arXiv subjects

A. I. Kolesnikov

Publications and source records attributed to A. I. Kolesnikov.

At least 19 recordsLinked to original sources

arXiv2026

Proximate Spin Liquid Ground State Arising from Competing Stripy and 120$^{\circ}$ Spin Correlations in the Triangular Quantum Antiferromagnet ErMgGaO$_4$

ErMgGaO$_4$ is a quantum antiferromagnet wherein the pseudospin-1/2 degrees of freedom of Er$^{3+}$ decorate two-dimensional triangular planes separated by disordered non-magnetic bilayers of Mg$^{2+}$ and Ga$^{3+}$. Unlike its sister compound, YbMgGaO$_4$, our powder ErMgGaO$_4$ sample shows a clear spin glass transition near $T_g \sim 2.5$~K, about 1/6 of its Curie-Weiss temperature. We have carried out new inelastic neutron scattering measurements on these powder ErMgGaO$_4$ samples. At high energies, we observed crystalline electric field (CEF) transitions within the $J=15/2$ multiplet of Er$^{3+}$, but with the first excited CEF level sufficiently low in energy ($\sim$ 3~meV) so as to allow the possibility that virtual CEF transitions influence the exchange couplings. At E=0, we observe diffuse elastic scattering which is analysed using Warren lineshapes appropriate for two dimensional correlations. This reveals dominant 2D stripy correlations below $T_g$, coexisting with 2D 120$^\circ$-type correlations that persist above $T_g$. At low temperatures, the low energy inelastic component of the scattering shows a continuum with bandwidth of $\sim$ 0.8~meV. This dynamic magnetic spectral weight can be modeled at all $Q$, energies, and temperatures as the sum of high energy and low energy damped harmonic oscillators (DHO), with the high energy DHO defining the bandwidth of $\sim$ 0.8~meV. We use linear spin wave theory to model this inelastic scattering and to estimate its spin Hamiltonian parameters in terms of a $J_1-J_2-Δ$ model on the triangular lattice. This gives a good description of the low lying spectral weight for ErMgGaO4, and allows us to place it on the theoretical $J_1-J_2-Δ$ phase diagram with $\frac{J_1}{J_2}=0.13 \pm 0.03$ and $Δ=0.4 \pm 0.1$, which is close to the expected quantum phase boundary between the spin liquid and the stripy ordered phases.

cond-mat.str-el↗

arXiv2025

Novel bipartite entanglement in the quantum dimer magnet Yb$_2$Be$_2$SiO$_7$

The quantum dimer magnet, with antiferromagnetic intradimer and interdimer Heisenberg exchange between spin-1/2 moments, is known to host an up/down - down/up singlet ground state when the intradimer exchange is dominant. Rare-earth-based quantum dimer systems with strong spin-orbit coupling offer the opportunity for tuning their magnetic properties by using magnetic anisotropy as a control knob. Here, we present bulk characterization and neutron scattering measurements of the quantum dimer magnet Yb$_2$Be$_2$SiO$_7$. We find that the Yb$^{3+}$ ions can be described by an effective spin-1/2 model at low temperatures and the system does not show signs of magnetic order down to 50 mK. The magnetization, heat capacity, and neutron spectroscopy data can be well-described by an isolated dimer model with highly anisotropic exchange that stabilizes a singlet ground state with a wavefunction up/up - down/down or up/up + down/down. Our results show that strong spin-orbit coupling can induce novel entangled states of matter in quantum dimer magnets.

cond-mat.str-el↗

arXiv2025

Two-Peak Heat Capacity Accounts for $R\ln(2)$ Entropy and Ground State Access in the Dipole-Octupole Pyrochlore Ce$_2$Hf$_2$O$_7$

Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce$_2$Hf$_2$O$_7$ down to a temperature of $T = 0.02$ K are reported. These show a two-peaked structure, with a Schottky-like peak at $T_1 \sim 0.065$ K, similar to what is observed in its sister Ce-pyrochlores Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$. However, a second sharper peak is observed at $T_2 \sim 0.025$ K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to $C_P=0$ at $T = 0$ K fully accounts for the $R\ln(2)$ entropy associated with the pseudospin-1/2 doublet for Ce$^{3+}$ in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in $C_P$ at much higher temperatures than the measured $T_2$ for expectations from an all-in all-out ground state of the XYZ Hamiltonian for Ce$_2$Hf$_2$O$_7$. The sharp low-temperature peak could also signify a cross-over from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured $C_P$ with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below $T \sim 0.25$ K. The diffuse magnetic neutron scattering observed from Ce$_2$Hf$_2$O$_7$ at low temperatures between $T_2$ and $T_1$ resembles that observed from Ce$_2$Zr$_2$O$_7$, which is well established as a $π$-flux quantum spin ice (QSI). Together with the peak in the heat capacity at $T_2$, this diffuse scattering from Ce$_2$Hf$_2$O$_7$ is suggestive of a classical spin liquid regime above $T_2$ that is distinct from the zero-entropy quantum ground state below $T_2$.

cond-mat.str-el↗

arXiv2025

Cooper-Pair Localization in the Magnetic Dynamics of a Cuprate Ladder

We investigate the spin dynamics of the cuprate ladder Sr$_{2.5}$Ca$_{11.5}$Cu$_{24}$O$_{41}$ to elucidate the behavior of its intrinsically doped holes. Combining high-resolution neutron spectroscopy and density matrix renormalization group calculations enables a comprehensive analysis of the collective magnetic dynamics. We find a general absence of magnetic signatures from unpaired charges, indicating holes within the system form strongly bound localized Cooper pairs. A one-band Hubbard model fails to match the spectral features but a straightforward extension to a large attractive nearest-neighbor interaction quantitatively explains our results. Our finding shows the significance of additional interactions beyond the long-predicted quantum spin pairing in the ($d$-wave) charge pairing process. Considering the parallels between ladders and two-dimensional cuprates, these results are potentially relevant for square lattices as well.

cond-mat.str-el↗

arXiv2024

Stripe magnetic order and field-induced quantum criticality in the perfect triangular-lattice antiferromagnet CsCeSe$_2$

The two-dimensional triangular-lattice antiferromagnet (TLAF) is a textbook example of frustrated magnetic systems. Despite its simplicity, the TLAF model exhibits a highly rich and complex magnetic phase diagram, featuring numerous distinct ground states that can be stabilized through frustrated next-nearest-neighbor couplings or anisotropy. In this paper, we report low-temperature magnetic properties of the TLAF material CsCeSe$_2$. The inelastic neutron scattering (INS) together with specific heat measurements and density functional theory calculations of crystalline electric field suggest that the ground state of Ce ions is a Kramers doublet with strong easy-plane anisotropy. Elastic neutron scattering measurements demonstrate the presence of stripe-$yz$ magnetic order that develops below $T_{\rm N} = 0.35$ K, with the zero-field ordered moment of $m_{\rm Ce} \approx 0.65~μ_{\rm B}$. Application of magnetic field first increases the ordering temperature by about 20% at the intermediate field region and eventually suppresses the stripe order in favor of the field-polarized ferromagnetic state via a continuous quantum phase transition (QPT). The field-induced response demonstrates sizable anisotropy for different in-plane directions, $\mathbf{B}\parallel{}\mathbf{a}$ and $\mathbf{B}\perp{}\mathbf{a}$, which indicates the presence of bond-dependent coupling in the spin Hamiltonian. We further show theoretically that the presence of anisotropic bond-dependent interactions can change the universality class of QPT for $\mathbf{B}\parallel{}\mathbf{a}$ and $\mathbf{B}\perp{}\mathbf{a}$.

cond-mat.str-el↗

arXiv2024

Unraveling the magnetic ground-state in alkali-metal lanthanide oxide Na$_2$PrO$_3$

