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Veronika Sunko

Publications and source records attributed to Veronika Sunko.

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Strain continuously rotates the Néel vector in altermagnetic MnTe

Altermagnetism has recently emerged as a distinct class of collinear antiferromagnets that break time-reversal symmetry, exhibiting a host of novel properties. Applied strain has attracted particular attention as a key tuning parameter for altermagnets. Although several experimental studies have demonstrated the preparation of single-domain states through a combination of applied strain and magnetic field, the route to such states remains unclear. Here, we use magneto-optical measurements on single crystals of MnTe under applied strain to show that, in contrast to previous reports, strain acts primarily to rotate the Néel vector L continuously. Since the orientation of L determines the magnetic point group symmetry, this continuous rotation effectively tunes the symmetry and its associated physical properties. Furthermore, we demonstrate that built-in strain in free-standing crystals is sufficient to pin L into continuous textures over millimeter length scales. Together, these results provide guidance for future device design and open the door to leveraging the Néel vector orientation as a tunable degree of freedom in spintronic applications.

cond-mat.mtrl-sci

Deterministic domain selection of antiferromagnets via magnetic fields

Antiferromagnets (AFMs) hold promise for applications in digital logic. However, switching AFM domains is challenging, as magnetic fields do not couple to the bulk antiferromagnetic order parameter. Here we show that magnetic-field-driven switching of AFM domains can in many cases be enabled by a generic reduction of magnetic exchange at surfaces. We use statistical mechanics and Monte Carlo simulations to demonstrate that an inequivalence in magnetic exchange between top and bottom surface moments, combined with the enhanced magnetic susceptibility of surface spins, can enable deterministic selection of antiferromagnetic domains depending on the magnetic-field ramping direction. We further show that this mechanism provides a natural interpretation for experimental observations of hysteresis in magneto-optical response of the van der Waals AFM $\mathrm{MnBi_2Te_4}$. Our findings highlight the critical role of surface spins in responses of antiferromagnets to magnetic fields. Furthermore, our results suggest that antiferromagnetic domain selection via purely magnetic means may be a more common and experimentally accessible phenomenon than previously assumed.

cond-mat.mtrl-sci

Anisotropic Multi-Q Order in CoxTaS2

The cobalt-intercalated transition metal dichalcogenide Co$_x$TaS$_2$ hosts a rich landscape of magnetic phases that depend sensitively on $x$. While the stoichiometric compound with $x=1/3$ exhibits a single magnetic transition, samples with $x\leq 0.325$ display two transitions with an anomalous Hall effect (AHE) emerging in the lower temperature phase. Here, we resolve the spin structure in each phase by employing a suite of magneto-optical probes that include the discovery of anomalous magneto-birefringence -- a spontaneous time-reversal sensitive rotation of the principal optic axes. A symmetry-based analysis identifies the AHE-active phase as an anisotropic (2+1)\textbf{Q} state, in which magnetic modulation at one wavevector (\textbf{Q}) differs in symmetry from that at the remaining two. The (2+1)\textbf{Q} state naturally exhibits scalar spin chirality as a mechanism for the AHE and expands the classification of multi-Q magnetic phases.

cond-mat.str-el

Unconventional superlattice ordering in intercalated transition metal dichalcogenide V$_{1/3}$NbS$_2$

The interplay between symmetry and topology in magnetic materials makes it possible to engineer exotic phases and technologically useful properties. A key requirement for these pursuits is achieving control over local crystallographic and magnetic structure, usually through sample morphology (such as synthesis of bulk crystals versus thin-films) and application of magnetic or electric fields. Here we show that V$_{1/3}$NbS$_2$ can be crystallized in two ordered superlattices, distinguished by the periodicity of out-of-plane magnetic intercalants. Whereas one of these structures is metallic and displays the hallmarks of altermagnetism, the other superlattice, which has not been isolated before in this family of intercalation compounds, is a semimetallic noncollinear antiferromagnet that may enable access to topologically nontrivial properties. This observation of an unconventional superlattice structure establishes a powerful route for tailoring the tremendous array of magnetic and electronic behaviors hosted in related materials.

