arXiv subjects

Alexander A. Tsirlin

Publications and source records attributed to Alexander A. Tsirlin.

At least 37 records · Page 2Linked to original sources

arXiv2025

Pressure-induced strange metal phase in a metallic kagome ferromagnet

Strange metallicity with $T$-linear electrical resistance preceding high-$T_c$ superconductivity remains an enigmatic, yet crucial, signature of correlation physics. Using electrical transport and magnetization measurements up to 50 GPa, we show that such a strange-metal phase is formed in pressurized kagome ferromagnet CrNiAs. In contrast to other kagome materials, a linear suppression of the Curie temperature is found, with the ferromagnetic quantum critical point at $p_{\rm{c}} \approx 12.5$ GPa. Remarkably, from $p_{\rm{c}}$ up to the highest measured pressure, characteristic strange-metal behavior is observed, whereas magnetic field reinstates the Fermi liquid. Electronic structure calculations reveal robust weakly dispersive bands persisting unchanged beyond $p_{\rm{c}}$, possibly at the origin of the $T$-linear electrical resistance. This establishes pressurized kagome ferromagnets as an intriguing platform for strange-metal behavior.

cond-mat.str-el↗

arXiv2025

High-pressure modulation of breathing kagome lattice: Cascade of Lifshitz transitions and evolution of the electronic structure

The interplay between electronic correlations, density wave orders, and magnetism gives rise to several fascinating phenomena. In recent years, kagome metals have emerged as an excellent platform for investigating these unique properties, which stem from their itinerant carriers arranged in a kagome lattice. Here, we show that electronic structure of the prototypical kagome metal, Fe$_3$Sn$_2$, can be tailored by manipulating the breathing distortion of its kagome lattice with external pressure. The breathing distortion is suppressed around 15 GPa and reversed at higher pressures. These changes lead to a series of Lifshitz transitions that we detect using broadband and transient optical spectroscopy. Remarkably, the strength of the electronic correlations and the tendency to carrier localization are enhanced as the kagome network becomes more regular, suggesting that breathing distortion can be a unique control parameter for the microscopic regime of the kagome metals and their electron dynamics.

cond-mat.str-el↗

arXiv2025

Pressure-dependent magnetism of the Kitaev candidate Li$_2$RhO$_3$

We use magnetization measurements under pressure along with \textit{ab initio} and cluster many-body calculations to investigate magnetism of the Kitaev candidate Li$_2$RhO$_3$. Hydrostatic compression leads to a decrease in the magnitude of the nearest-neighbor ferromagnetic Kitaev coupling $K_1$ and the corresponding increase in the off-diagonal anisotropy $Γ_1$, whereas the experimental Curie-Weiss temperature changes from negative to positive with the slope of +40~K/GPa. On the other hand, spin freezing persists up to at least 3.46~GPa with the almost constant freezing temperature of 5~K that does not follow the large changes in the exchange couplings and indicates the likely extrinsic origin of spin freezing. Magnetic frustration in Li$_2$RhO$_3$ is mainly related to the interplay between ferromagnetic $K_1$ and antiferromagnetic $Γ_1$, along with the weakness of the third-neighbor coupling $J_3$ that would otherwise stabilize zigzag order. The small $J_3$ distinguishes Li$_2$RhO$_3$ from other Kitaev candidates.

cond-mat.str-el↗

arXiv2024

Tunable Dirac nodal line in orthorhombic RuO$_2$

Pressure evolution of RuO2 is studied using single-crystal x-ray diffraction in a diamond anvil cell, combined with \textit{ab initio} band-structure calculations. The tetragonal rutile structure transforms into the orthorhombic CaCl$_2$-type structure above 13 GPa under quasi-hydrostatic pressure conditions. This second-order transition is ferroelastic in nature and accompanied by tilts of the RuO$_6$ octahedra. Orthorhombic RuO$_2$ is expected to be paramagnetic metal, similar to ambient-pressure RuO$_2$. It shows the increased $t_{2g}-e_g$ crystal-field splitting that is responsible for the pressure-induced color change. It further features the Dirac nodal line that shifts across the Fermi level upon compression.