A comprehensive set of muon spin spectroscopy and neutron scattering measurements supported by ab-initio and model Hamiltonian simulations have been used to investigate the magnetic ground state of Na$_2$PrO$_3$. $μ$SR reveals Néel antiferromagnetic order below $T_{\rm N}\! \sim\! 4.9$ K, with a small static magnetic moment $m_{\rm static}\!\leq \! 0.22$~$μ_{\rm B}/{\rm Pr}$ collinearly aligned along the $c-$axis. Inelastic neutron measurements reveal the full spectrum of crystal field excitations and confirm that the Pr$^{4+}$ ground state wave function deviates significantly from the $Γ_7$ limit relevant to the Kitaev model. Single and two magnon excitations are observed in the ordered state below $T_N=4.6$ K and are well described by non-linear spin wave theory from the Néel state using a magnetic Hamiltonian with Heisenberg exchange $J=1$ meV and symmetric anisotropic exchange $Γ/J=0.1$, corresponding to an XY model. Intense two magnon excitations are accounted for by $g$-factor anisotropy $g_\mathrm{z}/g_\pm = 1.29$. A fluctuating moment $δm^2 = 0.57(22)$ $μ_{\rm B}^2/{\rm Pr}$ extracted from the energy and momentum integrated inelastic neutron signal is reduced from expectations for a local $J=1/2$ moment with average $g$-factor $g_{\rm avg}\approx 1.1$. Together, the results demonstrate that the small moment in Na$_2$PrO$_3$ arises from crystal field and covalency effects and that the material does not exhibit significant quantum fluctuations..

cond-mat.str-el↗

arXiv2024

Magnetic properties of the quasi-XY Shastry-Sutherland magnet Er$_2$Be$_2$SiO$_7$

Polycrystalline and single crystal samples of the insulating Shastry-Sutherland compound Er$_2$Be$_2$SiO$_7$ were synthesized via a solid-state reaction and the floating zone method respectively. The crystal structure, Er single ion anisotropy, zero-field magnetic ground state, and magnetic phase diagrams along high-symmetry crystallographic directions were investigated by bulk measurement techniques, x-ray and neutron diffraction, and neutron spectroscopy. We establish that Er$_2$Be$_2$SiO$_7$ crystallizes in a tetragonal space group with planes of orthogonal Er dimers and a strong preference for the Er moments to lie in the local plane perpendicular to each dimer bond. We also find that this system has a non-collinear ordered ground state in zero field with a transition temperature of 0.841 K consisting of antiferromagnetic dimers and in-plane moments. Finally, we mapped out the $H-T$ phase diagrams for Er$_2$Be$_2$SiO$_7$ along the directions $H \parallel$ [001], [100], and [110]. While an increasing in-plane field simply induces a phase transition to a field-polarized phase, we identify three metamagnetic transitions before the field-polarized phase is established in the $H \parallel$ [001] case. This complex behavior establishes insulating Er$_2$Be$_2$SiO$_7$ and other isostructural family members as promising candidates for uncovering exotic magnetic properties and phenomena that can be readily compared to theoretical predictions of the exactly soluble Shastry-Sutherland model.

cond-mat.str-el↗

arXiv2023

Quantum to classical crossover in generalized spin systems -- the temperature-dependent spin dynamics of FeI$_2$

Simulating quantum spin systems at finite temperatures is an open challenge in many-body physics. This work studies the temperature-dependent spin dynamics of a pivotal compound, FeI$_2$, to determine if universal quantum effects can be accounted for by a phenomenological renormalization of the dynamical spin structure factor $S(\mathbf{q}, ω)$ measured by inelastic neutron scattering. Renormalization schemes based on the quantum-to-classical correspondence principle are commonly applied at low temperatures to the harmonic oscillators describing normal modes. However, it is not clear how to extend this renormalization to arbitrarily high temperatures. Here we introduce a temperature-dependent normalization of the classical moments, whose magnitude is determined by imposing the quantum sum rule, i.e. $\int dωd\mathbf{q} S(\mathbf{q}, ω) = N_S S (S+1)$ for $N_S$ dipolar magnetic moments. We show that this simple renormalization scheme significantly improves the agreement between the calculated and measured $S(\mathbf{q}, ω)$ for FeI$_{2}$ at all temperatures. Due to the coupled dynamics of dipolar and quadrupolar moments in that material, this renormalization procedure is extended to classical theories based on SU(3) coherent states, and by extension, to any SU(N) coherent state representation of local multipolar moments.

