arXiv subjects

A. Bombardi

Publications and source records attributed to A. Bombardi.

At least 19 recordsLinked to original sources

arXiv2026

Phase-Sensitive Nonlinear X-Ray Response in a Charge-Density-Wave Quantum Material

We report a phase-sensitive nonlinear x-ray response in the charge-density-wave material 1T-TaS2, revealed through x-ray parametric down-conversion into the ultraviolet. Extending nonlinear x-ray wave mixing beyond conventional crystalline systems to a correlated quantum material, we employ reciprocal-lattice phase matching to isolate distinct Fourier components of the nonlinear susceptibility. By selecting a fundamental reciprocal-lattice vector and a stacking-sensitive half-integer reciprocal-lattice vector, we probe the response across the nearly commensurate and incommensurate charge-density-wave phases. Tuning the ultraviolet photon energy through Ta O-shell resonances uncovers pronounced Fourier-component and phase-dependent resonant structure, indicating that the stacking-related nonlinear susceptibility couples differently to Ta-centered resonant states than the average lattice response. Remarkably, the nonlinear signal is strongly enhanced in the nearly commensurate phase despite weaker Bragg diffraction, demonstrating that the nonlinear susceptibility provides information inaccessible to linear probes. These results establish nonlinear x-ray spectroscopy as a phase-sensitive and orbital-selective probe of electronic reconstruction in quantum materials.

physics.optics↗

arXiv2025

Symmetry-designed BiFeO3 single domain spin cycloid for efficient spintronics

Deterministic control of coupled ferroelectric and antiferromagnetic orders remains a central challenge in multiferroics, limiting their integration into functional magnetoelectrics and magnonic-devices. (111)pc BiFeO3 with a robust single spin cycloid, offers direct magnetoelectric-coupling and a platform for efficient spin transport, yet multi-magnetic domains and ferroelectric-fatigue have prevented reproducible control. Here, we show that anisotropic-compressive in-plane strain stabilizes a single antiferromagnetic domain with unique spin-cycloid vector, by breaking the symmetry of the (111)pc plane. Epitaxial BiFeO3 films grown on orthorhombic NdGaO3 (011)o [(111)pc] substrates impose the required anisotropic in-plane strain and stabilizes single antiferromagnetic domain, as confirmed through direct imaging with scanning NV microscopy and non-resonant-x-ray-magnetic-scattering. Remarkably, these engineered films exhibit deterministic and non-volatile 180° switching of ferroelectric and single antiferromagnetic domains over 1,000 cycles. The monodomain state also enables anisotropic and threefold enhanced magnon transport with reduced scattering. Thus, symmetry-designed (111)pc monodomain BiFeO3 offers a robust platform for advanced magnetoelectric and magnonic applications.

cond-mat.mtrl-sci↗

arXiv2024

Competing charge and magnetic order in the candidate centrosymmetric skyrmion host EuGa$_2$Al$_2$

Eu(Ga$_{1-x}$Al$_x$)$_4$ are centrosymmetric systems that have recently been identified as candidates to stabilise topologically non-trivial magnetic phases, such as skyrmion lattices. In this Letter, we present a high-resolution resonant x-ray and neutron scattering study on EuAl2Ga2 that provides new details of the complex coupling between the electronic ordering phenomena. Our results unambiguously demonstrate that the system orders to form a spin density wave with moments aligned perpendicular to the direction of the propagation vector, and upon further cooling, a cycloid with moments in the ab plane, in contrast to what has been reported in the literature. We show that concomitant with the onset of the spin density wave is the suppression of the charge order, indicative of a coupling between the localised 4$f$ electrons and itinerant electron density. Furthermore we demonstrate that the charge density wave order breaks the four-fold symmetry present in the I4/mmm crystal structure, thus declassifying these systems as square-net magnets.

cond-mat.str-el↗

arXiv2024

Spontaneous spin chirality reversal and competing phases in the topological magnet EuAl$_4$

