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Alexander I. Kolesnikov

Publications and source records attributed to Alexander I. Kolesnikov.

At least 37 records · Page 2Linked to original sources

Two-Step Electronic Response to Magnetic Ordering in a van der Waals Ferromagnet

The two-dimensional (2D) material Cr$_2$Ge$_2$Te$_6$ is a member of the class of insulating van der Waals magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te $p$-orbital-dominated bands to undergo changes at the Curie transition temperature T$_C$ while the Cr $d$-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets.

cond-mat.str-el↗

Static magnetic order with strong quantum fluctuations in spin-1/2 honeycomb magnet Na2Co2TeO6

Kitaev interactions, arising from the interplay of frustration and bond anisotropy, can lead to strong quantum fluctuations and, in an ideal case, to a quantum-spin-liquid state. However, in many nonideal materials, spurious non-Kitaev interactions typically promote a zigzag antiferromagnetic order in the d-orbital transition metal compounds. By combining neutron scattering with muon-spin rotation and relaxation techniques, we provide new insights into the exotic properties of Na2Co2TeO6, a candidate Kitaev material. Below TN, the zero-field muon-spin relaxation rate becomes almost constant (at 0.45 us-1). We attribute this temperature-independent muon-spin relaxation rate to the strong quantum fluctuations, as well as to the frustrated Kitaev interactions. As the magnetic field increases, neutron scattering data indicate a much broader spin-wave-excitation gap at the K-point. Therefore, quantum fluctuations seem not only robust, but are even enhanced by the applied magnetic field. Our findings provide valuable hints for understanding the onset of the quantum-spin-liquid state in Kitaev materials.

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Fluctuation-driven, topology-stabilized order in a correlated nodal semimetal

The interplay between strong electron correlation and band topology is at the forefront of condensed matter research. As a direct consequence of correlation, magnetism enriches topological phases and also has promising functional applications. However, the influence of topology on magnetism remains unclear, and the main research effort has been limited to ground state magnetic orders. Here we report a novel order above the magnetic transition temperature in magnetic Weyl semimetal (WSM) CeAlGe. Such order shows a number of anomalies in electrical and thermal transport, and neutron scattering measurements. We attribute this order to the coupling of Weyl fermions and magnetic fluctuations originating from a three-dimensional Seiberg-Witten monopole, which qualitatively agrees well with the observations. Our work reveals a prominent role topology may play in tailoring electron correlation beyond ground state ordering, and offers a new avenue to investigate emergent electronic properties in magnetic topological materials.

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Realization of two-sublattice exchange physics in the triangular lattice compound Ba3Er(BO3)3

We have synthesized high-quality single crystal samples of the erbium-based triangular lattice compound Ba3Er(BO3)3. Thermal and magnetic measurements reveal large anisotropy and a possible phase transition at 100 mK. The low-temperature magnetic heat capacity can be understood from the two Wyckoff positions that the magnetic ions Er3+ occupy, which have distinct symmetry properties and crystal field environments. A point charge calculation for the crystal electric field levels is consistent with this understanding. Based on symmetry analysis and classical simulation, we argue that Ba3Er(BO3)3 realizes an interesting two-sublattice exchange physics, in which the honeycomb lattice spins develop ferromagnetic correlations due to the additional spins at the hexagon centers but eventually order antiferromagnetically. Additionally, our results suggest that quantum fluctuations need to be considered in order to fully explain the experimental observations.

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Coupling of magnetism and Dirac fermions in YbMnSb2

We report inelastic neutron scattering measurements of magnetic excitations in YbMnSb2, a low-carrier-density Dirac semimetal in which the antiferromagnetic Mn layers are interleaved with Sb layers that host Dirac fermions. We observe a considerable broadening of spin waves, which is consistent with substantial spin fermion coupling. The spin wave damping, $γ$, in YbMnSb2 is roughly twice larger compared to that in a sister material, YbMnBi2, where an indication of a small damping consistent with theoretical analysis of the spin-fermion coupling was reported. The inter-plane interaction between the Mn layers in YbMnSb2 is also much stronger, suggesting that the interaction mechanism is rooted in the same spin-fermion coupling. Our results establish the systematics of spin-fermion interactions in layered magnetic Dirac materials.