cond-mat.mtrl-sci

Goldstone mode of the broken helix in U(1) magnet EuIn2As2

Goldstone modes acquire a frequency gap in the presence of perturbations that break the underlying continuous symmetry. Here, we study the response of a spin-based Goldstone mode to strain and magnetic field in the broken helix, a multi-$\textbf{Q}$ phase of EuIn$_2$As$_2$. Optical polarimetry with spatial and temporal resolution allows us to access information about both the structure and frequency of optically excited spin-wave modes under different strain conditions. We observe nearly uniform spin precession characteristic of a Goldstone mode only when magnetic field dominates over strain. In this regime, the frequency depends linearly on the applied field. A symmetry analysis for predicting the mode frequency near zero field demonstrates that the observed scaling is of the lowest allowed order. This work thus demonstrates the connections between magnetic symmetries and the frequency dependence of the Goldstone mode in an external field, and illustrates the power of our technique for studying the dynamics of complex magnets.

cond-mat.mtrl-sci

Orbital-spin Locking and its Optical Signatures in Altermagnets

Altermagnets, magnetic materials with zero magnetization and spin-split band structure, have gained tremendous attention recently for their rich physics and potential applications. Here, we report on a microscopic tight-binding model that unveils a unique coupling between orbitals and spins in $d$-wave altermagnets which gives rise to momentum-dependent and spin-selective optical absorption. This coupling promotes the controlled optical excitation of up or down spins depending on the polarization direction of linearly polarized light. Such an effect originates from the coupling of orbitals to the sublattice degree of freedom through the crystal field, which is then coupled to spins through the antiferromagnetic interaction. Our crystal field analysis, which is general to any type of altermagnet, helps understand the onset of altermagnetism from a microscopic point of view, and we use our results to propose clear magneto-optical signatures of our predictions. Our findings shine light on the interplay between orbitals and spins in altermagnets, thus paving the way towards novel orbitronic and opto-spintronic devices.

cond-mat.mtrl-sci

Linear magneto-conductivity as a DC probe of time-reversal symmetry breaking

Several optical experiments have shown that in magnetic materials the principal axes of response tensors can rotate in a magnetic field. Here we offer a microscopic explanation of this effect, and propose a closely related DC transport phenomenon -- an off-diagonal \emph{symmetric} conductivity linear in a magnetic field, which we refer to as linear magneto-conductivity (LMC). Although LMC has the same functional dependence on magnetic field as the Hall effect, its origin is fundamentally different: LMC requires time-reversal symmetry to be broken even before a magnetic field is applied, and is therefore a sensitive probe of magnetism. We demonstrate LMC in three different ways: via a tight-binding toy model, density functional theory calculations on MnPSe$_3$, and a semiclassical calculation. The third approach additionally identifies two distinct mechanisms yielding LMC: momentum-dependent band magnetization and Berry curvature. Finally, we propose an experimental geometry suitable for detecting LMC, and demonstrate its applicability using Landauer-Büttiker simulations. Our results emphasize the importance of measuring the full conductivity tensor in magnetic materials, and introduce LMC as a new transport probe of symmetry.

cond-mat.mes-hall

Elastocaloric signatures of symmetric and antisymmetric strain-tuning of quadrupolar and magnetic phases in DyB2C2

The adiabatic elastocaloric effect measures the temperature change of given systems with strain and probes the entropic landscape in the temperature-strain space. In this study we demonstrate that the DC bias strain-dependence of AC elastocaloric effect can be used to decompose the latter into contributions from symmetric (rotation-symmetry-preserving) and antisymmetric (rotation-symmetry-breaking) strains, using a tetragonal f-electron system DyB2C2--whose antiferroquadrupolar order locally breaks four-fold rotational site symmetries while globally remaining tetragonal--as a showcase example. We capture the strain evolution of the quadrupolar and magnetic phase transitions in the system using both singularities in the elastocaloric coefficient and its jump at the transitions, and the latter we show follows a modified Ehrenfest relation. We find that antisymmetric strain couples to the underlying order parameter in a bi-quadratic manner in the antiferroquadrupolar (AFQ) phase but in a linear-quadratic manner in the canted antiferromagnetic (CAFM) phase; the contrast is attributed to a preserved (broken) tetragonal symmetry in the AFQ (CAFM) phase, respectively. The broken tetragonal symmetry in the CAFM phase is further supported by elastocaloric strain-hysteresis and observation of two sets of domains with mutually perpendicular principal axes in optical birefringence. Additionally, when the quadrupolar moments are ordered in a staggered fashion, we uncover an elastocaloric response that reflects a quadratic increase of entropy with antisymmetric strain, analogous to the role magnetic field plays for Ising antiferromagnets by promoting pseudospin flips. Our results show that AC elastocaloric effect is a compact and incisive thermodynamic probe into the coupling between electronic degrees of freedom and strain, which can potentially be applied to broader classes of quantum materials.

