arXiv subjects

Alexander A. Tsirlin

Publications and source records attributed to Alexander A. Tsirlin.

At least 91 records · Page 5Linked to original sources

arXiv2017

Frustrated spin chain physics near the Majumdar-Ghosh point in szenicsite Cu$_3$(MoO$_4$)(OH)$_4$

In this joint experimental and theoretical work magnetic properties of the Cu$^{2+}$ mineral szenicsite Cu$_3$(MoO$_4$)(OH)$_4$ are investigated. This compound features isolated triple chains in its crystal structure, where the central chain involves an edge-sharing geometry of the CuO$_4$ plaquettes, while the two side chains feature a corner-sharing zig-zag geometry. The magnetism of the side chains can be described in terms of antiferromagnetic dimers with a coupling larger than 200 K. The central chain was found to be a realization of the frustrated antiferromagnetic $J_1$-$J_2$ chain model with $J_1\simeq 68$ K and a sizable second-neighbor coupling $J_2$. The central and side chains are nearly decoupled owing to interchain frustration. Therefore, the low-temperature behavior of szenicsite should be entirely determined by the physics of the central frustrated $J_1$-$J_2$ chain. Our heat-capacity measurements reveal an accumulation of entropy at low temperatures and suggest a proximity of the system to the Majumdar-Ghosh point of the antiferromagnetic $J_1$-$J_2$ spin chain, $J_2/J_1=0.5$.

cond-mat.str-el↗

arXiv2017

Crystalline Electric Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO$_4$

We apply moderate-high-energy inelastic neutron scattering (INS) measurements to investigate Yb$^{3+}$ crystalline electric field (CEF) levels in the triangular spin-liquid candidate YbMgGaO$_4$. Three CEF excitations from the ground-state Kramers doublet are centered at the energies $\hbar ω$ = 39, 61, and 97\,meV in agreement with the effective \mbox{spin-1/2} $g$-factors and experimental heat capacity, but reveal sizable broadening. We argue that this broadening originates from the site mixing between Mg$^{2+}$ and Ga$^{3+}$ giving rise to a distribution of Yb--O distances and orientations and, thus, of CEF parameters that account for the peculiar energy profile of the CEF excitations. The CEF randomness gives rise to a distribution of the effective spin-1/2 $g$-factors and explains the unprecedented broadening of low-energy magnetic excitations in the fully polarized ferromagnetic phase of YbMgGaO$_4$, although a distribution of magnetic couplings due to the Mg/Ga disorder may be important as well.

cond-mat.str-el↗

arXiv2016

Antiferroelectric instability in kagome francisites Cu$_3$Bi(SeO$_3$)$_2$O$_2$X (X = Cl, Br)

Density-functional calculations of lattice dynamics and high-resolution synchrotron powder diffraction uncover antiferroelectric distortion in the kagome francisite Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl below 115K. Its Br-containing analogue is stable in the room-temperature crystal structure down to at least 10K, although the Br compound is on the verge of a similar antiferroelectric instability and reveals local displacements of Cu and Br atoms. The I-containing compound is stable in its room-temperature structure according to density-functional calculations. We show that the distortion involves cooperative displacements of Cu and Cl atoms, and originates from the optimization of interatomic distances for weakly bonded halogen atoms. The distortion introduces a tangible deformation of the kagome spin lattice and may be responsible for the reduced net magnetization of the Cl compound compared to the Br one. The polar structure of Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl is only slightly higher in energy than the non-polar antiferroelectric structure, but no convincing evidence of its formation could be obtained.

cond-mat.mtrl-sci↗

arXiv2016

$μ$SR evidence for the U(1) quantum spin liquid ground state in the triangular antiferromagnet YbMgGaO$_4$

Muon spin relaxation and rotation ($μ$SR) experiments on single crystals of the structurally perfect triangular antiferromagnet YbMgGaO$_4$ indicate the absence of both static long-range magnetic order and spin freezing down to 0.048 K in zero field. Below 0.4 K, the $μ^{+}$ spin relaxation rates, which are proportional to the dynamic correlation function of the Yb$^{3+}$ spins,exhibit temperature-independent plateaus. Same behavior is revealed by temperature-independent local susceptibilities extracted from the Knight shifts of the $μ^{+}$ spin rotation frequencies under a transverse field of 20 Oe. All these $μ$SR results unequivocally support the formation of a gapless U(1) quantum spin liquid ground state in the triangular antiferromagnet YbMgGaO$_4$.

cond-mat.str-el↗

arXiv2016

Ternary borides Nb$_7$Fe$_3$B$_8$ and Ta$_7$Fe$_3$B$_8$ with Kagome-type iron framework