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Chemical Design of Electronic and Magnetic Energy Scales in Tetravalent Praseodymium

Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the 4+ oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr4+ oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f1 configuration with ligand valence electrons, analogous to transition metals. The resulting competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr4+, which departs from the Jeff =1/2 limit and resembles that of high-valent actinides. Our results show that Pr4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials.

cond-mat.mtrl-sci↗

Antiferromagnetic fluctuations and orbital-selective Mott transition in the van der Waals ferromagnet Fe3-xGeTe2

Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal that the competing magnetic fluctuations are driven by an orbital selective Mott transition, where only the plane-perpendicular a1g orbital of the Fe(3d) manifold remains itinerant. Our results highlight the multi-orbital character in Fe3-xGeTe2 that supports a rare coexistence of local and itinerant physics within this material.

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Anisotropic magnon damping by zero-temperature quantum fluctuations in ferromagnetic CrGeTe$_3$

Spin and lattice are two fundamental degrees of freedom in a solid, and their fluctuations about the equilibrium values in a magnetic ordered crystalline lattice form quasiparticles termed magnons (spin waves) and phonons (lattice waves), respectively. In most materials with strong spin-lattice coupling (SLC), the interaction of spin and lattice induces energy gaps in the spin wave dispersion at the nominal intersections of magnon and phonon modes. Here we use neutron scattering to show that in the two-dimensional (2D) van der Waals honeycomb lattice ferromagnetic CrGeTe3, spin waves propagating within the 2D plane exhibit an anomalous dispersion, damping, and break-down of quasiparticle conservation, while magnons along the c axis behave as expected for a local moment ferromagnet. These results indicate the presence of dynamical SLC arising from the zero-temperature quantum fluctuations in CrGeTe3, suggesting that the observed in-plane spin waves are mixed spin and lattice quasiparticles fundamentally different from pure magnons and phonons.

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Geometrical frustration versus Kitaev interactions in BaCo$_2$(AsO$_4$)$_2$

Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid state. One of the front-runners is BaCo$_2$(AsO$_4$)$_2$ (BCAO), where it was suggested that the exchange processes between Co$^{2+}$ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze comprehensive inelastic neutron scattering studies of BCAO with fields in the honeycomb plane. Combining the constraints from the magnon excitations in the high-field polarized state and the inelastic spin structure factor measured in zero magnetic field, we examine two leading theoretical models: the Kitaev-type \JKG model and the \XXZ model. We show that the existing experimental data can be consistently accounted for by the \XXZ model but not by the \JKG model, and we discuss the implications of these results for the realization of a spin liquid phase in BCAO and more generally for the realization of the Kitaev model in cobaltates.

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Dynamic Parallel Spin Stripes from the 1/8 anomaly to the End of Superconductivity in La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$

We have carried out new neutron spectroscopic measurements on single crystals of La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ from 0.12 to 0.26 using time-of-flight techniques. These measurements allow us to follow the evolution of parallel spin stripe fluctuations with energies less than 33 meV, from x=0.12 to 0.26. Samples at these hole-doping levels are known to display static (on the neutron scattering time scale) parallel spin stripes at low temperature, with onset temperatures and intensities which decrease rapidly with increasing x. Nonetheless, we report remarkably similar dynamic spectral weight for the corresponding dynamic parallel spin stripes, between 5 meV to 33 meV, from the 1/8 anomaly near x=0.12, to optimal doping near x=0.19 to the quantum critical point for the pseudogap phase near x=0.24, and finally to the approximate end of superconductivity near x=0.26. This observed dynamic magnetic spectral weight is structured in energy with a peak near 17 meV at all dopings studied. Earlier neutron and resonant x-ray scattering measurements on related cuprate superconductors have reported both a disappearance with increasing doping of magnetic fluctuations at ($π$, $π$) wavevectors characterizing parallel spin stripe structures, and persistant paramagnon scattering away from this wavevector, respectively. Our new results on La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ from 0.12 < x <0.26 clearly show persistent parallel spin stripe fluctuations at and around at ($π$, $π$), and across the full range of doping studied. These results are also compared to recent theory. Together with a rapidly declining x-dependence to the static parallel spin stripe order, the persistent parallel spin stripe fluctuations show a remarkable similarity to the expectations of a quantum spin glass, random t-J model, recently introduced to describe strong local correlations in cuprates.

cond-mat.supr-con↗

Massless Dirac magnons in the two dimensional van der Waals honeycomb magnet CrCl3