cond-mat.mtrl-sci↗

arXiv2024

Intermediate field-induced phase of the honeycomb magnet BaCo$_2$(AsO$_4$)$_2$

We use magnetometry, calorimetry, and high-resolution capacitive dilatometry, as well as single-crystal neutron diffraction to explore temperature-field phase diagram of the anisotropic honeycomb magnet BaCo$_2$(AsO$_4)_2$. Our data reveal four distinct ordered states observed for in-plane magnetic fields. Of particular interest is the narrow region between 0.51 and 0.55 T that separates the up-up-down order from the fully polarized state and coincides with the field range where signatures of the spin-liquid behavior have been reported. We show that magnetic Bragg peaks persist in this intermediate phase, thus ruling out its spin-liquid nature. However, the simultaneous nonmonotonic evolution of nuclear Bragg peaks suggests the involvement of the lattice, witnessed also in other regions of the phase diagram where large changes in the sample length are observed upon entering the magnetically ordered states. Our data highlight the importance of lattice effects in BaCo$_2$(AsO$_4)_2$.

cond-mat.str-el↗

arXiv2024

Kitaev Interactions Through an Extended Superexchange Pathway in the jeff = 1/2 Ru3+ Honeycomb Magnet, RuP3SiO11

Magnetic materials are composed of the simple building blocks of magnetic moments on a crystal lattice that interact via magnetic exchange. Yet from this simplicity emerges a remarkable diversity of magnetic states. Some reveal the deep quantum mechanical origins of magnetism, for example, quantum spin liquid (QSL) states in which magnetic moments remain disordered at low temperatures despite being strongly correlated through quantum entanglement. A promising theoretical model of a QSL is the Kitaev model, composed of unusual bond-dependent exchange interactions, but experimentally, this model is challenging to realise. Here we show that the material requirements for the Kitaev QSL survive an extended pseudo-edge-sharing superexchange pathway of Ru3+ octahedra within the honeycomb layers of the inorganic framework solid, RuP3SiO11. We confirm the requisite jeff = 1/2 state of Ru3+ in RuP3SiO11 and resolve the hierarchy of exchange interactions that provide experimental access to an unexplored region of the Kitaev model.

cond-mat.str-el↗

arXiv2024

Fermi-liquid behavior of non-altermagnetic RuO$_2$

Presence of magnetism in potentially altermagnetic RuO$_2$ has been a subject of intense debate. Using broadband infrared spectroscopy combined with density-functional band-structure calculations, we show that optical conductivity of RuO$_2$, the bulk probe of its electronic structure, is well described by the nonmagnetic model of this material. The sharp Pauli edge demonstrates the presence of a Dirac nodal line lying 45 meV below the Fermi level. Good match between the experimental and ab initio plasma frequencies underpins weakness of electronic correlations. The intraband part of the optical conductivity indicates Fermi-liquid behavior with two distinct scattering rates below 150 K. Fermi-liquid theory also accounts for the temperature-dependent magnetic susceptibility of RuO$_2$ and allows a consistent description of this material as paramagnetic metal.

cond-mat.mtrl-sci↗

arXiv2024

Magnetic versus nonmagnetic polymorphs of RuBr$_3$ under pressure

Pressure evolution of the crystal structure and magnetism of the honeycomb $α$-RuBr$_3$ is studied using high-pressure x-ray diffraction, magnetometry, and density-functional band-structure calculations. Hydrostatic compression transforms antiferromagnetic $α$-RuBr$_3$ ($R\bar 3$) into paramagnetic $α'$-RuBr$_3$ ($P\bar 1$) where short Ru-Ru bonds cause magnetism collapse above 1.3 GPa at 0 K and 2.5 GPa at 295 K. Below this critical pressure, the Néel temperature of $α$-RuBr$_3$ increases with the slope of 1.8 K/GPa. Pressure tunes $α$-RuBr$_3$ away from the Kitaev limit, whereas increased third-neighbor in-plane coupling and interlayer coupling lead to a further stabilization of the collinear zigzag state. Both $α$- and $α'$-RuBr$_3$ are metastable at ambient pressure, but their transformation into the thermodynamically stable $β$-polymorph is kinetically hindered at room temperature.

cond-mat.str-el↗

arXiv2023

Frustration relief and reorientation transition in the kagome-like dolerophanite Cu$_2$OSO$_4$