cond-mat.str-el↗

arXiv2023

Suppression of stacking order with doping in 1T-TaS$_{2-x}$Se$_x$

In 1T-TaS$_{2-x}$Se$_x$, the charge density wave (CDW) state features a star of David lattice that expands across layers as the system becomes commensurate on cooling. The layers can also order along the c-axis and different stacking orders have been proposed. Using neutron scattering on powder samples, we compared the stacking order previously observed in 1T-TaS$_2$ as the system is doped with Se. While at low temperature, a 13c layer sequence stacking was observed in TaS$_2$, this type of ordering was not evident with doping. Doping with Se results in a nearly commensurate state with the Mott state suppressed which may be linked to the absence of the layer stacking.

cond-mat.mtrl-sci↗

arXiv2023

High-energy spin waves in the spin-1 square-lattice antiferromagnet La$_2$NiO$_4$

Inelastic neutron scattering is used to study the magnetic excitations of the $S=1$ square-lattice antiferromagnet La$_2$NiO$_4$. We find that the spin waves cannot be described by a simple classical (harmonic) Heisenberg model with only nearest-neighbor interactions. The spin-wave dispersion measured along the antiferromagnetic Brillouin-zone boundary shows a minimum energy at the $(1/2,0)$ position as is observed in some $S=1/2$ square-lattice antiferromagnets. Thus, our results suggest that the quantum dispersion renormalization effects or longer-range exchange interactions observed in cuprates and other $S=1/2$ square-lattice antiferromagnets are also present in La$_2$NiO$_4$. We also find that the overall intensity of the spin-wave excitations is suppressed relative to linear spin-wave theory indicating that covalency is important. Two-magnon scattering is also observed.

cond-mat.str-el↗

arXiv2022

Spin excitations in the kagome-lattice metallic antiferromagnet Fe$_{0.89}$Co$_{0.11}$Sn

Kagome-lattice materials have attracted tremendous interest due to the broad prospect for seeking superconductivity, quantum spin liquid states, and topological electronic structures. Among them, the transition-metal kagome lattices are high-profile objects for the combination of topological properties, rich magnetism, and multiple-orbital physics. Here we report an inelastic neutron scattering study on the spin dynamics of a kagome-lattice antiferromagnetic metal Fe$_{0.89}$Co$_{0.11}$Sn. Although the magnetic excitations can be observed up to $\sim$250 meV, well-defined spin waves are only identified below $\sim$90 meV and can be modeled using Heisenberg exchange with ferromagnetic in-plane nearest-neighbor coupling $J_1$, in-plane next-nearest-neighbor coupling $J_2$, and antiferromagnetic (AFM) interlayer coupling $J_c$ under linear spin-wave theory. Above $\sim$90 meV, the spin waves enter the itinerant Stoner continuum and become highly damped particle-hole excitations. At the K point of the Brillouin zone, we reveal a possible band crossing of the spin wave, which indicates a potential Dirac magnon. Our results uncover the evolution of the spin excitations from the planar AFM state to the axial AFM state in Fe$_{0.89}$Co$_{0.11}$Sn, solve the magnetic Hamiltonian for both states, and confirm the significant influence of the itinerant magnetism on the spin excitations.

cond-mat.str-el↗

arXiv2022

Chern numbers of topological phonon band crossing determined with inelastic neutron scattering

Topological invariants in the band structure, such as Chern numbers, are crucial for the classification of topological matters and dictate the occurrence of exotic properties, yet their direct spectroscopic determination has been largely limited to electronic bands. Here, we use inelastic neutron scattering in conjunction with ab initio calculations to identify a variety of topological phonon band crossings in MnSi and CoSi single crystals. We find a distinct relation between the Chern numbers of a band-crossing node and the scattering intensity modulation in momentum space around the node. Given sufficiently high resolution, our method can be used to determine arbitrarily large Chern numbers of topological phonon band-crossing nodes.

