipoles, and radial integrals calculated with an established atomic code, are used to scrutinize a recent claim to have observed an octupole-ice configuration in a powder sample of pyrochlore Ce2Sn2O7. Three equally plausible suites of multipoles belonging to uncorrelated cerium ions give equally satisfactory accounts of the available diffraction pattern. Our multipoles are suitable for future experiments using Bragg diffraction from a compound that supports long-range magnetic order.

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arXiv2019

Circular dichroism of second harmonic generation response

Polarization-dependent photon spectroscopy (dichroism) of the second-harmonic generation (SHG) response is shown to reveal chiral and magnetic properties of a sample. Two dichroic signals are allowed with electric-dipole (E1) and electric-quadrupole (E2) scattering events, and both require circular polarization in the primary beam. Explicit expressions for electronic multipoles, which benefit from equivalent electronic operators, in NCD and MCD of the SHG response are derived using theoretical techniques from atomic physics.

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arXiv2018

Field-induced magnetic charge in a cubic Laves compound UAl2

Magnetic diffraction of polarized neutrons by the cubic Laves compound UAl2 in a magnetic field has unveiled weak Bragg spots that are nominally forbidden. On the one hand, they can be viewed as magnetic analogues of the basis-forbidden (2, 2, 2) reflection in diamond-type structures that has been painstakingly and frequently investigated over almost a century. Alternatively, the pattern of weak intensities can be assigned to Dirac multipoles imbedded in field-induced magnetic charge. To this end, a published diffraction pattern is successfully confronted with intensities calculated from the appropriate magnetic space-group that includes Dirac dipoles (anapoles) to describe the basis-forbidden magnetic reflections, and conventional (axial) dipole and octupole multipoles to describe basis-allowed magnetic reflections.

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arXiv2018

Direct observation of anapoles by neutron diffraction

The scope of magnetic neutron scattering has been expanded by the observation of electronic Dirac dipoles (anapoles) that are polar (parity-odd) and magnetic (time-odd). A zero-magnetization ferromagnet Sm0.976Gd0.024Al2 with a diamond-type structure presents Dirac multipoles at basis-forbidden reflections that include the standard (2, 2, 2) reflection. Magnetic amplitudes measured at four such reflections are in full accord with a structure factor calculated from the appropriate magnetic space group.

cond-mat.mtrl-sci↗

arXiv2018

Superchiral photons unveil magnetic circular dichroism

Polarization-dependent photon spectroscopy (dichroism) using signal-enhancing superchiral beams is shown to be sensitive to magnetic properties of the sample, whereas previous investigations explored charge-like electronic properties of chiral samples. In the process of unveiling the potential to observe magnetic circular dichroism (MCD), we underline an affinity between spectroscopies using the Borrmann effect, twisted beams and superchiral beams. Use of an effective wavevector in a quantum-mechanical theory unites the aforementioned spectroscopies and vastly improves our understanding of their advantages. Exploiting an effective wavevector for superchiral beams, natural circular dichroism (NCD) is derived from electric dipole - magnetic dipole (E1-M1) and electric dipole - electric quadrupole (E1-E2) absorption events, and MCD is derived from electric quadrupole-electric quadrupole (E2-E2) absorption. Signal enhancement by superchiral beams is a straightforward gain for the user because NCD and MCD are otherwise precisely the same as for a circularly polarized beam, according to our calculations. Our analysis shows that enhancement of E2-E2 is superior to that available for parity-odd events under consideration. Electronic degrees of freedom in all dichroic signals are encapsulated in atomic multipoles that are frequently used in theoretical interpretations of several established experimental techniques.

cond-mat.mtrl-sci↗

arXiv2018

Direct observation of electron density reconstruction at the metal-insulator transition in NaOsO3

5d transition metal oxides offer new opportunities to test our understanding of the interplay of correlation effects and spin-orbit interactions in materials in the absence of a single dominant interaction. The subtle balance between solid-state interactions can result in new mechanisms that minimize the interaction energy, and in material properties of potential use for applications. We focus here on the 5d transition metal oxide NaOsO3, a strong candidate for the realization of a magnetically driven transition from a metallic to an insulating state exploiting the so-called Slater mechanism. Experimental results are derived from non-resonant and resonant x-ray single crystal diffraction at the Os L-edges. A change in the crystallographic symmetry does not accompany the metal-insulator transition in the Slater mechanism and, indeed, we find no evidence of such a change in NaOsO3. An equally important experimental observation is the emergence of the (300) Bragg peak in the resonant condition with the onset of magnetic order. The intensity of this space-group forbidden Bragg peak continuously increases with decreasing temperature in line with the square of intensity observed for an allowed magnetic Bragg peak. Our main experimental results, the absence of crystal symmetry breaking and the emergence of a space-group forbidden Bragg peak with developing magnetic order, support the use of the Slater mechanism to interpret the metal-insulator transition in NaOsO3. We successfully describe our experimental results with simulations of the electronic structure and, also, with an atomic model based on the established symmetry of the crystal and magnetic structure.

