arXiv subjects

A. Podlesnyak

Publications and source records attributed to A. Podlesnyak.

At least 37 records · Page 2Linked to original sources

arXiv2021

Field-Induced Spin Excitations in the Spin-1/2 Triangular-Lattice Antiferromagnet CsYbSe$_2$

A layered triangular lattice with spin-1/2 ions is an ideal platform to explore highly entangled exotic states like quantum spin liquid (QSL). Here, we report a systematic in-field neutron scattering study on a perfect two-dimensional triangular-lattice antiferromagnet, CsYbSe$_2$, a member of the large QSL candidate family rare-earth chalcogenides. The elastic neutron scattering measured down to 70 mK shows that there is a short-range 120$^{\circ}$ magnetic order at zero field. In the field-induced ordered states, the spin-spin correlation lengths along the $c$ axis are relatively short, although the heat capacity results indicate long-range magnetic orders at 3 T $-$ 5 T. The inelastic neutron scattering spectra evolve from highly damped continuum-like excitations at zero field to relatively sharp spin wave modes at the plateau phase. Our extensive large-cluster density-matrix renormalization group calculations with a Heisenberg triangular-lattice nearest-neighbor antiferromagnetic model reproduce the essential features of the experimental spectra, including continuum-like excitations at zero field, series of sharp magnons at the plateau phase as well as two-magnon excitations at high energy. This work presents comprehensive experimental and theoretical overview of the unconventional field-induced spin dynamics in triangular-lattice Heisenberg antiferromagnet and thus provides valuable insight into quantum many-body phenomena.

cond-mat.str-el↗

arXiv2021

Direct determination of the zero-field splitting for Fe$^{3+}$ ion in a synthetic polymorph of the oxalate mineral stepanovite NaMgFe(C$_2$O$_4$)$_3\cdot$9H$_2$O: a natural MOF

We employed inelastic neutron scattering (INS), specific heat, and magnetization analysis to study the magnetism in a synthetic polymorph of the quasi-two-dimensional natural metal-organic framework material, stepanovite NaMgFe(C$_2$O$_4$)$_3\cdot$9H$_2$O. No long-range magnetic order can be observed down to 0.5 K. The INS spectra show two dispersionless excitations at energy transfer 0.028(1) and 0.050(1) meV at base temperature, which are derived from the magnetic transitions between zero-field splitting (ZFS) of $S$ = 5/2 ground state multiplets of Fe$^{3+}$ ion. Further analysis of the INS results shows that the Fe$^{3+}$ ion has an easy-axis anisotropy with axial ZFS parameter $D$ = $-$0.0128(5) meV and rhombic parameter $E$ = 0.0014(5) meV. The upward behavior at zero field and Schottky-like peak under magnetic field of the low-temperature magnetic specific heat further support the INS results. Our results clearly reveal the magnetic ground and excited state of this stepanovite polymorph.

cond-mat.mtrl-sci↗

arXiv2021

Low-energy spin dynamics in rare-earth perovskite oxides

We review recent studies of spin dynamics in rare-earth orthorhombic perovskite oxides of the type $RM$O$_3$, where $R$ is a rare-earth ion and $M$ is a transition-metal ion, using single-crystal inelastic neutron scattering (INS). After a short introduction to the magnetic INS technique in general, the results of INS experiments on both transition-metal and rare-earth subsystems for four selected compounds (YbFeO$_3$, TmFeO$_3$, YFeO$_3$, YbAlO$_3$) are presented. We show that the spectrum of magnetic excitations consists of two types of collective modes that are well separated in energy: gapped magnons with a typical bandwidth of $<$70 meV, associated with the antiferromagnetically (AFM) ordered transition-metal subsystem, and AFM fluctuations of $<$5 meV within the rare-earth subsystem, with no hybridization of those modes. We discuss the high-energy conventional magnon excitations of the 3$d$ subsystem only briefly, and focus in more detail on the spectacular dynamics of the rare-earth sublattice in these materials. We observe that the nature of the ground state and the low-energy excitation strongly depends on the identity of the rare-earth ion. In the case of non-Kramers ions, the low-symmetry crystal field completely eliminates the degeneracy of the multiplet state, creating a rich magnetic field-temperature phase diagram. In the case of Kramers ions, the resulting ground state is at least a doublet, which can be viewed as an effective quantum spin-1/2. Equally important is the fact that in Yb-based materials the nearest-neighbor exchange interaction dominates in one direction, despite the three-dimensional nature of the orthoperovskite crystal structure. The observation of a fractional spinon continuum and quantum criticality in YbAlO$_3$ demonstrates that Kramers rare-earth based magnets can provide realizations of various aspects of quantum low-dimensional physics.