Two dimensional van der Waals ferromagnets with honeycomb structures are expected to host the bosonic version of Dirac particles in their magnon excitation spectra. Using inelastic neutron scattering, we study spin wave excitations in polycrystalline CrCl$_3$, which exhibits ferromagnetic honeycomb layers with antiferromagnetic stackings along the $c$-axis. For comparison, polycrystal samples of CrI$_3$ with different grain sizes are also studied. We find that the powder-averaged spin wave spectrum of CrCl$_3$ at $T$ = 2 K can be adequately explained by the two dimensional spin Hamiltonian including in-plane Heisenberg exchanges only. The observed excitation does not exhibit noticeable broadening in energy, which is in remarkable contrast to the substantial broadening observed in CrI$_3$. Based on these results, we conclude that the ferromagnetic phase of CrCl$_3$ hosts massless Dirac magnons and is thus not topological.

cond-mat.str-el↗

Unusual exchange couplings and intermediate temperature Weyl state in Co3Sn2S2

Understanding the magnetism and its possible correlations to the topological properties has emerged as a forefront and difficult topic in studying magnetic Weyl semimetals. Co$_{3}$Sn$_{2}$S$_{2}$ is a newly discovered magnetic Weyl semimetal with a kagome lattice of cobalt ions and has triggered intense interest for rich fantastic phenomena. Here, we report the magnetic exchange couplings of Co$_{3}$Sn$_{2}$S$_{2}$ using inelastic neutron scattering and two density functional theory (DFT) based methods: constrained magnetism and multiple-scattering Green's function methods. Co$_{3}$Sn$_{2}$S$_{2}$ exhibits highly anisotropic magnon dispersions and linewidths below $T_{C}$, and paramagnetic excitations above $T_{C}$. The spin-wave spectra in the ferromagnetic ground state is well described by the dominant third-neighbor "across-hexagon" $J_{d}$ model. Our density functional theory calculations reveal that both the symmetry-allowed 120$^\circ$ antiferromagnetic orders support Weyl points in the intermediate temperature region, with distinct numbers and the locations of Weyl points. Our study highlights the important role Co$_{3}$Sn$_{2}$S$_{2}$ can play in advancing our understanding of kagome physics and exploring the interplay between magnetism and band topology.

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Magnetic field effect on topological spin excitations in CrI$_3$

The search for topological spin excitations in recently discovered two-dimensional (2D) van der Waals (vdW) magnetic materials is important because of their potential applications in dissipation-less spintronics. In the 2D vdW ferromagnetic (FM) honeycomb lattice CrI$_3$(T$_C$= 61 K), acoustic and optical spin waves were found to be separated by a gap at the Dirac points. The presence of such a gap is a signature of topological spin excitations if it arises from the next nearest neighbor(NNN) Dzyaloshinskii-Moriya (DM) or bond-angle dependent Kitaev interactions within the Cr honeycomb lattice. Alternatively, the gap is suggested to arise from an electron correlation effect not associated with topological spin excitations. Here we use inelastic neutron scattering to conclusively demonstrate that the Kitaev interactions and electron correlation effects cannot describe spin waves, Dirac gap and their in-plane magnetic field dependence. Our results support the DM interactions being the microscopic origin of the observed Dirac gap. Moreover, we find that the nearest neighbor (NN) magnetic exchange interactions along the axis are antiferromagnetic (AF)and the NNN interactions are FM. Therefore, our results unveil the origin of the observedcaxisAF order in thin layers of CrI$_3$, firmly determine the microscopic spin interactions in bulk CrI$_3$, and provide a new understanding of topology-driven spin excitations in 2D vdW magnets.

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Stoichiometric Tuning of Lattice Flexibility and Na Diffusion in NaAlSiO4: Quasielastic Neutron Scattering Experiment and Ab-initio Molecular Dynamics Simulations

We have performed quasielastic neutron scattering (QENS) experiments up to 1243 K and ab-initio molecular dynamics (AIMD) simulations to investigate the Na diffusion in various phases of NaAlSiO4 (NASO), namely, low-carnegieite (L-NASO; trigonal), high-carnegieite (H-NASO; cubic) and nepheline (N-NASO; hexagonal) phases. The QENS measurements reveal Na ions localized diffusion behavior in L-NASO and N-NASO, but long-range diffusion behavior in H-NASO. The AIMD simulation supplemented the QENS measurements and showed that excess Na ions in H-NASO enhance the host network flexibility and activate the AlO4/SiO4 tetrahedra rotational modes. These framework modes enable the long-range diffusion of Na across a pathway of interstitial sites. The simulations also show Na diffusion in Na-deficient N-NASO through vacant Na sites along the hexagonal c-axis.

