arXiv subjects

Devashibhai T. Adroja

Publications and source records attributed to Devashibhai T. Adroja.

At least 19 recordsLinked to original sources

arXiv2026

Dispersive-phonon-driven room-temperature Ni1+-Ni2+ polaron hopping in spin-charge coupled rutile niobate

Understanding how lattice dynamics mediate polaron hopping is essential for designing multifunctional correlated oxides. Here, we demonstrate room-temperature dispersive phonon excitations and elucidate the Ni1+-Ni2+ polaron-hopping mechanism and the presence of rare spin-charge-phonon coupling even in a magnetically short-range-ordered state in rutile niobate, a rare room-temperature magnetodielectric system. We reveal room-temperature dispersive phonon excitations using inelastic neutron scattering (INS), complemented by machine-learning-based phonon calculations, to establish the microscopic origin of the polaron-hopping mechanism. Experimental evidence of dispersive phonon-driven polaron hopping is scarce. INS measurements show significant dispersive phonon excitations at 21, 33, and 47 meV, implying collective lattice dynamics that enable delocalized polaron propagation via coupled charge-spin-phonon interactions. Dispersive phonons couple to charge carriers and promote correlated NiO6 lattice distortions, facilitating delocalized polaron hopping. Low-energy magnetic excitations at 4 and 8 meV indicate the presence of local short-range magnetic correlations or spin-orbit-coupling-induced anisotropy in deformed NiO6 octahedra, which are thoroughly discussed. Machine-learning phonon calculations replicate the experimentally observed phonon excitations and demonstrate lattice instability, which is compatible with dynamic local distortions caused by polaron production. These findings provide microscopic evidence for a coupled charge-spin-phonon mechanism that mediates polaron hopping in rutile oxide systems.

cond-mat.mtrl-sci↗

arXiv2026

Interplay of Spin Waves, Crystal-Field Excitations, and Phonons in Multiferroic Ba3HoRu2O9 revealed by Inelastic Neutron Scattering, Crystal-Field Analysis, and Machine-Learned Phonon Calculations

Understanding the microscopic origin of spin-dipole coupling and high-energy excitations in correlated 4d-4f multiferroic oxides is challenging because magnetic, crystal-field, and lattice excitations frequently overlap in energy. The hexagonal 6H perovskite Ba3HoRu2O9 provides an ideal platform to investigate this interplay owing to the coexistence of Ru2O9 molecular units and localized Ho3+ moments. To identify the contributions from these different excitations, we combine inelastic neutron scattering (INS) with linear spin-wave calculations, crystal-field analysis, Raman spectroscopy, and machine-learned force field (MLFF) phonon calculations. A dispersive magnetic excitation below 6.2 meV is accurately reproduced by linear spin-wave theory, establishing its origin as a collective spin-wave excitation of the coupled Ru-Ho magnetic network. At higher energies, broad excitations centered near 20, 39, 70, and 90 meV is observed that are present far above magnetic ordering temperature. Crystal-field calculations based on the Stevens formalism place the strongest Ho3+ transitions within the experimentally observed energy window, while Raman spectroscopy and MLFF phonon calculations identify optical phonons with comparable energies. Together, these complementary results show that the broad INS feature near 39 meV is consistent with overlapping contributions from Ho3+ crystal-field excitations, lattice vibrations, and previously reported Ru2O9 molecular magnetic excitations. These findings establish a microscopic framework for understanding the interplay between spin, crystal-field, and lattice degrees of freedom in this multiferroic 4d-4f compound.

cond-mat.str-el↗

arXiv2026

Quasiparticle Dynamics in the 4d-4f Ising-like Double Perovskite Ba2DyRuO6 studied using Neutron Scattering and Machine-Learning Framework

