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Dharmalingam Prabhakaran

Publications and source records attributed to Dharmalingam Prabhakaran.

At least 19 recordsLinked to original sources

Resolving the Magnetic Ground State and Field-Induced Transitions in Magnetic Dirac Semimetal Candidate EuMnSb$_2$

The magnetic structure of a magnetic topological semimetal EuMnSb$_2$ is investigated in fields up to 30 T using polarized and unpolarized neutron diffraction, pulsed-field x-ray magnetic circular dichroism and pulsed-field magnetometry. We determine the zero-field magnetic structures of the Eu and Mn sublattices, and find that magnetic transitions induced by applied fields below 2 T correspond to changes in the magnetic order of the Eu spins alone without detectable perturbation to the order of the Mn spins. An additional magnetic transition is observed at fields close to the saturation field for the Eu spins. We present a mean-field model which describes key features of the magnetic behavior and allows us to estimate the dominant Eu--Eu and Eu--Mn exchange interactions responsible for the coupling between magnetism and electronic topology.

cond-mat.str-el

Antiferroquadrupolar Order in Altermagnetic CoF$_2$

Altermagnets host non-relativistic spin-split electronic states whose microscopic origin is theoretically linked to a hidden charge order, yet experimental studies of this charge order are limited. We therefore investigate charge order within CoF$_2$, a $d$-wave altermagnetic compound with a rutile crystal structure and $\Gamma$-point antiferromagnetism. Combining resonant elastic X-ray scattering, symmetry analysis and ab initio calculations, we directly observe charge ordering and identify it as antiferroquadrupolar in nature. Via electronic structure calculations, we show that the experimentally observed antiferroquadrupolar order gives rise to the characteristic altermagnetic spin-splitting, thereby establishing empirical evidence for the decomposition of the altermagnetic order parameter into magnetic and charge degrees of freedom. We hence demonstrate that antiferroquadrupolar order is the microscopic origin of altermagnetism in CoF$_2$, with implications to the wider family of rutile altermagnets. Furthermore, our approach is applicable to studying altermagnetism in general, having demonstrated that resonant elastic X-ray scattering can serve as a direct probe of the charge multipoles that underpin spin-split electronic states in these materials.

cond-mat.str-el

Higher-order Weyl nodes driven by helical magnetic order in EuAgAs

Magnetic topological semimetals provide a fertile ground for exploring how long-range magnetic order can alter electronic band structures and generate novel quasiparticles such as Weyl fermions. Here, we investigate the coupled magnetic and electronic structure of single-crystalline EuAgAs, a hexagonal pnictide whose magnetic ground state has remained elusive. Using neutron diffraction and resonant elastic X-ray scattering, we identify an unusual magnetic ordering sequence with two successive phase transitions at $T_\mathrm{N1} = 12$ K and $T_\mathrm{N2} = 8$ K. We observe two slightly different magnetic propagation vectors, one associated with $T_\mathrm{N1}$ and the other with $T_\mathrm{N2}$. Spherical neutron polarimetry reveals that the magnetic structure is a transverse helix aligned along the $c$ axis with a period that is approximately twice the $c$ lattice parameter. First-principles calculations for the helical phase predict subtle band folding effects and the emergence of effective higher-order Weyl nodes. These topological features appear near the calculated Fermi energy $E_{\mathrm{F}}$ which, however, lies above the position of $E_{\mathrm{F}}$ obtained from angle-resolved photoemission spectroscopy so could not be probed in this study.

cond-mat.str-el

X-ray magnetic circular dichroism evidence of intrinsic $d$-wave altermagnetism in rutile-structure NiF$_2$

We present the x-ray magnetic circular dichroism (XMCD) at the Ni $L_{2,3}$-edge as an evidence of the $d$-wave altermagnetism in rutile-structure NiF$_2$. Sizable XMCD signal is observed in excellent agreement with theoretical simulations. Owing to a considerable net magnetization due to spin canting, the XMCD spectrum consists of an altermagnetic signal as well as a non-negligible ferromagnetic contribution. We verify experimentally that the XMCD spectrum can be written as a sum of contributions from altermagnetism and weak ferromagnetism. Two experimental methods to isolate the ferromagnetic contribution are shown to yield essentially the same result. These are dependence of XMCD on applied magnetic fields below the N\'eel temperature and the XMCD measured in applied field above the N\'eel temperature. Our results demonstrate the utility of XMCD as a probe for altermagnetic materials with the coexisting weak ferromagnetism induced by the relativistic spin-orbit coupling.