We demonstrate the spontaneous reversal of spin chirality in a single crystal sample of the intermetallic magnet EuAl$_4$. We solve the nanoscopic nature of each of the four magnetically phases of EuAl$_4$ using resonant magnetic x-ray scattering, and demonstrate all four phases order with single-k incommensurate magnetic modulation vectors. Below 15.4 K the system forms a spin density modulated spin structure where the spins are orientated in the ab plane perpendicular to the orientation of the magnetic propagation vector. Below 13.2 K a second spin density wave orders with moments aligned parallel to the c-axis, such that the two spin density wave orders coexist. Below 12.2 K a magnetic helix of a single chirality is stabilised across the entire sample. Below 10 K the chirality of the magnetic helix reverses, and the sample remains a single chiral domain. Concomitant with the establishment of the helical magnetic ordering is the lowering of the crystal symmetry to monoclinic, as evidenced the formation of uniaxial charge and spin strip domains. A group theoretical analysis demonstrates that below 12.2 K the symmetry lowers to polar monoclinic, which is necessary to explain the observed asymmetry in the chiral states of the magnetic helix and the spin chiral reversal. We find that in every magnetically ordered phase of EuAl4 the in-plane moment is perpendicular to the orientation of the magnetic propagation vector, which we demonstrate is favoured by magnetic dipolar interactions.

cond-mat.str-el↗

arXiv2023

Unusual magnetism of the axion-insulator candidate Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is a member of a family of orthorhombic nonsymmorphic rare-earth intermetallics that combines large localized magnetic moments and itinerant exchange with a low carrier density and perpendicular glide planes. This may result in special topological crystalline (wallpaper fermion) or axion insulating phases. Recent studies of Eu$_5$In$_2$Sb$_6$ single crystals have revealed colossal negative magnetoresistance and multiple magnetic phase transitions. Here, we clarify this ordering process using neutron scattering, resonant elastic X-ray scattering, muon spin-rotation, and magnetometry. The nonsymmorphic and multisite character of Eu$_5$In$_2$Sb$_6$ results in coplanar noncollinear magnetic structure with an Ising-like net magnetization along the $a$ axis. A reordering transition, attributable to competing ferro- and antiferromagnetic couplings, manifests as the onset of a second commensurate Fourier component. In the absence of spatially resolved probes, the experimental evidence for this low-temperature state can be interpreted either as an unusual double-$q$ structure or in a phase separation scenario. The net magnetization produces variable anisotropic hysteretic effects which also couple to charge transport. The implied potential for functional domain physics and topological transport suggests that this structural family may be a promising platform to implement concepts of topological antiferromagnetic spintronics.

cond-mat.str-el↗

arXiv2020

Colossal magnetoresistance in a nonsymmorphic antiferromagnetic insulator

Here we investigate antiferromagnetic Eu$_{5}$In$_{2}$Sb$_{6}$, a nonsymmorphic Zintl phase. Our electrical transport data show that Eu$_{5}$In$_{2}$Sb$_{6}$ is remarkably insulating and exhibits an exceptionally large negative magnetoresistance, which is consistent with the presence of magnetic polarons. From {\it ab initio} calculations, the paramagnetic state of Eu$_{5}$In$_{2}$Sb$_{6}$ is a topologically nontrivial semimetal within the generalized gradient approximation (GGA), whereas an insulating state with trivial topological indices is obtained using a modified Becke-Johnson potential. Notably, GGA+U calculations suggest that the antiferromagnetic phase of Eu$_{5}$In$_{2}$Sb$_{6}$ may host an axion insulating state. Our results provide important feedback for theories of topological classification and highlight the potential of realizing clean magnetic narrow-gap semiconductors in Zintl materials.