cond-mat.str-el↗

arXiv2021

High-field spin-flop state in green dioptase

The high-field magnetic properties and magnetic order of the gem mineral green dioptase Cu$_6[$Si$_6$O$_{18}]\cdot 6$H$_2$O have been studied by means of single-crystal neutron diffraction in magnetic fields up to $21~$T and magnetization measurements up to $30~$T. In zero field, the Cu$^{2+}$-moments in the antiferromagnetic chains are oriented along the $c$-axis with a small off-axis tilt. For a field applied parallel to the $c$-axis, the magnetization shows a spin-flop-like transition at $B^*=12.2~$T at $1.5~$K. Neutron diffraction experiments show a smooth behavior in the intensities of the magnetic reflections without any change in the periodicity of the magnetic structure. Bulk and microscopic observations are well described by a model of ferromagnetically coupled antiferromagnetic $XXZ$ spin-$\frac{1}{2}$ chains, taking into account a change of the local easy-axis direction. We demonstrate that the magnetic structure evolves smoothly from a deformed Néel state at low fields to a deformed spin-flop state in a high field via a strong crossover around $B^*$. The results are generalized for different values of interchain coupling and spin anisotropy.

cond-mat.str-el↗

arXiv2020

Electron-phonon coupling and superconductivity in the doped topological-crystalline insulator (Pb$_{0.5}$Sn$_{0.5}$)$_{1-x}$In$_x$Te

We present a neutron scattering study of phonons in single crystals of (Pb$_{0.5}$Sn$_{0.5}$)$_{1-x}$In$_x$Te with $x=0$ (metallic, but nonsuperconducting) and $x=0.2$ (nonmetallic normal state, but superconducting). We map the phonon dispersions (more completely for $x=0$) and find general consistency with theoretical calculations, except for the transverse and longitudinal optical (TO and LO) modes at the Brillouin zone center. At low temperature, both modes are strongly damped but sit at a finite energy ($\sim4$ meV in both samples), shifting to higher energy at room temperature. These modes are soft due to a proximate structural instability driven by the sensitivity of Pb-Te and Sn-Te $p$-orbital hybridization to off-center displacements of the metal atoms. The impact of the soft optical modes on the low-energy acoustic modes is inferred from the low thermal conductivity, especially at low temperature. Given that the strongest electron-phonon coupling is predicted for the LO mode, which should be similar for both studied compositions, it is intriguing that only the In-doped crystal is superconducting. In addition, we observe elastic diffuse (Huang) scattering that is qualitatively explained by the difference in Pb-Te and Sn-Te bond lengths within the lattice of randomly distributed Pb and Sn sites. We also confirm the presence of anomalous diffuse low-energy atomic vibrations that we speculatively attribute to local fluctuations of individual Pb atoms between off-center sites.

cond-mat.supr-con↗

arXiv2020

Gradual pressure-induced enhancement of magnon excitations in CeCoSi

CeCoSi is an intermetallic antiferromagnet with a very unusual temperature-pressure phase diagram: at ambient pressure it orders below $T_{\mathrm{N}} = 8.8$ K, while application of hydrostatic pressure induces a new magnetically ordered phase with exceptionally high transition temperature of $\sim40$ K at 1.5 GPa. We studied the magnetic properties and the pressure-induced magnetic phase of CeCoSi by means of elastic and inelastic neutron scattering (INS) and heat capacity measurements. At ambient pressure CeCoSi orders into a simple commensurate AFM structure with a reduced ordered moment of only $m_{\mathrm{Ce}} = 0.37(6)$ $μ_{\mathrm{B}}$. Specific heat and low-energy INS indicate a significant gap in the low-energy magnon excitation spectrum in the antiferromagnetic phase, with the CEF excitations located above 10 meV. Hydrostatic pressure gradually shifts the energy of the magnon band towards higher energies, and the temperature dependence of the magnons measured at 1.5 GPa is consistent with the phase diagram. Moreover, the CEF excitations are also drastically modified under pressure.

cond-mat.str-el↗

arXiv2020

Spin-Coupling Topology in the Copper Hexamer Compounds A$_2$Cu$_3$O(SO$_4$)$_3$ (A=Na, K)