cond-mat.mtrl-sci↗

Freezing of a disorder induced quantum spin liquid

$\rm{Sr_2CuTe_{0.5}W_{0.5}O_6}$ is a square-lattice magnet with super-exchange between S=1/2 $\rm{Cu^{2+}}$ spins mediated by randomly distributed Te and W ions. Here, using sub-K temperature and 20 $\rmμ$eV energy resolution neutron scattering experiments we show that this system transits from a gapless disorder-induced quantum spin liquid to a new quantum state below $\rm{T_f}$ = 1.7(1) K, exhibiting a weak frozen moment of /S ~ 0.1 and low energy dynamic susceptibility,$χ''({\hbarω})$ linear in energy which is surprising for such a weak freezing in this highly fluctuating quantum regime.

cond-mat.mtrl-sci↗

Collective excitations in the tetravalent lanthanide honeycomb antiferromagnet, Na2PrO3

Thermomagnetic and inelastic neutron scattering measurements on Na2PrO3 are reported. This material is an antiferromagnetic honeycomb magnet based on the tetravalent lanthanide Pr4+ and has been proposed to host dominant antiferromagnetic Kitaev interactions. These measurements reveal magnetic fluctuations in Na2PrO3 below an energy of 2 meV as well as crystal-field excitations around 230 meV. The latter energy is comparable to the scale of the spin-orbit interaction and explains both the very small effective moment of around 1.0 μB per Pr4+ and the difficulty to uncover any static magnetic scattering below the ordering transition at TN = 4.6 K. By comparing the low-energy magnetic excitations in Na2PrO3 to that of the isostructural spin-only compound, Na2TbO3, a microscopic model of exchange interactions is developed that implicates dominant and surprisingly large Heisenberg exchange interactions J approximately equal to 1.1(1) meV. Although antiferromagnetic Kitaev interactions with K less than or equal to 0.2J cannot be excluded, the inelastic neutron scattering data of Na2PrO3 is best explained with a delta = 1.24(2) easy-axis XXZ exchange anisotropy.

cond-mat.str-el↗

Parallel Spin Stripes and Their Coexistance with Superconducting Ground States at Optimal and High Doping in La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$

Quasi-two dimensional quantum magnetism is clearly highly correlated with superconducting ground states in cuprate-based High T$_c$ superconductivity. Three dimensional, commensurate long range magnetic order in La$_2$CuO$_4$ quickly evolves to quasi-two dimensional, incommensurate correlations on doping with mobile holes, and superconducting ground states follow for x as small as 0.05 in the La$_{2-x}$Sr$_x$/Ba$_x$CuO$_4$ family of superconductors. It has long been known that the onset of superconducting ground states in these systems is coincident with a remarkable rotation of the incommensurate spin order from "diagonal stripes" below x = 0.05, to "parallel stripes" above. However, little is known about the spin correlations at optimal and high doping levels, where the dome of superconductivity draws to an end. Here we present new elastic and inelastic neutron scattering measurements on single crystals of La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ with x = 0.125, 0.19, 0.24 and 0.26, and show that two dimensional, quasi-static, parallel spin stripes are observed to onset at temperatures such that the parallel spin stripe phase envelopes all superconducting ground states in this system. Parallel spin stripes stretch across 0.05 < < 0.26, with rapidly decreasing moment size and onset temperatures for x > 0.125. We also show that the low energy, parallel spin stripe fluctuations for optimally doped x = 0.19 display dynamic spectral weight which grows with decreasing temperature and saturates below its superconducting T$_c$. The elastic order parameter for x = 0.19 also shows plateau behavior coincident with the onset of superconductivity. This set of observations assert the foundational role played by two dimensional parallel spin stripe order and fluctuations in High T$_c$ cuprate superconductivity.

cond-mat.supr-con↗

Unconventional Hund Metal in a Weak Itinerant Ferromagnet

The physics of weak itinerant ferromagnets is challenging due to their small magnetic moments and the ambiguous role of local interactions governing their electronic properties, many of which violate Fermi liquid theory. While magnetic fluctuations play an important role in the materials' unusual electronic states, the nature of these fluctuations and the paradigms through which they arise remain debated. Here we use inelastic neutron scattering to study magnetic fluctuations in the canonical weak itinerant ferromagnet MnSi. Data reveal that short-wavelength magnons continue to propagate until a mode crossing predicted for strongly interacting quasiparticles is reached, and the local susceptibility peaks at a coherence energy predicted for a correlated Hund metal by first-principles many-body theory. Scattering between electrons and orbital and spin fluctuations in MnSi can be understood at the local level to generate non-Fermi liquid character. These results provide crucial insight into the role of interorbital Hund's exchange within the broader class of enigmatic multiband itinerant, weak ferromagnets.

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