cond-mat.str-el

Vector spin polarization evolution determined in an entangled muon-fluorine system under pulsed excitation

A spin-polarized muon implanted into a fluoride forms a coupled F--$\mu$--F complex in which the muon spin and neighbouring fluorine nuclear spins become entangled. Here we apply radio-frequency (RF) excitation to this coupled system and use the three-dimensional distribution of emitted positrons to reconstruct the time-dependent evolution of the muon spin polarization. This three-dimensional readout, using single spin detection, is not possible in a single NMR experiment and demonstrates significant advantages that are achieved by using RF muon techniques. We demonstrate the application of this vector-readout method to the experimental observation of a muon spin echo signal that is controlled by the dipolar coupling to fluorine, as well as to a double resonance experiment, in which we use pulses tuned to separate frequencies to address both the muon and fluorine spins. This targeted approach, in which selective RF pulses can control the muon spin and other spins to which it is coupled, provides a novel route for probing systems of entangled spins.

cond-mat.str-el

Fermi surface and effective masses of IrO$_2$ probed by de Haas-van Alphen quantum oscillations

Iridium-containing conducting materials are widely investigated for their strong spin-orbit coupling and potential topological properties. Recently the commonly used electrode material iridium dioxide was found to host a large spin-Hall conductivity and was shown to support Dirac nodal lines. Here we present quantum-oscillation experiments on high-quality IrO$_2$ single crystals using the de Haas-van Alphen effect measured using torque magnetometry with a piezo-resistive microcantilever as well as density functional theory-based band-structure calculations. The angle, temperature and field dependencies of the oscillations and the calculated band dispersion provide valuable information on the properties of the charge carriers, including the Fermi-surface geometry and electronic correlations. Comparison of experimental results to calculations allows us to assigns the observed de Haas-van Alphen frequencies to the calculated Fermi surface topology. We find that the effective masses of IrO$_2$ are enhanced compared to the rest electron mass $m_e$, ranging from 1.9 to 3.0~$m_e$, whereas the scattering times indicate excellent sample quality. We discuss our results in context with recent ARPES and band-structure calculation results that found Dirac nodal lines in IrO$_2$ and compare the effective masses and other electronic properties to those of similar materials like the nodal chain metal ReO$_2$ in which Dirac electrons with very light effective masses have been observed.

cond-mat.str-el

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

AFM-based Functional Tomography-To Mill or not to Mill, that is the Question!

The electrical response of ferroelectric domain walls is often influenced by their geometry underneath the sample surface. Tomographic imaging in these material systems has therefore become increasingly important for its ability to correlate the surface-level functional response with subsurface domain microstructure. In this context, AFM-based tomography emerges as a compelling choice because of its simplicity, high resolution and robust contrast mechanism. However, to date, the technique has been implemented in a limited number of ferroelectric materials, typically to depths of a few hundred nanometers or on relatively soft materials, resulting in an unclear understanding of its capabilities and limitations. In this work, AFM tomography is carried out in YbMnO3, mapping its complex domain microstructure up to a depth of around 1.8 um along with its current pathways. A model is presented, describing the impact of interconnected domain walls within the network, which act as current dividers and codetermine how currents distribute. Finally, challenges such as tip-blunting and subsurface amorphisation are identified through TEM studies, and strategies to address them are also put forward. This study highlights the potential of AFM tomography and could spur interest within the ferroics community for its use in the investigation of similar material systems.

cond-mat.mtrl-sci

Elastic softness of low-symmetry frustrated $A$Ti$_2$O$_5$ ($A$ = Co, Fe)

Orthorhombic pseudobrookites CoTi$_2$O$_5$ and FeTi$_2$O$_5$ have a low-symmetry crystal structure comprising magnetic Co$^{2+}$/Fe$^{2+}$ ions and nonmagnetic Ti$^{4+}$ ions, where the orbital-nondegenerate Co$^{2+}$/Fe$^{2+}$ ions form one-dimensional chains running along the orthorhombic $a$ axis. These compounds undergo an antiferromagnetic phase transition at $T_N \sim$ 26 K for CoTi$_2$O$_5$ and $T_N \sim$ 40 K for FeTi$_2$O$_5$. Ultrasound velocity measurements on single crystals of CoTi$_2$O$_5$ and FeTi$_2$O$_5$ reveal that CoTi$_2$O$_5$ exhibits unusual elastic softness above $T_N$ in the symmetry-lowering elastic mode of $ac$-plane shear elastic modulus, inconsistent with the structural symmetry breaking caused by antiferromagnetic ordering at $T_N$. This suggests the presence of two distinct types of magnetostructural fluctuations above $T_N$ that should be a precursor to the symmetry-lowering lattice distortion at $T_N$. In contrast, FeTi$_2$O$_5$ exhibits either negligible or smaller elastic softness, indicating weaker spin-lattice coupling. These findings highlight CoTi$_2$O$_5$ and FeTi$_2$O$_5$ as unique spin-latticed-coupled frustrated systems with low crystal symmetry, where, while the exchange interactions are quasi-one-dimensional in nature, the frustration is released by further lowering the crystal symmetry through three-dimensional spin-lattice coupling, which is stronger in CoTi$_2$O$_5$ than in FeTi$_2$O$_5$.