cond-mat.mes-hall↗

arXiv2022

Spin waves and magnetic exchange Hamiltonian in CrSBr

CrSBr is an air-stable 2D van der Waals semiconducting magnet with great technological promise, but its atomic-scale magnetic interactions -- crucial information for high-frequency switching -- are poorly understood. We present an experimental study to determine the CrSBr magnetic exchange Hamiltonian and bulk magnon spectrum. We confirm the $A$-type antiferromagnetic order using single crystal neutron diffraction. We also measure the magnon dispersions using inelastic neutron scattering and rigorously fit the excitation modes to a spin wave model. The magnon spectrum is well described by an intra-plane ferromagnetic Heisenberg exchange model with seven nearest in-plane exchanges. This fitted exchange Hamiltonian enables theoretical predictions of CrSBr behavior: as one example, we use the fitted Hamiltonian to predict the presence of chiral magnon edge modes with a spin-orbit enhanced CrSBr heterostructure.

cond-mat.mtrl-sci↗

arXiv2022

Magnetic molecular orbitals in MnSi

A large body of knowledge about magnetism is attained from models of interacting spins, which usually reside on magnetic ions. Proposals beyond the ionic picture are uncommon and seldom verified by direct observations in conjunction with microscopic theory. Here, using inelastic neutron scattering to study the itinerant near-ferromagnet MnSi, we find that the system's fundamental magnetic units are interconnected, extended molecular orbitals consisting of three Mn atoms each, rather than individual Mn atoms. This result is further corroborated by magnetic Wannier orbitals obtained by ab initio calculations. It contrasts the ionic picture with a concrete example, and presents a novel regime of the spin waves where the wavelength is comparable to the spatial extent of the molecular orbitals. Our discovery brings important insights into not only the magnetism of MnSi, but also a broad range of magnetic quantum materials where structural symmetry, electron itinerancy and correlations act in concert.

cond-mat.str-el↗

arXiv2022

Single-ion properties of the transverse-field Ising model material CoNb$_2$O$_6$

CoNb$_2$O$_6$ is one of the few materials that is known to approximate the one-dimensional transverse-field Ising model (1D-TFIM) near its quantum critical point. It has been inferred that Co$^{2+}$ acts as a pseudo-spin 1/2 with anisotropic exchange interactions that are largely Ising-like, enabling the realization of the TFIM. However, the behavior of CoNb$_2$O$_6$ is known to diverge from the ideal TFIM under transverse magnetic fields that are far from the quantum critical point, requiring the consideration of additional anisotropic, bond-dependent (Kitaev-like) terms in the microscopic pseudo-spin 1/2 Hamiltonian. These terms are expected to be controlled in part by single-ion physics, namely the wavefunction for the pseudo-spin 1/2 angular momentum doublet. Here, we present the results of both inelastic neutron scattering measurements and electron paramagnetic resonance spectroscopy on CoNb$_2$O$_6$, which elucidate the single-ion physics of Co$^{2+}$ in CoNb$_2$O$_6$ for the first time. We find that the system is well-described by an intermediate spin-orbit coupled Hamiltonian, and the ground state is a well-isolated Kramers doublet with an anisotropic $g$-tensor. We provide the approximate wavefunctions for this doublet, which we expect will be useful in theoretical investigations of the anisotropic exchange interactions.

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

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

Magnetic exchange interactions in the van der Waals layered antiferromagnet MnPSe3

Two-dimensional van der Waals compounds with magnetic ions on a honeycomb lattice are hosts to a variety of exotic behavior. The magnetic interactions in one such compound, MnPSe$_3$, are investigated with elastic and inelastic neutron scattering. Magnetic excitations are observed in the magnetically ordered regime and persist to temperatures well above the ordering temperature, $\rm T_N$ = 74 K, consistent with low dimensional magnetic interactions. The inelastic neutron scattering results allow a model spin Hamiltonian to be presented that includes dominant intralayer interactions of $J_{1ab}$=0.45 meV, $J_{2ab}$=0.03 meV, $J_{3ab}$=0.19 meV, and appreciable interlayer interactions of $J_c$=0.031(5) meV. No evidence for anisotropy in the form of a spin-gap is observed in the data collected. The measurements on MnPSe$_3$ are contrasted with those on MnPS$_3$ and reveal a large increase in the interlayer exchange interactions in MnPSe$_3$, despite the quasi-2D magnetic behavior.

cond-mat.str-el↗