Two new ternary borides $TM$$_7$Fe$_3$B$_8$ ($TM$ = Nb, Ta) were synthesized by high-temperature thermal treatment of samples obtained by arc-melting. This new type of structure with space group $P$6/$mmm$, comprises $TM$ slabs containing isolated planar hexagonal [B$_6$] rings and iron centered $TM$ columns in a Kagome type of arrangement. Chemical bonding analysis in Nb$_7$Fe$_3$B$_8$ by means of the electron localizability approach reveals two-center interactions forming the Kagome net of Fe and embedded B, while weaker multicenter bonding present between this net and Nb atoms. Magnetic susceptibility measurements reveal antiferromagnetic order below $T_N$ = 240 K for Nb$_7$Fe$_3$B$_8$ and $T_N$ =265 K for Ta$_7$Fe$_3$B$_8$. Small remnant magnetization below 0.01 $μ_B$/f.u. is observed in the antiferromagnetic state. The bulk nature of the magnetic transitions was confirmed by the hyperfine splitting of the Mößbauer spectra, the sizable anomalies in the specific heat capacity, and the kinks in the resistivity curves. The high-field paramagnetic susceptibilities fitted by the Curie-Weiss law show effective paramagnetic moments $μ_{eff}$ about 3.1 $μ_B$/Fe in both compounds. The temperature dependence of the electrical resistivity also reveals metallic character of both compounds. Density functional calculations corroborate the metallic behaviour of both compounds and demonstrate the formation of a sizable local magnetic moment on the Fe-sites. They indicate the presence of both antiferro- and ferromagnetic interactions.

cond-mat.mtrl-sci↗

arXiv2016

Hydration induced spin glass state in a frustrated Na-Mn-O triangular lattice

Birnessite compounds are stable across a wide range of compositions that produces a remarkable diversity in their physical, electrochemical and functional properties. These are hydrated analogues of the magnetically frustrated, mixed-valent manganese oxide structures, with general formula, NaxMnO2. Here we demonstrate that the direct hydration of layered rock-salt type a-NaMnO2, with the geometrically frustrated triangular lattice topology, yields the birnessite type oxide, Na0.36MnO2 0.2H2O, transforming its magnetic properties. This compound has a much-expanded interlayer spacing compared to its parent a-NaMnO2 compound. We show that while the parent a-NaMnO2 possesses a Neel temperature of 45 K as a result of broken symmetry in the Mn3+ sub-lattice, the hydrated derivative undergoes collective spin-freezing at 29 K within the Mn3+/Mn4+ sub-lattice. Scaling-law analysis of the frequency dispersion of the AC susceptibility, as well as the temperature-dependent, low-field DC magnetization confirm a cooperative spin-glass state of strongly interacting spins. This is supported by complementary spectroscopic analysis (HAADF-STEM, EDS, EELS) as well as by a structural investigation (high-resolution TEM, X-ray and neutron powder diffraction) that yield insights into the chemical and atomic structure modifications. We conclude that the spin-glass state in birnessite is driven by the spin-frustration imposed by the underlying triangular lattice topology that is further enhanced by the in-plane bond-disorder generated by the mixed-valent character of manganese in the layers.

cond-mat.mtrl-sci↗

arXiv2015

Strong electron-phonon coupling in the intermetallic superconductor Mo$_{8}$Ga$_{41}$

Crystals of superconducting Mo$_{8}$Ga$_{41}$ ($T_{\text{c}}=9.8$ K) and Mo$_{\text{8-x}}$V$_{\text{x}}$Ga$_{41}$ limited solid solution $(x_{\text{max}}=1.9(2))$ have been grown from the high-temperature Ga flux and confirmed to have the V$_{8}$Ga$_{41}$ type of crystal structure at room temperature. Thermodynamic and transport measurements as well as electronic structure calculations were performed to investigate both normal- and superconducting-state properties of Mo$_{8}$Ga$_{41}$. The discontinuity in the heat capacity at $T_{\text{c}}$, $Δc_{\text{p}}/γ_{\text{N}}T_{\text{c}}=2.83$ in zero magnetic field, indicates a much stronger electron-phonon coupling than in the standard BCS limit. From the heat capacity data, we estimated the electron-phonon coupling constant $λ_{\text{ep}}=0.9$. The upper critical field is $μ_{0}H_{\text{c2}}(0)=8.3$ T, while the lower one is only $μ_{0}H_{\text{c1}}(0)=131$ Oe. The upper critical field of Mo$_{8}$Ga$_{41}$ exhibits a clear enhancement with respect to the Werthamer-Helfand-Honenberg prediction, consistent with the strong electron-phonon coupling. The Mo$_{\text{8-x}}$V$_{\text{x}}$Ga$_{41}$ limited solid solution also exhibits superconducting properties, and the critical temperature $T_{\text{c}}$ is reduced only slightly with increasing $x$.