cond-mat.str-el

A resonant valence bond spin liquid in the dilute limit of doped frustrated Mott insulators

Ideas about resonant valence bond liquids and spin-charge separation have led to key concepts in physics such as quantum spin liquids, emergent gauge symmetries, topological order, and fractionalisation. Despite extensive efforts to demonstrate the existence of a resonant valence bond phase in the Hubbard model that originally motivated the concept, a definitive realisation has yet to be achieved. Here we present a solution to this long-standing problem by uncovering a resonant valence bond phase exhibiting spin-charge separation in realistic Hamiltonians. We show analytically that this ground state emerges in the dilute-doping limit of a half-filled Mott insulator on corner-sharing tetrahedral lattices with frustrated hopping, in the absence of exchange interactions. We confirm numerically that the results extend to finite exchange interactions, finite-sized systems and finite dopant density. Although much attention has been devoted to the emergence of unconventional states from geometrically frustrated interactions, our work demonstrates that kinetic energy frustration in doped Mott insulators may be essential for stabilising robust, topologically ordered states in real materials.

cond-mat.str-el

Ultrafast surface melting of orbital order in La0.5Sr1.5MnO4

Understanding how light modifies long-range order in quantum materials is key to improving our ability to control functionality. However, this is challenging if the response is heterogeneous. Here we address the most common form of light-induced heterogeneity, surface melting, and measure the dynamics of orbital order in the layered manganite, La0.5Sr1.5MnO4. We isolate the surface dynamics from the bulk by measuring the orbital truncation rod as well as orbital Bragg peak. After photoexcitation, the orbital Bragg peak shows an unusual narrowing, which suggests an increase in the correlation length in the probed volume. In contrast, the correlation length at the surface decreases. These differences can be reconciled if the material is heterogeneous, and light melts a less ordered surface. By isolating the surface response, we determine that the loss of long-range order is an incoherent process, which is likely accompanied by the formation of local polarons.

cond-mat.str-el

Characterizing the diffuse continuum excitations in the classical spin liquid $h$-YMnO$_3$

We extend previous inelastic neutron scattering results on the geometrically frustrated antiferromagnet hexagonal-YMnO$_3$, which has been suggested to belong to the class of classical spin liquids. We extend the energy transfer coverage of the diffuse signal up to 6.9 meV within a wide temperature range around the ordering temperature, $T_\mathrm{N}$. The two distinct diffuse signals in the a-b plane, the signal localized at $\Gamma$' and the scattering intensity connecting $\Gamma$' points over the M', are shown to be only weakly energy dependent. In addition, an external magnetic field of up to 10.5 T applied along c is shown to have no effect on the diffuse signal. In the orthogonal scattering plane, the signals are shown to be dependent on l only through the magnetic form factor, showing that the correlations are purely two-dimensional, and supporting its origin to be the frustrated Mn$^{3+}$ triangles. This result is corroborated by atomistic spin dynamics simulations showing similar scattering vector and temperature behaviours. Lastly, data for the spin wave scattering in the (h, 0, l) plane allow for a discussion of the magnetic ground state where better agreement is found between the data and an ordered structure of the $\Gamma_1$ or $\Gamma_3$ symmetry, albeit crystal electric field arguments dismisses the $\Gamma_1$ as possibility.

cond-mat.str-el

Switching of ferrotoroidal domains via an intermediate mixed state in the multiferroic Y-type hexaferrite Ba$_{0.5}$Sr$_{1.5}$Mg$_2$Fe$_{12}$O$_{22}$

We report a detailed study of the magnetic field switching of ferrotoroidal/multiferroic domains in the Y-type hexaferrite compound Ba$_{0.5}$Sr$_{1.5}$Mg$_2$Fe$_{12}$O$_{22}$. By combining data from SQUID magnetometry, magneto-current measurements, and resonant X-ray scattering experiments, we arrive at a complete description of the deterministic switching, which involves the formation of a temperature-dependent mixed state in low magnetic fields. This mechanism is likely to be shared by other members of the hexaferrite family, and presents a challenge for the development of high-speed read-write memory devices based on these materials.