Double perovskites containing 4d--4f interactions provide a platform to study complex magnetic phenomena in correlated systems. Here, we investigate the magnetic ground state and quasiparticle excitations of the fascinating double perovskite system, Ba$_2$DyRuO$_6$, through Time of flight (TOF) neutron diffraction (TOF), inelastic neutron scattering (INS), and theoretical modelling. The compound Ba$_2$DyRuO$_6$ is reported to exhibit a single magnetic transition, in sharp contrast to most of the other rare-earth (R) members in this family, A$_2$RRuO$_6$ (A = Ca/Sr/Ba), which typically show magnetic ordering of the Ru ions, followed by R-ion ordering. Our neutron diffraction results confirm that long-range antiferromagnetic order emerges at $T_\mathrm{N} \approx 47$~K, primarily driven by 4d--4f Ru$^{5+}$--Dy$^{3+}$ exchange interactions, where both Dy and Ru moments start to order simultaneously. The ordered ground state is a collinear antiferromagnet with Ising character, carrying ordered moments of $μ_{\mathrm{Ru}} = 1.6(1)~μ_\mathrm{B}$ and $μ_{\mathrm{Dy}} = 5.1(1)~μ_\mathrm{B}$ at 1.5~K. Low-temperature INS reveals well-defined magnon excitations below 10~meV. SpinW modelling of the INS spectra evidences complex exchange interactions and the presence of magnetic anisotropy, which governs the Ising ground state and accounts for the observed magnon spectrum. Combined INS and Raman spectroscopy reveal crystal-electric-field (CEF) excitations of Dy$^{3+}$ at 46.5 and 71.8~meV in the paramagnetic region. The observed CEF levels are reproduced by point-charge calculations consistent with the $O_h$ symmetry of Dy$^{3+}$. A complementary machine-learning approach is used to analyse the phonon spectrum and compare with INS data. Together, these results clarify the origin of phonon and magnon excitations and their role in the ground-state magnetism of Ba$_2$DyRuO$_6$.

cond-mat.str-el↗

arXiv2026

Non-collinear ferromagnetism in the Kondo lattice Ce$_5$CoGe$_2$

The dense Kondo lattice Ce$_5$CoGe$_2$ exhibits superconductivity once the magnetic ordering is suppressed by pressure. Here the ambient pressure magnetic state is investigated via magnetization, heat capacity, powder neutron diffraction, and muon spin relaxation ($μ$SR) measurements. Neutron diffraction results reveal a noncollinear ferromagnetic structure, where the four inequivalent Ce sites exhibit different magnetic moments. Point-charge model calculations of the crystalline-electric field (CEF) ground states corroborate different moments between the sites, and suggest sizeable components of the moments along different directions, consistent with the non-collinear structure. Analysis of the Dzyaloshinskii-Moriya (DM) interaction for the bonds connecting Ce atoms demonstrates that most of these bonds exhibit a nonzero DM vector, suggesting that competition between intersite magnetic exchange interactions, CEF driven single-ion anisotropy, the Kondo effect and the DM interaction may drive the non-collinear ferromagnetism.

cond-mat.str-el↗

arXiv2026

Coherent magnetic excitations in a topological Kondo semimetal

In Kondo insulators the many-body Kondo lattice effect drives the formation of bands containing heavy charge carriers with a hybridization gap, leading to insulating properties. These renormalized bands can host non-trivial topologies driven by strong electron-electron interactions, but probing narrow heavy bands at low temperatures is challenging. We use inelastic neutron scattering (INS) to probe the Kondo lattice CeNiSn, which hosts both semimetallic transport properties and a hybridization gap. The INS response exhibits momentum-dependent magnetic excitations and a spin-gap in the low-temperature Kondo coherent state, which electronic structure calculations corroborate as arising from the renormalized heavy band structure. Dynamical-mean field theory demonstrates that this renormalized band structure corresponds to a topological Kondo insulating state, and hence the INS probes bulk excitations of heavy topological bands. This identification of a Kondo insulator addresses the long-standing mystery of the electronic properties of CeNiSn, and demonstrates the manifestation of a topological many-body coherent state in spectroscopic measurements of strongly correlated narrow band materials.