We present a theoretical study of dolerophanite Cu$_2$OSO$_4$, a layered kagome-like spin-$\frac{1}{2}$ magnetic insulator that can be described either as a system of chains coupled through dimers or as a kagome lattice where every third spin is replaced by a ferromagnetic spin dimer. Building on insights from ab initio calculations, classical numerical minimizations, and semiclassical expansions, we arrive at a minimal microscopic description that accounts for the experimental data reported so far, including the nature of the magnetic order, the reported spin length, and the observed anisotropy. The latter arises by a peculiar competition between the antisymmetric (Dzyaloshinskii-Moriya) and the symmetric part of the exchange anisotropy, which gives rise to a two-step re-orientation process involving two successive continuous phase transitions. Our work uncovers mechanisms stabilizing canted ferrimagnetic order in kagome systems, and highlights strong magnetic anisotropy in the presence if dissimilar magnetic orbitals on crystallographically nonequivalent Cu sites. We also show how these anisotropy terms affect the spin-wave spectrum and how they can be tracked experimentally.

cond-mat.str-el↗

arXiv2023

Pressure evolution of electron dynamics in the superconducting kagome metal CsV$_3$Sb$_5$

The coexistence of the charge-density wave (CDW) and superconducting phases and their tunability under external pressure remains one of the key points in understanding the electronic structure of $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) kagome metals. Here, we employ synchrotron-based infrared spectroscopy assisted by density-functional calculations to study the pressure evolution of the electronic structure at room temperature up to 17 GPa experimentally. The optical spectrum of CsV$_3$Sb$_5$ is characterized by the presence of localized carriers seen as a broad peak at finite frequencies in addition to the conventional metallic Drude response. The pressure dependence of this low-energy peak reflects the re-entrant behavior of superconductivity and may be interpreted in terms of electron-phonon coupling, varying with the growth and shrinkage of the Fermi surface. Moreover, drastic modifications in the low-energy interband absorptions are observed upon the suppression of CDW. These changes are related to the upward shift of the Sb2 $p_x+p_y$ band that eliminates part of the Fermi surface around the $M$-point, whereas band saddle points do not move significantly. These observations shed new light on the mixed electronic and lattice origin of the CDW in CsV$_3$Sb$_5$.

cond-mat.str-el↗

arXiv2023

Geometrical frustration and incommensurate magnetic order in Na$_3$RuO$_4$ with two triangular motifs

Incommensurate magnetic order in the spin-3/2 antiferromagnet Na$_3$RuO$_4$ is uncovered by neutron diffraction combined with ab initio calculations. The crystal structure of Na$_3$RuO$_4$ contains two triangular motifs on different length scales. The magnetic Ru$^{5+}$ ions form a lozenge (diamond) configuration, with tetramers composed of two isosceles triangles. These tetramers are further arranged in layers, such that an effective triangular lattice is formed. The tetramers are nearly antiferromagnetic but frustration between them leads to an incommensurately modulated magnetic structure described by the propagation vector $\vec{k}=(0.242(1), 0, 0.313(1))$. We show that the long-range Ru-O-O-Ru couplings between the tetramers play a major role in Na$_3$RuO$_4$ and suggest an effective description in terms of the spatially anisotropic triangular lattice if the tetramers are treated as single sites.

cond-mat.str-el↗

arXiv2023

Role of alkaline metal in the rare-earth triangular antiferromagnet KYbO$_2$

We report crystal structure and magnetic behavior of the triangular antiferromagnet KYbO$_2$, the A-site substituted version of the quantum spin liquid candidate NaYbO$_2$. The replacement of Na by K introduces an anisotropic tensile strain with 1.6% in-plane and 12.1% out-of-plane lattice expansion. Compared to NaYbO$_2$, both Curie-Weiss temperature and saturation field are reduced by about 20% as the result of the increased Yb--O--Yb angles, whereas the $g$-tensor of Yb$^{3+}$ becomes isotropic with $g=3.08(3)$. Field-dependent magnetization shows the plateau at 1/2 of the saturated value and suggests the formation of the up-up-up-down field-induced order in the triangular AYbO$_2$ oxides (A = alkali metal), in contrast to the isostructural selenides that exhibit the 1/3 plateau and the up-up-down field-induced order.