cond-mat.str-el↗

arXiv2020

Spin-wave gap collapse in Rh-doped Sr2IrO4

We use resonant inelastic x-ray scattering (RIXS) at the Ir L3 edge to study the effect of hole doping upon the Jeff=1/2 Mott-insulating state in Sr2IrO4, via Rh replacement of the Ir site. The spin-wave gap, associated with XY-type spin-exchange anisotropy, collapses with increasing Rh content, prior to the suppression of the Mott-insulating state and in contrast to electron doping via La substitution of the Sr site. At the same time, despite heavy damping, the d-d excitation spectra retain their overall amplitude and dispersion character. A careful study of the spin-wave spectrum reveals that deviations from the J1-J2-J3 Heisenberg used to model the pristine system disappear at intermediate doping levels. These findings are interpreted in terms of a modulation of Ir-Ir correlations due to the influence of Rh impurities upon nearby Ir wave functions, even as the single-band Jeff=1/2 model remains valid up to full carrier delocalization. They underline the importance of the transition metal site symmetry when doping pseudospin systems such as Sr2IrO4.

cond-mat.str-el↗

arXiv2019

Spin-wave directional anisotropies in antiferromagnetic Ba$_{3}$NbFe$_{3}$Si$_{2}$O$_{14}$

Ba$_{3}$NbFe$_{3}$Si$_{2}$O$_{14}$ (langasite) is structurally and magnetically single domain chiral with the magnetic helicity induced through competing symmetric exchange interactions. Using neutron scattering, we show that the spin-waves in antiferromagnetic langasite display directional anisotropy. On applying a time reversal symmetry breaking magnetic field along the $c$-axis, the spin wave energies differ when the sign is reversed for either the momentum transfer $\pm$ $\vec{Q}$ or applied magnetic field $\pm$ $μ_{0}$H. When the field is applied within the crystallographic $ab$-plane, the spin wave dispersion is directionally \textit{isotropic} and symmetric in $\pm$ $μ_{0}$H. However, a directional anisotropy is observed in the spin wave intensity. We discuss this directional anisotropy in the dispersion in langasite in terms of a field induced precession of the dynamic unit cell staggered magnetization. Directional anisotropy, or often referred to as non reciprocal responses, can occur in antiferromagnetic phases in the absence of the Dzyaloshinskii-Moriya interaction or other effects resulting from spin-orbit coupling.

cond-mat.mtrl-sci↗

arXiv2018

Magnetic Anisotropy and Orbital Ordering in Ca$_2$RuO$_4$

We review the magnetic and orbital ordered states in \cro{} by performing Resonant Elastic X-ray Scattering (REXS) at the Ru L$_{2,3}$-edges. In principle, the point symmetry at Ru sites does not constrain the direction of the magnetic moment below $T_N$. However early measurements reported the ordered moment entirely along the $\vec{b}$ orthorhombic axis. Taking advantage of the large resonant enhancement of the magnetic scattering close to the Ru L$_2$ and L$_3$ absorption edges, we monitored the azimuthal, thermal and energy dependence of the REXS intensity and find that a canting ($m_c \simeq 0.1 m_b$) along the $\vec{c}$-orthorhombic axis is present. No signal was found for $m_a$ despite this component also being allowed by symmetry. Such findings are interpreted by a microscopic model Hamiltonian, and pose new constraints on the parameters describing the model. Using the same technique we reviewed the accepted orbital ordering picture. We detected no symmetry breaking associated with the signal increase at the "so-called" orbital ordering temperature ($\simeq 260$ K). We did not find any changes of the orbital pattern even through the antiferromagnetic transition, suggesting that, if any, only a complex rearrangement of the orbitals, not directly measurable using linearly polarized light, can take place.