cond-mat.str-el↗

arXiv2025

Emergent ferromagnetic ladder excitations in heavy fermion superconductor CeSb$_{2}$

Low-dimensional spin fluctuations play a crucial role in unconventional superconductors, with quasi-one-dimensional spin excitations potentially linked with spin-triplet superconductivity. The heavy fermion superconductor CeSb$_2$ exhibits an unusual large inverted S-shaped upper critical field that suggests a possible triplet pairing state within its pressure-induced superconducting dome. Using inelastic neutron scattering, we discover quasi-one-dimensional magnetic excitations in CeSb$_2$ emerging from nearly square Ce layers with minor orthorhombic deformation. We show that the data are well described by a ferromagnetic spin ladder model, where the "rungs" of the ladder straddle Ce bilayers. Moreover, we find that diffuse excitations akin to those in the ordered phase persist well above $T_{\rm N}$, suggesting that quasi-one-dimensional ferromagnetic paramagnons may significantly contribute to the unusual superconductivity that appears under pressure once magnetic order is suppressed.

cond-mat.supr-con↗

arXiv2023

Large Energy Shifts of Crystal-field Excitations in Erbium Orthoferrite Driven by Internal Magnetic Fields

Due to the complex interactions between rare-earth elements and transition metals, as well as between themselves, rare-earth transition-metal oxides are likely to exhibit highly intriguing and novel magnetic structures and dynamic behaviours. Rare-earth elements in these compounds frequently demonstrate unusual behaviours in their crystal-field (CF) excitations, which necessitate thorough studies for in-depth comprehensions. When cooling from 10 K to 1.5 K through the magnetic ordering temperature of $Er^{3+}$ at 4.1 K, we observed a significant energy shift of the low-lying CF excitation of $Er^{3+}$ in erbium orthoferrite ($ErFeO_3$) from 0.32 meV to 0.75 meV utilizing the inelastic neutron-scattering technique. A sound CF model was proposed for $Er^{3+}$ in $ErFeO_3$ by fitting to the observed CF excitation peaks, which enables to explain all the observed experimental results in a very consistent manner. According to the model, the ground crystal field level of $Er^{3+}$, which corresponds to the lowest Kramers doublet supposed to be at zero energy transfer, has been shifted by the internal magnetic fields induced by both $Er^{3+}$ and $Fe^{3+}$ spin orders below and above the $Er^{3+}$ ordering temperature, respectively. Additional measurements in various magnetic fields offer compelling evidence in favour of this hypothesis. The measured external field dependence of the CF excitation energy led to a derivation of the internal field of $Er^{3+}$ as 0.54 T, which is strongly corroborated by theoretical modelling. Additionally, the g-factor for the $Er^{3+}$ ground state in $ErFeO_3$ shows an exceptionally significant anisotropy.

cond-mat.str-el↗

arXiv2023

Spin Fluctuations in Sr$_{1.8}$La$_{0.2}$RuO$_4$

We use inelastic neutron scattering to study spin fluctuations in Sr$_{1.8}$La$_{0.2}$RuO$_4$, where Lanthanum doping triggers a Lifshitz transition by pushing the van Hove singularity in the $γ$ band to the Fermi energy. Strong spin fluctuations emerge at an incommensurate wave vector $\mathbf{Q}_{ic} = (0.3,0.3)$, corresponding to the nesting vector between $α$ and $β$ Fermi sheets. The incommensurate antiferromagnetic fluctuations shift toward $(0.25,0.25)$ with increasing energy up to ${\sim}110$ meV. By contrast, scatterings near the ferromagnetic wave vectors $\mathbf{Q} = (1,0)$ and $(1,1)$ remain featureless at all energies. This contradicts the weak-coupling perspective that suggests a sharp enhancement of ferromagnetic susceptibility due to the divergence of density of states in the associated $γ$ band. Our findings imply that ferromagnetic fluctuations in Sr$_2$RuO$_4$ and related materials do not fit into the weak-coupling paradigm, but instead are quasi-local fluctuations induced by Hund's coupling. This imposes significant constraints for the pairing mechanism involving spin fluctuations.