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arXiv2017

Neutron scattering by Dirac multipoles

Ordered magnetic charge created by Dirac multipoles that are magnetic and polar is examined. It has previously been revealed in the pseudo-gap phase of high-Tc materials by use of the Kerr effect and magnetic neutron Bragg diffraction. There are several forms of the polar operator for magnetic neutron scattering built from spin and electric dipole operators of unpaired electrons. Construction of Dirac quadrupoles that emerge from centrosymmetric sites used by Cu ions in the ceramic superconductor Hg1201 is illustrated, together with selection rules for excitations that will feature in neutron inelastic scattering, and RIXS experiments. Most reported expressions and results have universal value, because they are not specific to ceramic superconductors. To illustrate this aspect of our work we simulate neutron diffraction from a magnetically ordered iridate (Sr2IrO4).

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arXiv2016

Electronic and magnetic properties of orthorhombic iron selenide (FeSe)

Iron orbitals in orthorhombic iron selenide (FeSe) can produce charge-like multipoles that are polar (parity-odd). Orbitals in question include Fe(3d), Fe(4p) and p-type ligands that participate in transport properties and bonding. The polar multipoles may contribute weak, space-group forbidden Bragg spots to diffraction patterns collected with x-rays tuned in energy to a Fe atomic resonance (Templeton & Templeton scattering). Ordering of conventional, axial magnetic dipoles does not accompany the tetragonal-orthorhombic structural phase transition in FeSe, unlike other known iron-based superconductors. We initiate a new line of inquiry for this puzzling property of orthorhombic FeSe, using a hidden magnetic-order that belongs to the m'm'm' magnetic crystal-class. It is epitomized by the absence of ferromagnetism and axial magnetic dipoles, and the appearance of magnetic monopoles and magneto-electric quadrupoles. A similar magnetic order occurs in cuprate superconductors, YBCO & Hg1201, where it was unveiled with the Kerr effect and in Bragg diffraction patterns revealed by polarized neutrons. PACS number 75.25.-j

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arXiv2015

Ordered state of magnetic charge in the pseudo-gap phase of a cuprate superconductor (HgBa2CuO4)

A symmetry-based interpretation of published experimental results demonstrates that the pseudo-gap phase of underdoped HgBa2CuO4(Hg1201) possesses an ordered state of magnetic charge epitomized by Cu magnetic monopoles. Magnetic properties of one-layer Hg1201 and two-layer YBa2Cu3O6 + x (YBCO) cuprates have much in common, because their pseudo-gap phases possess the same magnetic space-group, e.g., both underdoped cuprates allow the magneto-electric (Kerr) effect. Differences in their properties stem from different Cu site symmetries, leaving Cu magnetic monopoles forbidden in YBCO. Resonant x-ray Bragg diffraction experiments can complement the wealth of information available from neutron diffraction experiments on five Hg1201 samples on which our findings are based. In the case of Hg1201 emergence of the pseudo-gap phase, with time-reversal violation, is accompanied by a reduction of Cu site symmetry that includes loss of a centre of inversion symmetry. In consequence, parity-odd x-ray absorption events herald the onset of the enigmatic phase, and we predict dependence of corresponding Bragg spots on magneto-electric multipoles, including the monopole, and the azimuthal angle (crystal rotation about the Bragg wavevector).

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arXiv2015

Ferro-type order of magneto-electric quadrupoles as an order-parameter for the pseudo-gap phase of a cuprate superconductor

Understanding the pseudo-gap phase from which a superconducting state emerges is a central problem in the physics of cuprates. The phase exists below a temperature T* for less than optimal doping of holes, and no clear jump in the specific heat or change in lattice symmetry is observed on crossing T*. Here we show that, two sets of intriguing experimental results in the literature concerning magnetic properties of underdoped YBCO are united in a single theory based on Cu quadrupole moments. The quadrupole is a product of spin and the electric dipole, so there is no magnetic dipole moment, and standard crystallography describes the magnetic motif. One experiment employed the Kerr effect and the second Bragg diffraction of polarized neutrons, and both are shown to imply an order-parameter for the pseudo-gap phase composed of magneto-electric quadrupoles at in-plane Cu sites in a ferro-type order. The successful interpretation of neutron diffraction data for YBCO yields the first experimental evidence that neutrons are deflected by magneto-electric multipoles. Predicted in 2014, our verification of the effect validates a new application for the experimental technique of choice in studies of magnetic motifs and excitations.