The compounds A$_2$Cu$_3$O(SO$_4$)$_3$ (A=Na, K) are characterized by copper hexamers which are weakly coupled to realize antiferromagnetic order below TN=3 K. They constitute novel quantum spin systems with S=1 triplet ground-states. We investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering experiments covering the entire range of the magnetic excitation spectra. The observed transitions are governed by very unusual selection rules which we ascribe to the underlying spin-coupling topology. This is rationalized by model calculations which allow an unambiguous interpretation of the magnetic excitations concerning both the peak assignments and the nature of the spin-coupling parameters.

cond-mat.str-el↗

arXiv2020

Experimental observation of magnetic dimers in diluted Yb:YAlO$_3$

We present a comprehensive experimental investigation of Yb magnetic dimers in Yb$_{0.04}$Y$_{0.96}$AlO$_3$, an Yb-doped Yttrium Aluminum Perovskite (YAP) YAlO$_3$ by means of specific heat, magnetization and high-resolution inelastic neutron scattering (INS) measurements. In our sample, the Yb ions are randomly distributed over the lattice and $\sim 7$\% of Yb ions form quantum dimers due to nearest-neighbor antiferromagnetic coupling along the $c$-axis. At zero field, the dimer formation manifests itself in an appearance of an inelastic peak at $Δ\approx 0.2$~meV in the INS spectrum and a Schottky-like anomaly in the specific heat. The structure factor of the INS peak exhibits a cosine modulation along the $L$ direction, in agreement with the $c$-axis nearest-neighbor intra-dimer coupling. A careful fitting of the low-temperature specific heat shows that the excited state is a degenerate triplet, which indicates a surprisingly small anisotropy of the effective Yb-Yb exchange interaction despite the low crystal symmetry and anisotropic magnetic dipole contribution, in agreement with previous reports for the Yb parent compound, YbAlO$_3$ [arXiv:1904.11513, arXiv:1902.04112], and in contrast to Yb$_2$Pt$_2$Pb [arXiv:1606.01309, arXiv:1907.01067]. The obtained results are precisely reproduced by analytical calculations for the Yb dimers.

cond-mat.str-el↗

arXiv2020

Field-angle resolved magnetic excitations as a probe of hidden-order symmetry in CeB6

In contrast to magnetic order formed by electrons' dipolar moments, ordering phenomena associated with higher-order multipoles (quadrupoles, octupoles, etc.) are more difficult to characterize because of the limited choice of experimental probes that can distinguish different multipolar moments. The heavy-fermion compound CeB6 and its La-diluted alloys are among the best-studied realizations of the long-range-ordered multipolar phases, often referred to as "hidden order". Previously the hidden order in phase II was identified as primary antiferroquadrupolar (AFQ) and field-induced octupolar (AFO) order. Here we present a combined experimental and theoretical investigation of collective excitations in the phase II of CeB6. Inelastic neutron scattering (INS) in fields up to 16.5 T reveals a new high-energy mode above 14 T in addition to the low-energy magnetic excitations. The experimental dependence of their energy on the magnitude and angle of the applied magnetic field is compared to the results of a multipolar interaction model. The magnetic excitation spectrum in rotating field is calculated within a localized approach using the pseudo-spin presentation for the Gamma8 states. We show that the rotating-field technique at fixed momentum can complement conventional INS measurements of the dispersion at constant field and holds great promise for identifying the symmetry of multipolar order parameters and the details of inter-multipolar interactions that stabilize hidden-order phases.

cond-mat.str-el↗

arXiv2019

Chemical composition induced quantum phase transition in Cs$_{1-x}$Rb$_{x}$FeCl$_{3}$

The isostructural series of $S=1$ quantum magnets Cs$_{1-x}$Rb$_{x}$FeCl$_{3}$ is investigated, using both thermodynamic measurements and inelastic neutron scattering experiments. It is found that increasing Rb content the system evolves from the gapped state at $x=0$, through a quantum phase transition at $x\sim 0.35$, and to the magnetically ordered state at larger $x$. Inelastic neutron experiments for $x=0$, $x=0.3$, and $x=1$ demonstrate that the magnetic anisotropy and spin interactions are continuously tuned by the chemical composition. For the intermediate concentration all magnetic excitations are substantial broadened suggesting that disorder plays a key role in this species. For the two end-compounds, excitations remain sharp.

cond-mat.str-el↗

arXiv2019

Evolution of the propagation vector of antiferroquadrupolar phases in Ce3Pd20Si6 with magnetic field