cond-mat.str-el↗

arXiv2023

Diffusive Excitonic Bands from Frustrated Triangular Sublattice in a Singlet-Ground-State System

Magnetic order in most materials occurs when magnetic ions with finite moments in a crystalline lattice arrange in a particular pattern below the ordering temperature determined by exchange interactions between the ions. However, when the crystal electric field (CEF) effect results in a spin-singlet ground state on individual magnetic sites, the collective ground state of the system can either remain non-magnetic, or more intriguingly, the exchange interactions between neighboring ions, provided they are sufficiently strong, can admix the excited CEF levels, resulting in a magnetically ordered ground state. The collective magnetic excitations in such a state are so-called spin excitons that describe the CEF transitions propagating through the lattice. In most cases, spin excitons originating from CEF levels of a localized single ion are dispersion-less in momentum (reciprocal) space and well-defined in both the magnetically ordered and paramagnetic states. Here we use thermodynamic and neutron scattering experiments to study stoichiometric Ni2Mo3O8 without site disorder, where Ni2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has long-range magnetic order. Furthermore, CEF spin excitons from the triangular-lattice arrangement of tetrahedral sites form, in both the antiferromagnetic and paramagnetic states, a dispersive diffusive pattern around the Brillouin zone boundary in reciprocal space. The present work thus demonstrates that spin excitons in an ideal triangular lattice magnet can have dispersive excitations, irrespective of the existence of static magnetic order, and this phenomenon is most likely due to spin entanglement and geometric frustrations.

cond-mat.str-el↗

arXiv2023

Inelastic neutron scattering study of crystalline electric field excitations in the caged compounds NdT2Zn20 (T = Co, Rh, and Ir)

We have measured crystalline electric field (CEF) excitations of Nd3+ ions in the two-channel Kondo lattice candidates NdT2Zn20 (T = Co, Rh, and Ir) by means of inelastic neutron scattering (INS). In the INS measurements at 5 K, dispersionless excitations were observed at 3.8 and 7.2 meV for T = Co, 3.1 and 5.8 meV for T = Rh, and 3.0 and 5.3 meV for T = Ir. Analyses of the temperature dependence of the INS spectra confirm that the CEF ground states are the Gamma 6 doublet, that is a requisite for manifestation of the magnetic two-channel Kondo effect. For T = Co, a shoulder was observed at 7.7 meV close to the CEF excitation peak centered at 7.2 meV. The shoulder is attributed to a bound state of the CEF and low-lying optical phonon excitations.

cond-mat.str-el↗

arXiv2023

Occupational Disorder as the Origin of Flattening of the Acoustic Phonon Branches in the Clathrate Ba$_{8}$Ga$_{16}$Ge$_{30}$

In the search for high-performance thermoelectrics, materials such as clathrates have drawn attention due to having both glass-like low phonon thermal conductivity and crystal-like high electrical conductivity. Ba$_{8}$Ga$_{16}$Ge$_{30}$ (BGG) has a loosely bound guest Ba atom trapped inside rigid Ga/Ge cage structures. Avoided crossings between acoustic phonons and the flat guest atom branches have been proposed to be the source of the low lattice thermal conductivity of BGG. Ga/Ge site disorder with Ga and Ge exchanging places in different unit cells has also been reported. We used time-of-flight neutron scattering to measure the complete phonon spectrum in a large single crystal of BGG and compared these results with predictions of density functional theory to elucidate the effect of the disorder on heat-carrying phonons. Experimental results agreed much better with the calculation assuming the disorder than with the calculation assuming the ordered configuration. Although atomic masses of Ga and Ge are nearly identical, we found that disorder strongly reduces phonon group velocities, which significantly reduces thermal conductivity. Our work points at a new path towards optimizing thermoelectrics.