cond-mat.str-el↗

arXiv2018

Strain engineering a multiferroic monodomain in thin-film BiFeO$_3$

The presence of domains in ferroic materials can negatively affect their macroscopic properties and hence their usefulness in device applications. From an experimental perspective, measuring materials comprising multiple domains can complicate the interpretation of material properties and their underlying mechanisms. In general, BiFeO$_3$ films tend to grow with multiple magnetic domains and often contain multiple ferroelectric and ferroelastic domain variants. By growing (111)-oriented BiFeO$_3$ films on an orthorhombic TbScO$_3$ substrate, we are able to overcome this, and, by exploiting the magnetoelastic coupling between the magnetic and crystal structures, bias the growth of a given magnetic-, ferroelectric-, and structural-domain film. We further demonstrate the coupling of the magnetic structure to the ferroelectric polarisation by showing the magnetic polarity in this domain is inverted upon 180$^\circ$ ferroelectric switching

cond-mat.str-el↗

arXiv2018

Persistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca$_2$RuO$_4$

The chemical and magnetic structures of the series of compounds Ca$_{2-x}$La$_x$RuO$_4$ [$x = 0$, $0.05(1)$, $0.07(1)$, $0.12(1)$] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low temperature S-Pbca space group of the parent compound is retained in all insulating samples [$x\leq0.07(1)$], but with significant changes to the atomic positions within the unit cell. These changes can be characterised in terms of the local RuO$_6$ octahedral coordination: with increasing doping the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasi-tetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic $k=(0,0,0)$, $b$-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of $x\approx0.11$. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favouring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the $d^4$ Mott insulator Ca$_2$RuO$_4$, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.

cond-mat.str-el↗

arXiv2018

Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr2O4

In spinels ACr2O4 (A=Mg, Zn) realisation of the classical pyrochlore Heisenberg antiferromagnet model is complicated by a strong spin-lattice coupling: the extensive degeneracy of the ground state is lifted by a magneto-structural transition at TN=12.5 K. We study the resulting low-temperature low-symmetry crystal structure by synchrotron x-ray diffraction. The consistent features of x-ray low-temperature patterns are explained by the tetragonal model of Ehrenberg et. al (Pow. Diff. 17, 230( 2002)), while other features depend on sample or cooling protocol. Complex partially ordered magnetic state is studied by neutron diffraction and spherical neutron polarimetry. Multiple magnetic domains of configuration arms of the propagation vectors k1=(1/2 1/2 0), k2=(1 0 1/2) appear. The ordered moment reaches 1.94(3) muB/Cr3+ for k1 and 2.08(3) muB/Cr3+ for k2, if equal amount of the k1 and k2 phases is assumed. The magnetic arrangements have the dominant components along the [110] and [1-10] diagonals and a smaller c-component. By inelastic neutron scattering we investigate the spin excitations, which comprise a mixture of dispersive spin waves propagating from the magnetic Bragg peaks and resonance modes centered at equal energy steps of 4.5 meV. We interpret these as acoustic and optical spin wave branches, but show that the neutron scattering cross sections of transitions within a unit of two corner-sharing tetrahedra match the observed intensity distribution of the resonances. The distinctive fingerprint of cluster-like excitations in the optical spin wave branches suggests that propagating excitations are localized by the complex crystal structure and magnetic orders.

cond-mat.str-el↗

arXiv2017

Electrical switching of magnetic polarity in a multiferroic BiFeO3 device at room temperature

We have directly imaged reversible electrical switching of the cycloidal rotation direction (magnetic polarity) in a (111)-BiFeO3 epitaxial-film device at room temperature by non-resonant x-ray magnetic scattering. Consistent with previous reports, fully relaxed (111)-BiFeO3 epitaxial films consisting of a single ferroelectric domain were found to comprise a sub-micron-scale mosaic of magneto-elastic domains, all sharing a common direction of the magnetic polarity, which was found to switch reversibly upon reversal of the ferroelectric polarization without any measurable change of the magneto-elastic domain population. A real-space polarimetry map of our device clearly distinguished between regions of the sample electrically addressed into the two magnetic states with a resolution of a few tens of micron. Contrary to the general belief that the magneto-electric coupling in BiFeO3 is weak, we find that electrical switching has a dramatic effect on the magnetic structure, with the magnetic moments rotating on average by 90 degrees at every cycle.