cond-mat.str-el

Weyl metallic state induced by helical magnetic order

In the rapidly expanding field of topological materials there is growing interest in systems whose topological electronic band features can be induced or controlled by magnetism. Magnetic Weyl semimetals, which contain linear band crossings near the Fermi level, are of particular interest owing to their exotic charge and spin transport properties. Up to now, the majority of magnetic Weyl semimetals have been realized in ferro- or ferrimagnetically ordered compounds, but a disadvantage of these materials for practical use is their stray magnetic field which limits the minimum size of devices. Here we show that Weyl nodes can be induced by a helical spin configuration, in which the magnetization is fully compensated. Using a combination of neutron diffraction and resonant elastic x-ray scattering, we find that EuCuAs develops a planar helical structure below $T_\textrm{N}$ = 14.5 K which induces Weyl nodes along the $Γ$--A high symmetry line in the Brillouin zone.

cond-mat.str-el

Capturing dynamical correlations using implicit neural representations

The observation and description of collective excitations in solids is a fundamental issue when seeking to understand the physics of a many-body system. Analysis of these excitations is usually carried out by measuring the dynamical structure factor, S(Q, $ω$), with inelastic neutron or x-ray scattering techniques and comparing this against a calculated dynamical model. Here, we develop an artificial intelligence framework which combines a neural network trained to mimic simulated data from a model Hamiltonian with automatic differentiation to recover unknown parameters from experimental data. We benchmark this approach on a Linear Spin Wave Theory (LSWT) simulator and advanced inelastic neutron scattering data from the square-lattice spin-1 antiferromagnet La$_2$NiO$_4$. We find that the model predicts the unknown parameters with excellent agreement relative to analytical fitting. In doing so, we illustrate the ability to build and train a differentiable model only once, which then can be applied in real-time to multi-dimensional scattering data, without the need for human-guided peak finding and fitting algorithms. This prototypical approach promises a new technology for this field to automatically detect and refine more advanced models for ordered quantum systems.

cond-mat.str-el

Nonlocal drag by topological surface magnons in a pyrochlore ferromagnet

The nontrivial topology of quasiparticle wavefunctions can manifest themselves in the form of observable surface states. This is now well established in electronic systems, with Dirac and Weyl semimetals bringing to fore the exotic nature of these topologically protected entities. Magnons - which refer to collective excitations of localized spins - offer another sector where many of these concepts could be realized. Here, we report magneto-thermal measurements on a pyrochlore ferromagnet which is theoretically predicted to host such topological magnons. It is demonstrated that the thermoelectric potential across a metal layer deposited on single crystalline specimens of Y$_2$V$_2$O$_7$ can be used to measure the magnon Hall effect. Moreover, a direct manifestation of topologically protected magnon surface states is observed - via the interfacial drag which these surface spin currents impose on the conduction electrons of the adjacent metallic layer.

cond-mat.str-el

Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase

Spontaneous C4-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C4 symmetry is restored. A leading approach is based on time-dependent Ginzburg-Landau theory, which explains the coherence response seen in many systems. However, we show that, for the case of the single layered manganite La0.5Sr1.5MnO4, the theory fails. Instead, we find an ultrafast inhomogeneous disordering transition in which the mean-field order parameter no longer reflects the atomic-scale state of the system. Our results suggest that disorder may be common to light-induced phase transitions, and methods beyond the mean-field are necessary for understanding and manipulating photoinduced phases.

cond-mat.str-el

A model for coupled $4f-3d$ magnetic spectra: a neutron scattering study of the Yb$-$Fe hybridisation in Yb$_3$Fe$_5$O$_{12}$

In this work, we explore experimentally and theoretically the spectrum of magnetic excitations of the Fe$^{3+}$ and Yb$^{3+}$ ions in ytterbium iron garnet (Yb$_3$Fe$_5$O$_{12}$). We present a complete description of the crystal-field splitting of the $4f$ states of Yb$^{3+}$, including the effect of the exchange field generated by the magnetically ordered Fe subsystem. We also consider a further effect of the Fe-Yb exchange interaction, which is to hybridise the Yb crystal field excitations with the Fe spin-wave modes at positions in the Brillouin zone where the two types of excitations cross. We present detailed measurements of these hybridised excitations, and propose a framework which can be used in the quantitative analysis of the coupled spectra in terms of the anisotropic $4f-3d$ exchange interaction.

cond-mat.str-el