cond-mat.str-el↗

arXiv2023

Effect of nonhydrostatic pressure on the superconducting kagome metal CsV$_3$Sb$_5$

High-pressure single-crystal x-ray diffraction experiments reveal that the superconducting kagome metal CsV$_3$Sb$_5$ transforms from hexagonal ($P6/mmm$) to monoclinic ($C2/m$) symmetry above 10 GPa if nonhydrostatic pressure conditions are created in a diamond anvil cell with silicon oil as pressure-transmitting medium. This is contrary to the behavior of CsV$_3$Sb$_5$ under quasi-hydrostatic conditions in neon, with the hexagonal symmetry retained up to at least 20 GPa. Monoclinic distortion leaves the kagome planes almost unchanged but deforms honeycomb nets of the Sb atoms. While the onset of the distortion almost coincides with the reentrance of superconductivity, our \textit{ab initio} density-functional calculations reveal only minor changes in the electronic structure compared to the quasi-hydrostatic case. In particular, Fermi surface reconstruction driven by the formation of interlayer Sb-Sb bonds is observed in both monoclinic and hexagonal CsV$_3$Sb$_5$ structures at high pressures and comes out as the likely cause for the reentrant behavior.

cond-mat.supr-con↗

arXiv2023

One-dimensional magnetism in synthetic Pauflerite, $β$-VOSO$_4$

We have synthesized single-crystal samples of $β$-VOSO$_4$ and fully characterized their magnetic properties. Our magnetic susceptibility, high field magnetization and powder inelastic neutron scattering results are in excellent agreement with theoretical expressions for a one-dimensional spin-1/2 Heisenberg chain with an exchange parameter of $3.83(2)$ meV. Ab initio calculations identify the superexchange pathway, revealing that the spin-chain does not run along the expected crystallographic chain $a$ direction but instead between V$^{4+}$O$_{6}$ octahedra that are linked via SO$_{4}$ tetrahedra along the $b$ axis. We do not detect any phase transition to a long-range magnetic order within our experimental conditions, indicating $β$-VOSO$_4$ is very close to an ideal one-dimensional magnetic system.

cond-mat.str-el↗

arXiv2023

Frustration on a centred pyrochlore lattice in metal-organic frameworks

Geometric frustration inhibits magnetic systems from ordering, opening a window to unconventional phases of matter. The paradigmatic frustrated lattice in three dimensions to host a spin liquid is the pyrochlore, although there remain few experimental compounds thought to realize such a state. Here we go beyond the pyrochlore via molecular design in the metal-azolate framework [Mn(II)(ta)$_2$], which realizes a closely related centred pyrochlore lattice of Mn-spins with $S=5/2$. Despite a Curie-Weiss temperature of $-21$ K indicating the energy scale of magnetic interactions, [Mn(II)(ta)$_2$] orders at only 430 mK, putting it firmly in the category of highly frustrated magnets. Comparing magnetization and specific heat measurements to numerical results for a minimal Heisenberg model, we predict that this material displays distinct features of a classical spin liquid with a structure factor reflecting Coulomb physics in the presence of charges.

cond-mat.str-el↗

arXiv2022

Effect of antifluorite layer on the magnetic order in Eu-based 1111 compounds, EuTAsF (T = Zn, Mn, and Fe)

The 1111 compounds with an alternating sequence of fluorite and antifluorite layers serve as structural hosts for the vast family of Fe-based superconductors. Here, we use neutron powder diffraction and density-functional-theory (DFT) band-structure calculations to study magnetic order of Eu2+ in the [EuF]+ fluorite layers depending on the nature of the [TAs]- antifluorite layer that can be non-magnetic semiconducting (T = Zn), magnetic semiconducting (T = Mn), or magnetic metallic (T = Fe). Antiferromagnetic transitions at TN ~ 2.4 - 3 K due to an ordering of the Eu2+ magnetic moments were confirmed in all three EuTAsF compounds. Whereas in EuTAsF (T = Zn and Mn), the commensurate k1 = (1/2 1/2 0) stripe order pattern with magnetic moments within the ab-plane is observed, the order in EuFeAsF is incommensurate with k = (0 0.961(1) 1/2) and represents a cycloid of Eu2+ magnetic moments confined within the bc-plane. Additionally, the Mn2+ sublattice in EuMnAsF features a robust G-type antiferromagnetic order that persists at least up to room temperature, with magnetic moments along the c-direction. Although DFT calculations suggest stripe antiferromagnetic order in the Fe-sublattice of EuFeAsF as the ground state, neutron diffraction reveals no evidence of long-range magnetic order associated with Fe. We show that the frustrating interplane interaction J3 between the adjacent [EuF]+ layers is comparable with in-plane J1-J2 interactions already in the case of semiconducting fluorite layers [TAs]- (T = Zn and Mn) and becomes dominant in the case of the metallic [FeAs]- ones. The latter, along with a slight orthorhombic distortion, is proposed to be the origin of the incommensurate magnetic structure observed in EuFeAsF.