Hidden-order phases that occur in a number of correlated f-electron systems are among the most elusive states of electronic matter. Their investigations are hindered by the insensitivity of standard physical probes, such as neutron diffraction, to the order parameter that is usually associated with higher-order multipoles of the f-orbitals. The heavy-fermion compound Ce3Pd20Si6 exhibits magnetically hidden order at subkelvin temperatures, known as phase II. Additionally, for magnetic field applied along the [001] cubic axis, another phase II' was detected, but the nature of the transition from phase II to phase II' remained unclear. Here we use inelastic neutron scattering to demonstrate that this transition is associated with a change in the propagation vector of the antiferroquadrupolar order from (111) to (100). Despite the absence of magnetic Bragg scattering in phase II', its ordering vector is revealed by the location of an intense magnetic soft mode at the (100) wave vector, orthogonal to the applied field. At the II-II' transition, this mode softens and transforms into quasielastic and nearly Q-independent incoherent scattering, which is likely related to the non-Fermi-liquid behavior recently observed at this transition. Our experiment also reveals sharp collective excitations in the field-polarized paramagnetic phase, after phase II' is suppressed in fields above 4 T.

cond-mat.str-el↗

arXiv2019

Antiferromagnetic ordering and dipolar interactions of YbAlO$_3$

In this paper we report low-temperature magnetic properties of the rare-earth perovskite material YbAlO$_3$. Results of elastic and inelastic neutron scattering experiment, magnetization measurements along with the crystalline electrical field (CEF) calculations suggest that the ground state of Yb moments is a strongly anisotropic Kramers doublet, and the moments are confined in the $ab$-plane, pointing at an angle of $φ= \pm 23.5^{\circ}$ to the $a$-axis. With temperature decreasing below $T_{\rm N}=0.88$ K, Yb moments order into the coplanar, but non-collinear antiferromagnetic (AFM) structure $AxGy$, where the moments are pointed along their easy-axes. In addition, we highlight the importance of the dipole-dipole interaction, which selects the type of magnetic ordering and may be crucial for understanding magnetic properties of other rare-earth orthorhombic perovskites. Further analysis of the broad diffuse neutron scattering shows that one-dimensional interaction along the $c$-axis is dominant, and suggests YbAlO$_3$ as a new member of one dimensional quantum magnets.

cond-mat.str-el↗

arXiv2019

Clamp cell with $in$ $situ$ pressure monitoring for low-temperature neutron scattering measurements

A clamp pressure cell for neutron scattering experiments at low temperatures and in external magnetic fields under pressure up to 2~GPa has been fabricated and tested. The cell provides optical access to the sample space that allows instantaneous pressure determination during sample loading, cooling and measuring using ruby and/or samarium doped strontium tetraborate fluorescence monitoring. A new calibration curve of the pressure-induced shift of the $^7D_0 - ^5F_0$ (0-0) line in the fluorescent spectrum of SrB$_4$O$_7$:Sm$^{2+}$ for moderate pressures, $P\leqslant{2}$ GPa, is given.

physics.ins-det↗

arXiv2019

Tomonaga-Luttinger Liquid Behavior and Spinon Confinement in YbAlO$_3$

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth based magnets because of the large effective spin anisotropy induced by the combination of strong spin-orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO$_3$ provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga-Luttinger liquid behavior and spinon confinement-deconfinement transitions in different regions of magnetic field-temperature phase diagram.

cond-mat.str-el↗

arXiv2018

Spin Triplet Ground-State in the Copper Hexamer Compounds A2Cu3O(SO4)3 (A=Na,K)

The compounds A2Cu3O(SO4)3 (A=Na,K) are characterized by copper hexamers which are weakly coupled along the b-axis to realize one-dimensional antiferromagnetic chains below TN=3 K, whereas the interchain interactions along the a- and c-axes are negligible. We investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering below and above TN. The eight lowest-lying hexamer states could be unambiguously assigned and parametrized in terms of a Heisenberg exchange Hamiltonian, providing direct experimental evidence for an S=1 triplet ground-state associated with the copper hexamers. Therefore, the compounds A2Cu3O(SO4)3 serve as novel cluster-based spin-1 antiferromagnets to support Haldane's conjecture that a gap appears in the excitation spectrum below TN, which was verified by inelastic neutron scattering.

cond-mat.mtrl-sci↗

arXiv2018

Decoupled spin dynamics in the rare-earth orthoferrite YbFeO$_3$: Evolution of magnetic excitations through the spin-reorientation transition