cond-mat.mtrl-sci↗

arXiv2022

Investigation of metamagnetism and crystal-field splitting in pseudo-hexagonal CeRh$_3$Si$_2$

CeRh$_3$Si$_2$ has been reported to exhibit metamagnetic transitions below 5~K, a giant crystal field splitting, and anisotropic magnetic properties from single crystal magnetization and heat capacity measurements. Here we report results of neutron and x-ray scattering studies of the magnetic structure and crystal-field excitations to further understand the magnetism of this compound. Inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) reveal a $J_z$\,=\,1/2 groundstate for Ce when considering the crystallographic $a$ direction as quantization axis, thus explaining the anisotropy of the static susceptibility. Furthermore, we find a total splitting of 78\,meV for the $J$\,=\,5/2 multiplet. The neutron diffraction study in zero field reveals that on cooling from the paramagnetic state, the system first orders at $T_{\text{N}_1}=4.7$\,K in a longitudinal spin density wave with ordered Ce moments along the $b$-axis (i.e. the [0 1 0] crystal direction) and an incommensurate propagation vector $\textbf{k}=(0,0.43,0$). Below the lower-temperature transition $T_{\text{N}_2}=4.48$\,K, the propagation vector locks to the commensurate value $\textbf{k}=(0,0.5,0)$, with a so-called lock-in transition. Our neutron diffraction study in applied magnetic field $H\parallel b$-axis shows a change in the commensurate propagation vector and development of a ferromagnetic component at $H=3$\,kOe, followed by a series of transitions before the fully field-induced ferromagnetic phase is reached at $H = 7$\,kOe. This explains the nature of the steps previously reported in field-dependent magnetization measurements. A very similar behaviour is also observed for the $H\parallel$ [0 1 1] crystal direction.

cond-mat.str-el↗

arXiv2022

A ferrotoroidic candidate with well-separated spin chains

The search of novel quasi one-dimensional (1D) materials is one of the important aspects in the field of material science. Toroidal moment, the order parameter of ferrotoroidic order, can be generated by a head-to-tail configuration of magnetic moment. It has been theoretically proposed that one-dimensional (1D) dimerized and antiferromagnetic-like spin chain hosts ferrotoroidicity and has the toroidal moment composed of only two antiparallel spins. Here, we report a ferrotoroidic candidate of Ba6Cr2S10 with such a theoretical model of spin chain. The structure consists of unique dimerized face-sharing CrS6 octahedral chains along the c axis. An antiferromagnetic-like ordering at ~10 K breaks both space- and time-reversal symmetries and the magnetic point group of mm'2' allows three ferroic orders in Ba6Cr2S10: (anti)ferromagnetic, ferroelectric and ferrotoroidic orders. Our investigation reveals that Ba6Cr2S10 is a rare ferrotoroidic candidate with quasi 1D spin chain, which can be considered as a starting point for the further exploration of the physics and applications of ferrotoroidicity.

cond-mat.str-el↗

arXiv2021

Neutron Scattering Studies of the Breathing Pyrochlore Antiferromagnet LiGaCr$_{4}$O$_{8}$

We report neutron scattering measurements of the spinel oxide LiGaCr$_{4}$O$_{8}$, in which magnetic ions Cr$^{3+}$ form a breathing pyrochlore lattice. Our experiments reveal the coexistence of a nearly dispersionless resonance mode and dispersive spin wave excitations in the magnetically ordered state, which can be quantitatively described by a quantum spin model of hexagonal loops and linear spin wave theory with the same set of exchange parameters, respectively. Comparison to other Cr spinel oxides reveals a linear relationship between the resonance energy and lattice constant across all these materials, which is in agreement with our hexagonal loop calculations. Our results suggest a unified picture for spin resonances in Cr spinel oxides.