cond-mat.str-el↗

arXiv2022

One-Dimensional Quantum Magnetism in the S = 1/2 Mo(V) system, KMoOP2O7

We present a comprehensive experimental and ab-initio study of the $S=1/2$ Mo$^{5+}$ system, KMoOP$_2$O$_7$, and show that it realizes the $S = 1/2$ Heisenberg chain antiferromagnet model. Powder neutron diffraction reveals that KMoOP$_2$O$_7$ forms a magnetic network comprised of pairs of Mo$^{5+}$ chains within its monoclinic $P2_1/n$ structure. Antiferromagnetic interactions within the Mo$^{5+}$ chains are identified through magnetometry measurements and confirmed by analysis of the magnetic specific heat. The latter reveals a broad feature centred on $T_\textrm{N} = 0.54$ K, which we ascribe to the onset of long-range antiferromagnetic order. No magnetic Bragg scattering is observed in powder neutron diffraction data collected at 0.05 K, however, which is consistent with a strongly suppressed ordered moment with an upper limit $μ_\textrm{ord} < 0.15 μ_\textrm{B}$. The one-dimensional character of the magnetic correlations in KMoOP$_2$O$_7$ is verified through analysis of inelastic neutron scattering data, resulting in a model with $J_\textrm{1} \approx 34$ K and $J_\textrm{2} \approx -2$ K for the intrachain and interchain exchange interactions, respectively. The origin of these experimental findings are addressed through density-functional theory calculations.

cond-mat.str-el↗

arXiv2022

Deformation of the triangular spin-$\frac{1}{2}$ lattice in Na$_2$SrCo(PO$_4$)$_2$

Crystal structure and thermodynamic properties of Na$_2$SrCo(PO$_4$)$_2$, the chemical sibling of the triangular quantum spin-liquid candidate Na$_2$BaCo(PO$_4$)$_2$, are reported. From single crystal x-ray diffraction and high-resolution synchrotron x-ray powder diffraction, the compound was found to crystallize in the monoclinic space group $P2_1/a$ at room temperature, in contrast to the trigonal Na$_2$BaCo(PO$_4$)$_2$. Above 650 K, the symmetry of Na$_2$SrCo(PO$_4$)$_2$ changes to $C2/m$, while around 1025 K a further transformation toward trigonal symmetry is observed. The monoclinic symmetry leads to a small deformation of the CoO$_6$ octahedra beyond the trigonal distortion ubiquitous in this structure type, and results in the stronger $g$-tensor anisotropy ($g_{\text{z}}/g_{\text{xy}} = 1.6 $) as well as the increased XXZ anisotropy ($J_{\text{z}}/J_{\text{xy}} = 2.1$) compared to the Ba compound ($g_{\text{z}}/g_{\text{xy}} = 1.1 $, $J_{\text{z}}/J_{\text{xy}} = 1.5$), while the average coupling strength, $J_{\text{av}}/k_{\text{B}}=(2J_{\text{xy}}+J_{\text{z}})/3k_\text{B}\simeq 1.3\,\text{K}$, remains unchanged. The Néel temperature increases from 140 mK (Ba) to 600 mK (Sr), and an uncompensated in-plane moment of $0.066(4)μ_{\text{B}}/\text{f.u.}$ appears. We show that the ordering temperature of a triangular antiferromagnet is capably controlled by its structural distortions.

cond-mat.str-el↗