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arXiv2015

Ferro-type order of magneto-electric quadrupoles in the pseudo-gap phase of YBa2Cu3O6 + x unearthed by neutron diffraction

A theory that fully describes previously observed neutron Bragg spots indicative of magnetic order in the pseudo-gap phase of YBa2Cu3O6 + x is presented. Magnetic diffraction intensities, unveiled by polarization analysis, are explained by parity-violating magnetic (magneto-electric) quadrupoles at in-plane Cu sites arranged in a simple ferro-type motif. An absence of conventional spin and orbital angular momentum dipoles in the theory is compatible with the occurrence of superconductivity and strongly suggests, moreover, that magneto-electric quadrupoles are the primary order-parameter in the pseudo-gap phase.

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arXiv2014

A model of magneto-electric multipoles

An ancient Hamiltonian of electrons with entangled spin and orbital degrees of freedom is re-examined as a model of magneto-electric multipoles. In the model, a magnetic charge and simple quantum rotator are tightly locked in action, some might say they are enslaved entities. It is shown that magneto-electric multipoles almost perfectly accord with those inferred from an analysis of magnetic neutron diffraction data on a ceramic superconductor (YBCO) in the pseudo-gap phase. Nigh on perfection between Stone's model and inferred magneto-electric multipoles is achieved by addition to the original model of a crystal-field potential appropriate for the magnetic space-group used in the published data analysis

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arXiv2014

Symmetry of re-entrant tetragonal phase in Ba1-xNaxFe2As2: Magnetic versus orbital ordering mechanism

Magneto-structural phase transitions in Ba1-xAxFe2As2 (A = K, Na) materials are discussed for both magnetically and orbitally driven mechanisms, using a symmetry analysis formulated within the Landau theory of phase transitions. Both mechanisms predict identical orthorhombic space-group symmetries for the nematic and magnetic phases observed over much of the phase diagram, but they predict different tetragonal space-group symmetries for the newly discovered re-entrant tetragonal phase in Ba1-xNaxFe2As2 (x ~ 0.24-0.28). In a magnetic scenario, magnetic order with moments along the c-axis, as found experimentally, does not allow any type of orbital order, but in an orbital scenario, we have determined two possible orbital patterns, specified by P4/mnc1' and I4221' space groups, which do not require atomic displacements relative to the parent I4/mmm1' symmetry and, in consequence, are indistinguishable in conventional diffraction experiments. We demonstrate that the three possible space groups are however, distinct in resonant X-ray Bragg diffraction patterns created by Templeton & Templeton scattering. This provides an experimental method of distinguishing between magnetic and orbital models.

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arXiv2013

Chiral properties of hematite (α-Fe2O3) inferred from resonant Bragg diffraction using circularly polarized x-rays

Chiral properties of the two phases - collinear motif (below Morin transition temperature, TM=250 K) and canted motif (above TM) - of magnetically ordered hematite (α-Fe2O3) have been identified in single crystal resonant x-ray Bragg diffraction, using circular polarized incident x-rays tuned near the iron K-edge. Magneto-electric multipoles, including an anapole, fully characterize the high-temperature canted phase, whereas the low-temperature collinear phase supports both parity-odd and parity-even multipoles that are time-odd. Orbital angular momentum accompanies the collinear motif, while it is conspicuously absent with the canted motif. Intensities have been successfully confronted with analytic expressions derived from an atomic model fully compliant with chemical and magnetic structures. Values of Fe atomic multipoles previously derived from independent experimental data, are shown to be completely trustworthy.

cond-mat.mtrl-sci↗

arXiv2011

Triakontadipole and high-order dysprosium multipoles in the antiferromagnetic phase of DyB$_2$C$_2$

Resonant soft x-ray Bragg diffraction at the Dy M$_{4,5}$ edges has been used to study Dy multipoles in the combined magnetic and orbitally ordered phase of DyB$_2$C$_2$. The analysis incorporates both the intra-atomic magnetic and quadrupolar interactions between the 3d core and 4f valence shells. Additionally, we introduce to the formalism the interference of magnetic and nonmagnetic oscillators. This allows a determination of the higher order multipole moments of rank 1 (dipole) to 6 (hexacontatetrapole). The strength of the Dy 4f multipole moments have been estimated at being between 7 and 78 % of the quadrupolar moment.

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