cond-mat.str-el↗

arXiv2016

Coherent magneto-elastic domains in multiferroic BiFeO3 films

The physical properties of epitaxial films can fundamentally differ from those of bulk single crystals even above the critical thickness. By a combination of non-resonant x-ray magnetic scattering, neutron diffraction and vector-mapped x-ray magnetic linear dichroism photoemission electron microscopy, we show that epitaxial (111)-BiFeO3 films support sub-micron antiferromagnetic domains, which are magneto-elastically coupled to a coherent crystallographic monoclinic twin structure. This unique texture, which is absent in bulk single crystals, should enable control of magnetism in BiFeO3 film devices via epitaxial strain.

cond-mat.str-el↗

arXiv2016

Modulated spin helicity stabilized by incommensurate orbital density waves in a quadruple perovskite manganite

Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48 K, the primary magnetic order parameter is locked into the orbital wave by an admixture of helical and collinear spin density wave structures. Furthermore, our model naturally explains the lack of a sharp dielectric anomaly at TN1 and the unusual temperature dependence of the electrical polarisation.

cond-mat.str-el↗

arXiv2016

Incommensurate Counterrotating Magnetic Order Stabilized by Kitaev Interactions in the Layered Honeycomb $α$-Li$_2$IrO$_3$

The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counter-rotating on nearest-neighbour sites. This type of magnetic structure has not been reported experimentally before in honeycomb magnets and cannot be explained by a spin Hamiltonian with dominant isotropic (Heisenberg) couplings. The magnetic structure shares many key features with the magnetic order in the structural polytypes $β$ and $γ$-Li$_2$IrO$_3$, understood theoretically to be stabilized by dominant Kitaev interactions between Ir moments located on the vertices of three-dimensional hyperhoneycomb and stripyhoneycomb lattices, respectively. Based on this analogy and a theoretical soft-spin analysis of magnetic ground states for candidate spin Hamiltonians, we propose that Kitaev interactions also dominate in $α$-Li$_2$IrO$_3$, indicative of universal Kitaev physics across all three members of the harmonic honeycomb family of Li$_2$IrO$_3$ polytypes.

cond-mat.str-el↗

arXiv2015

Two-dimensional Cs-vacancy superstructure in iron-based superconductor $Cs_{0.8}Fe_{1.6}Se_2$

Single crystal neutron diffraction is combined with synchrotron x-ray scattering to identify the different superlattice phases present in $Cs_{0.8}Fe_{1.6}Se_2$. A combination of single crystal refinements and first principles modelling are used to provide structural solutions for the $\sqrt{5}\times\sqrt{5}$ and $\sqrt{2}\times\sqrt{2}$ superlattice phases. The $\sqrt{5}\times\sqrt{5}$ superlattice structure is predominantly composed of ordered Fe vacancies and Fe distortions, whereas the $\sqrt{2}\times\sqrt{2}$ superlattice is composed of ordered Cs vacancies. The Cs vacancies only order within the plane, causing Bragg rods in reciprocal space. By mapping x-ray diffraction measurements with narrow spatial resolution over the surface of the sample, the structural domain pattern was determined, consistent with the notion of a majority antiferromagnetic $\sqrt{5}\times\sqrt{5}$ phase and a superconducting $\sqrt{2}\times\sqrt{2}$ phase.

cond-mat.supr-con↗

arXiv2014

Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in $β$-Li2IrO3: full solution via magnetic resonant x-ray diffraction

The recently-synthesized iridate $β$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic structure. We find a complex, incommensurate magnetic order with non-coplanar and counter-rotating Ir moments, which surprisingly shares many of its features with the related structural polytype "stripyhoneycomb" $γ$-Li$_2$IrO$_3$, where dominant Kitaev interactions have been invoked to explain the stability of the observed magnetic structure. The similarities of behavior between those two structural polytypes, which have different global lattice topologies but the same local connectivity, is strongly suggestive that the same magnetic interactions and the same underlying mechanism governs the stability of the magnetic order in both materials, indicating that both $β$- and $γ$-Li$_2$IrO$_3$ are strong candidates to realize dominant Kitaev interactions in a solid state material.

cond-mat.str-el↗