cond-mat.supr-con↗

arXiv2014

Frustration and Dzyaloshinsky-Moriya anisotropy in the kagome francisites Cu$_3$Bi(SeO$_3)_2$O$_2$X

We investigate the antiferromagnetic canting instability of the spin-1/2 kagome ferromagnet, as realized in the layered cuprates Cu$_3$Bi(SeO$_3)_2$O$_2$X (X=Br, Cl, and I). While the local canting can be explained in terms of competing exchange interactions, the direction of the ferrimagnetic order parameter fluctuates strongly even at short distances on account of frustration which gives rise to an infinite ground state degeneracy at the classical level. In analogy with the kagome antiferromagnet, the accidental degeneracy is fully lifted only by non-linear 1/S corrections, rendering the selected uniform canted phase very fragile even for spins-1/2, as shown explicitly by coupled-cluster calculations. To account for the observed ordering, we show that the minimal description of these systems must include the microscopic Dzyaloshinsky-Moriya interactions, which we obtain from density-functional band-structure calculations. The model explains all qualitative properties of the kagome francisites, including the detailed nature of the ground state and the anisotropic response under a magnetic field. The predicted magnon excitation spectrum and quantitative features of the magnetization process call for further experimental investigations of these compounds.

cond-mat.str-el↗

arXiv2014

Novel non-magnetic hard boride Co5B16 synthesized under high pressure

A first cobalt boride with the Co:B ratio below 1:1, Co5B16, was synthesized under high-pressure high-temperature conditions. It has a unique orthorhombic structure (space group Pmma, a = 19.1736(12), b = 2.9329(1), and c = 5.4886(2) Å, R1 (all data) = 0.037). The material is hard, paramagnetic, with a weak temperature dependence of magnetic susceptibility.

cond-mat.mtrl-sci↗

arXiv2014

Nearly compensated exchange in the dimer compound callaghanite Cu$_2$Mg$_2$(CO$_3$)(OH)$_6$$\cdot$2H$_2$O

A combined theoretical and experimental study of the natural Cu(2+)-mineral callaghanite is presented. Its crystal structure features well separated Cu$_2$(OH)$_6$ structural dimers with weakly bonded carbonate groups and water molecules in between. Susceptibility, field-dependent magnetization and specific heat measurements reveal a compound with a small spin gap of about 7 K. The observed magnetic properties are well described by a model of isolated antiferromagnetic spin dimers. Possible ferromagnetic interactions between the dimers amount to -1.5 K, at most. Different flavors of electronic structure calculations have been employed to locate the magnetic dimers in the crystal structure, i.e., to determine whether they coincide with the structural dimers or not. Calculations of the coupling between the structural dimers clearly show that magnetic and structural dimers are the same. For the intradimer coupling, however, the computational results confirmed a coupling strength close to zero but the sign of the coupling could not be determined unambiguously. Based on this finding, we then discuss how the reliability of the numerical methods depends on the characteristics of exchange pathways and on structural features of the compound in general. Eventually, we try to provide a minimum coupling strength that is needed for a reliable computational description.

cond-mat.str-el↗

arXiv2014

Spin-chain magnetism and uniform Dzyaloshinsky-Moriya anisotropy in BaV$_3$O$_8$

We report on the microscopic magnetic model of a spin-1/2 magnet BaV$_3$O$_8$. In contrast to earlier phenomenological analysis, our density-functional band-structure calculations combined with quantum Monte-Carlo simulations establish a relatively simple and non-frustrated model of weakly coupled spin chains with the intrachain coupling of $J\sim$ 38 K and the Neel temperature of $T_N\sim$ 6 K, both in excellent agreement with the experiment. The intrachain coupling between the spin-1/2 V$^{+4}$ ions takes place via two contiguous V$^{+5}$O$_4$ tetrahedra forming an extended superexchange pathway with the V$^{+4}$--V$^{+4}$ distance of 7.44 A. Surprisingly, this pathway is preferred over shorter V$^{+4}$--V$^{+4}$ connections, owing to peculiarities in the interacting orbitals of the magnetic V$^{+4}$ ions and V$^{+5}$ ions that are non-magnetic, but feature low-lying $3d$ states contributing to the superexchange process. We also note that the crystal structure of BaV$_3$O$_8$ supports the long-sought uniform arrangement of Dzyaloshinsky-Moriya (DM) couplings on a spin-1/2 chain. While our calculations yield only a weak DM anisotropy in BaV$_3$O$_8$, the crystal structure of this compound provides a suitable framework for the search of spin chains with the uniform DM anisotropy in other compounds of the vanadate family.