In this paper we present a comprehensive study of magnetic dynamics in the rare-earth orthoferrite YbFeO$_3$ at temperatures below and above the spin-reorientation (SR) transition $T_{\mathrm{SR}}=7.6$ K, in magnetic fields applied along the $a, b$ and $c$ axes. Using single-crystal inelastic neutron scattering, we observed that the spectrum of magnetic excitations consists of two collective modes well separated in energy: 3D gapped magnons with a bandwidth of $\sim$60 meV, associated with the antiferromagnetically (AFM) ordered Fe subsystem, and quasi-1D AFM fluctuations of $\sim$1 meV within the Yb subsystem, with no hybridization of those modes. The spin dynamics of the Fe subsystem changes very little through the SR transition and could be well described in the frame of semiclassical linear spin-wave theory. On the other hand, the rotation of the net moment of the Fe subsystem at $T_{\mathrm{SR}}$ drastically changes the excitation spectrum of the Yb subsystem, inducing the transition between two regimes with magnon and spinon-like fluctuations. At $T < T_{\mathrm{SR}}$, the Yb spin chains have a well defined field-induced ferromagnetic (FM) ground state, and the spectrum consists of a sharp single-magnon mode, a two-magnon bound state, and a two-magnon continuum, whereas at $T > T_{\mathrm{SR}}$ only a gapped broad spinon-like continuum dominates the spectrum. In this work we show that a weak quasi-1D coupling within the Yb subsystem $J_\text{Yb-Yb}$, mainly neglected in previous studies, creates unusual quantum spin dynamics on the low energy scales. The results of our work may stimulate further experimental search for similar compounds with several magnetic subsystems and energy scales, where low-energy fluctuations and underlying physics could be "hidden" by a dominating interaction.

cond-mat.str-el↗

arXiv2018

Short range order in the quantum XXZ honeycomb lattice material BaCo$_2$(PO$_4$)$_2$

We present observations of highly frustrated quasi two-dimensional (2D) magnetic correlations in the honeycomb lattice layers of the S$_{eff}$ = 1/2 compound $γ$-BaCo$_2$(PO$_4$)$_2$ ($γ$-BCPO). Specific heat shows a broad peak comprised of two weak kink features at $T_{N1} \sim$ 6 K and $T_{N2} \sim$ 3.5 K, the relative weights of which can be modified by sample annealing. Neutron powder diffraction measurements reveal short range quasi-2D order that is established below $T_{N1}$ and $T_{N2}$, at which two separate, incompatible, short range magnetic orders onset: commensurate antiferromagnetic correlations with correlation length $ξ_c = 60\pm2$ Å\ ($T_{N1}$) and in quasi-2D helical domains with $ξ_h = 350 \pm 11$ Å\ ($T_{N2}$). The ac magnetic susceptibility response lacks frequency dependence, ruling out spin freezing. Inelastic neutron scattering data on $γ$-BCPO is compared with linear spin wave theory, and two separate parameter regions of the XXZ $J_1$-$J_2$-$J_3$ model with ferromagnetic nearest-neighbor exchange $J_1$ are favored, both near regions of high classical degeneracy. High energy coherent excitations ($\sim 10$ meV) persist up to at least 40 K, suggesting strong in-plane correlations persist above $T_N$. These data show that $γ$-BCPO is a rare highly frustrated, quasi-2D S$_{eff}$ = 1/2 honeycomb lattice material which resists long range magnetic order and spin freezing.

cond-mat.str-el↗

arXiv2018

Tunable Emergent Heterostructures in a Prototypical Correlated Metal

At the interface between two distinct materials desirable properties, such as superconductivity, can be greatly enhanced, or entirely new functionalities may emerge. Similar to in artificially engineered heterostructures, clean functional interfaces alternatively exist in electronically textured bulk materials. Electronic textures emerge spontaneously due to competing atomic-scale interactions, the control of which, would enable a top-down approach for designing tunable intrinsic heterostructures. This is particularly attractive for correlated electron materials, where spontaneous heterostructures strongly affect the interplay between charge and spin degrees of freedom. Here we report high-resolution neutron spectroscopy on the prototypical strongly-correlated metal CeRhIn5, revealing competition between magnetic frustration and easy-axis anisotropy -- a well-established mechanism for generating spontaneous superstructures. Because the observed easy-axis anisotropy is field-induced and anomalously large, it can be controlled efficiently with small magnetic fields. The resulting field-controlled magnetic superstructure is closely tied to the formation of superconducting and electronic nematic textures in CeRhIn5, suggesting that in-situ tunable heterostructures can be realized in correlated electron materials.

cond-mat.str-el↗