cond-mat.str-el↗

arXiv2019

Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore

A quantum spin liquid (QSL) is a state of matter where unpaired electrons' spins in a solid are quantum entangled, but do not show magnetic order in the zero-temperature limit. Because such a state may be important to the microscopic origin of high-transition temperature superconductivity and useful for quantum computation, the experimental realization of QSL is a long-sought goal in condensed matter physics. Although neutron scattering experiments on the two-dimensional (2D) spin-1/2 kagome-lattice ZnCu3(OD)6Cl2 and effective spin-1/2 triangular lattice YbMgGaO4 have found evidence for a continuum of magnetic excitations, the hallmark of a QSL carrying 'fractionalized quantum excitations', at very low temperature, magnetic and nonmagnetic site chemical disorder complicates the interpretation of the data. Recently, the three-dimensional (3D) Ce3+ pyrochlore lattice Ce2Sn2O7 has been suggested as a clean, effective spin-1/2 QSL candidate, but there is no evidence of a spin excitation continuum. Here we use thermodynamic, muon spin relaxation (μ SR), and neutron scattering experiments on single crystals of Ce2Zr2O7, a compound isostructural to Ce2Sn2O7, to demonstrate the absence of magnetic ordering and the presence of a spin excitation continuum at 35 mK, consistent with the expectation of a QSL. Since our neutron diffraction and diffuse scattering measurements on Ce2Zr2O7 reveal no evidence of oxygen deficiency and magnetic/nonmagnetic ion disorder as seen in other pyrochlores, Ce2Zr2O7 may be the first example of a 3D QSL material with minimum magnetic and nonmagnetic chemical disorder.

cond-mat.str-el↗

arXiv2019

Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO$_2$

We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70\,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.

cond-mat.str-el↗

arXiv2018

Evidence of nodal gap structure in the basal plane of the FeSe superconductor

Identifying the symmetry of the wave function describing the Cooper pairs is pivotal in understanding the origin of high-temperature superconductivity in iron-based superconductors. Despite nearly a decade of intense investigation, the answer to this question remains elusive. Here we use the muon spin rotation/relaxation (muSR) technique to investigate the underlying symmetry of the pairing state of the FeSe superconductor, the basic building block of all iron-chalcogenide superconductors. Contrary to earlier muSR studies on powders and crystals, we show that while the superconducting gap is most probably anisotropic but nodeless along the crystallographic c-axis, it is nodal in the ab-plane, as indicated by the linear increase of the superfluid density at low temperature. We further show that the superconducting properties of FeSe display a less pronounced anisotropy than expected.

cond-mat.supr-con↗

arXiv2018

Determining the local low-energy excitations in the Kondo semimetal CeRu$_4$Sn$_6$ using resonant inelastic x-ray scattering

We have investigated the local low-energy excitations in CeRu$_4$Sn$_6$, a material discussed recently in the framework of strongly correlated Weyl semimetals, by means of Ce $M_5$ resonant inelastic x-ray scattering (RIXS). The availability of both $^2$F$_\frac{5}{2}$ and $^2$F$_\frac{7}{2}$ excitations of the Ce $4f^1$ configuration in the spectra allows for the determination of the crystal-electric field parameters that explain quantitatively the temperature dependence and anisotropy of the magnetic susceptibility. The absence of an azimuthal dependence in the spectra indicates that all crystal-electric field states are close to being rotational symmetric. We show further that the non-negligible impact of the $\check A_6^0$ parameter on the ground state of CeRu$_4$Sn$_6$ leads to a reduction of the magnetic moment due to multiplet intermixing. The RIXS results are consistent with inelastic neutron scattering (INS) data and are compared to the predictions from \textsl{ab-initio} based electronic structure calculations.

cond-mat.str-el↗