cond-mat.str-el

Spin-carrier coupling induced ferromagnetism and giant resistivity peak in EuCd$_2$P$_2$

EuCd$_2$P$_2$ is notable for its unconventional transport: upon cooling the metallic resistivity changes slope and begins to increase, ultimately 100-fold, before returning to its metallic value. Surprisingly, this giant peak occurs at 18K, well above the Néel temperature ($T_N$) of 11.5K. Using a suite of sensitive probes of magnetism, including resonant x-ray scattering and magneto-optical polarimetry, we have discovered that ferromagnetic order onsets above $T_N$ in the temperature range of the resistivity peak. The observation of inverted hysteresis in this regime shows that ferromagnetism is promoted by coupling of localized spins and itinerant carriers. The resulting carrier localization is confirmed by optical conductivity measurements.

cond-mat.str-el

Tuneable electron-magnon coupling of ferromagnetic surface states in PdCoO$_2$

Controlling spin wave excitations in magnetic materials underpins the burgeoning field of magnonics. Yet, little is known about how magnons interact with the conduction electrons of itinerant magnets, or how this interplay can be controlled. Via a surface-sensitive spectroscopic approach, we demonstrate a strong and highly-tuneable electron-magnon coupling at the Pd-terminated surface of the delafossite oxide PdCoO$_2$, where a polar surface charge mediates a Stoner transition to itinerant surface ferromagnetism. We show how the coupling can be enhanced 7-fold with increasing surface disorder, and concomitant charge carrier doping, becoming sufficiently strong to drive the system into a polaronic regime, accompanied by a significant quasiparticle mass enhancement. Our study thus sheds new light on electron-magnon interactions in solid-state materials, and the ways in which these can be controlled.

cond-mat.str-el

$h/e$ Oscillations in Interlayer Transport of Delafossites

Transport of electrons in a bulk metal is usually well captured by their particle-like aspects, while their wave-like nature is commonly harder to observe. Microstructures can be are fully designed to reveal the quantum phase, for example mesoscopic metal rings resembling interferometers. Here we report a new type of phase coherent oscillation of the out-of-plane magnetoresistance in the layered delafossites PdCoO$_2$ and PtCoO$_2$. The oscillation period is equivalent to that determined by the magnetic flux quantum, $h/e$, threading an area defined by the atomic interlayer separation and the sample width. The phase of the electron wave function in these crystals appears remarkably robust over macroscopic length scales exceeding 10$μ$m and persisting up to elevated temperatures of $T$>50K. We show that, while the experimental signal cannot be explained in a standard Aharonov-Bohm analysis, it arises due to periodic field-modulation of the out-of-plane hopping. These results demonstrate extraordinary single-particle quantum coherence lengths in the delafossites, and identify a new form of quantum interference in solids.

cond-mat.mtrl-sci

Hidden kagome-lattice picture and origin of high conductivity in delafossite PtCoO$_2$

We study the electronic structure of delafossite PtCoO$_2$ to elucidate its extremely small resistivity and high mobility. The band exhibits steep dispersion near the Fermi level despite the fact that it is formed mainly by Pt $d$ orbitals that are typically localized. We propose a picture based on two hidden kagome-lattice-like electronic structure: one originating from Pt $s+p_x/p_y$ orbitals, and the other from Pt $d_{3z^2-r^2}+d_{xy}/d_{x^2-y^2}$ orbitals, each placed on the bonds of the triangular lattice. In particular, we find that the underlying Pt $s+p_x/p_y$ bands actually determine the steepness of the original dispersion, so that the large Fermi velocity can be attributed to the large width of the Pt $s+p_x/p_y$ band. More importantly, the kagome-like electronic structure gives rise to "orbital-momentum locking" on the Fermi surface, which reduces the electron scattering by impurities. We conclude that the combination of the large Fermi velocity and the orbital-momentum locking is likely to be the origin of the extremely small resistivity in PtCoO$_2$.

cond-mat.mtrl-sci

Orbital- and $k_z$-selective hybridisation of Se 4p and Ti 3d states in the charge density wave phase of TiSe$_2$

We revisit the enduring problem of the $2\times{}2\times{}2$ charge density wave (CDW) order in TiSe$_2$, utilising photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridisation that is strongly $k_z$-dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe$_2$.

cond-mat.str-el

Spin Hall effect in 2D metallic delafossite PtCoO$_2$ and vicinity topology

The two-dimensional (2D) metal PtCoO$_2$ is renowned for the lowest room temperature resistivity among all oxides, close to that of the top two materials Ag and Cu. In addition, we theoretically predict a strong intrinsic spin Hall effect. This originates from six strongly-tilted Dirac cones that we find in the electronic structure near the Fermi surface, where a gap is opened by large spin-orbit coupling (SOC). This is underpinned by rich topological properties; in particular, the phenomenology of a mirror Chern metal is realized not exactly, but very accurately, on account of an approximate crystalline symmetry. We expect that such 'vicinity topology' to be a feature of relevance well beyond this material. Our Wilson loop analysis indicates further elaborate features such as fragile topology. These findings highlight PtCoO$_2$ as a promising material for spintronic applications as well as a platform to study the interplay of symmetry and topology.

cond-mat.mes-hall

Unconventional magneto-transport in ultrapure PdCoO2 and PtCoO2

We have studied magneto transport in the single-band, quasi-two-dimensional metals PdCoO2 and PtCoO2, which have extremely long mean free paths. We observer a strong temperature dependence of the Hall resistivity in small applied, fields, linked to a large violation of Kohler's rule in the magnetoresistance. We discuss the extent to which these observations can be accounted for by standard transport theory, and describe other possible, unconventional contributions to magnetotransport in very high purity metals.

cond-mat.mes-hall

Maximal Rashba-like spin splitting via kinetic energy-driven inversion symmetry breaking

Engineering and enhancing inversion symmetry breaking in solids is a major goal in condensed matter physics and materials science, as a route to advancing new physics and applications ranging from improved ferroelectrics for memory devices to materials hosting Majorana zero modes for quantum computing. Here, we uncover a new mechanism for realising a much larger energy scale of inversion symmetry breaking at surfaces and interfaces than is typically achieved. The key ingredient is a pronounced asymmetry of surface hopping energies, i.e. a kinetic energy-driven inversion symmetry breaking, whose energy scale is pinned at a significant fraction of the bandwidth. We show, from spin- and angle-resolved photoemission, how this enables surface states of 3d and 4d-based transition-metal oxides to surprisingly develop some of the largest Rashba-like spin splittings that are known. Our findings open new possibilities to produce spin textured states in oxides which exploit the full potential of the bare atomic spin-orbit coupling, raising exciting prospects for oxide spintronics. More generally, the core structural building blocks which enable this are common to numerous materials, providing the prospect of enhanced inversion symmetry breaking at judiciously-chosen surfaces of a plethora of compounds, and suggesting routes to interfacial control of inversion symmetry breaking in designer heterostructures.

cond-mat.str-el

Quasi two-dimensional Fermi surface topography of the delafossite PdRhO$_2$

We report on a combined study of the de Haas-van Alphen effect and angle resolved photoemission spectroscopy on single crystals of the metallic delafossite PdRhO$_2$ rounded off by \textit{ab initio} band structure calculations. A high sensitivity torque magnetometry setup with SQUID readout and synchrotron-based photoemission with a light spot size of $~50\,μ\mathrm{m}$ enabled high resolution data to be obtained from samples as small as $150\times100\times20\,(μ\mathrm{m})^3$. The Fermi surface shape is nearly cylindrical with a rounded hexagonal cross section enclosing a Luttinger volume of 1.00(1) electrons per formula unit.

cond-mat.mtrl-sci

Nearly-free electrons in a 5d delafossite oxide metal

Understanding the role of electron correlations in strong spin-orbit transition-metal oxides is key to the realisation of numerous exotic phases including spin-orbit assisted Mott insulators, correlated topological solids, and prospective new high-temperature superconductors. To date, most attention has been focussed on the $5d$ iridium-based oxides. Here, we instead consider the Pt-based delafossite oxide PtCoO$_2$. Our transport measurements, performed on single-crystal samples etched to well-defined geometries using focussed ion-beam techniques, yield a room-temperature resistivity of only 2.1~$μΩ$cm, establishing PtCoO$_2$ as the most conductive oxide known. From angle-resolved photoemission and density-functional theory, we show that the underlying Fermi surface is a single cylinder of nearly hexagonal cross-section, with very weak dispersion along k$_z$. Despite being predominantly composed of $d$-orbital character, the conduction band is remarkably steep, with an average effective mass of only 1.14$m_e$. Moreover, the sharp spectral features observed in photoemission remain well-defined with little additional broadening for over 500~meV below E$_F$, pointing to suppressed electron-electron scattering. Together, our findings establish PtCoO$_2$ as a model nearly-free electron system in a $5d$ delafossite transition-metal oxide.

cond-mat.str-el