cond-mat.mtrl-sci↗

arXiv2013

Peierls distortion, magnetism, and high hardness of manganese tetraboride

We report crystal structure, electronic structure, and magnetism of manganese tetraboride, MnB4, synthesized under high-pressure high-temperature conditions. In contrast to superconducting FeB4 and metallic CrB4, which are both orthorhombic, MnB4 features a monoclinic crystal structure. Its lower symmetry originates from a Peierls distortion of the Mn chains. This distortion nearly opens the gap at the Fermi level, but despite the strong dimerization and the proximity of MnB4 to the insulating state, we find indications for a sizable paramagnetic effective moment of about 1.7 muB/f.u., ferromagnetic spin correlations and, even more surprisingly, a prominent electronic contribution to the specific heat. However, no magnetic order has been observed in standard thermodynamic measurements down to 2 K. Altogether, this renders MnB4 a structurally simple but microscopically enigmatic material; we argue that its properties may be influenced by electronic correlations.

cond-mat.mtrl-sci↗

arXiv2013

Magnetic frustration in BaCuSi2O6 released

Han Purple (BaCuSi2O6) is not only an ancient pigment, but also a valuable model material for studying Bose-Einstein condensation (BEC) of magnons in high magnetic fields. Using precise low-temperature structural data and extensive density-functional calculations, we elucidate magnetic couplings in this compound. The resulting magnetic model comprises two types of nonequivalent spin dimers, in excellent agreement with the (63,65)Cu nuclear magnetic resonance data. We further argue that leading interdimer couplings connect the upper site of one dimer to the bottom site of the contiguous dimer, and not the upper-to-upper and bottom-to-bottom sites, as assumed previously. This finding is verified by inelastic neutron scattering data and implies the lack of magnetic frustration in BaCuSi2O6, thus challenging existing theories of the magnon BEC in this compound.

cond-mat.mtrl-sci↗

arXiv2013

The spin gap in malachite Cu2(OH)2CO3 and its evolution under pressure

We report on the microscopic magnetic modeling of the spin-1/2 copper mineral malachite at ambient and elevated pressures. Despite the layered crystal structure of this mineral, the ambient-pressure susceptibility and magnetization data can be well described by an unfrustrated quasi-one-dimensional magnetic model. Weakly interacting antiferromagnetic alternating spin chains are responsible for a large spin gap of 120K. Although the intradimer Cu-O-Cu bridging angles are considerably smaller than the interdimer angles, density functional theory (DFT) calculations revealed that the largest exchange coupling of 190K operates within the structural dimers. The lack of the inversion symmetry in the exchange pathways gives rise to sizable Dzyaloshinskii-Moriya interactions which were estimated by full-relativistic DFT+U calculations. Based on available high-pressure crystal structures, we investigate the exchange couplings under pressure and make predictions for the evolution of the spin gap. The calculations evidence that intradimer couplings are strongly pressure-dependent and their evolution underlies the decrease of the spin gap under pressure. Finally, we assess the accuracy of hydrogen positions determined by structural relaxation within DFT and put forward this computational method as a viable alternative to elaborate experiments.

cond-mat.str-el↗

arXiv2013

Low-temperature phase diagram of Fe1+yTe

We used low-temperature synchrotron x-ray diffraction to investigate the structural phase transitions of Fe1+yTe in the vicinity of a tricitical point in the phase diagram. Detailed analysis of the powder diffraction patterns and temperature dependence of the peak-widths in Fe1+yTe showed that two-step structural and magnetic phase transitions occur within the compositional range 0.11 $\leq y \leq $ 0.13. The phase transitions are sluggish indicating a strong competition between the orthorhombic and the monoclinic phases. We combine high-resolution diffraction experiments with specific heat, resistivity, and magnetization measurements and present a revised temperature-composition phase diagram for Fe1+yTe.

cond-mat.supr-con↗

arXiv2013

Discovery of a superhard iron tetraboride superconductor

Single crystals of novel orthorhombic (space group Pnnm) iron tetraboride FeB4 were synthesised at pressures above 8 GPa and high temperatures. Magnetic susceptibility measurements demonstrated bulk superconductivity below 2.9 K. The putative isotope effect on the superconducting critical temperature indicates that FeB4 is likely a phonon-mediated superconductor, which is unexpected in the light of previous knowledge on Fe-based superconductors. The discovered iron tetraboride is highly incompressible and has the nanoindentation hardness of 65(5) GPa, thus, it opens a new class of highly desirable materials combining advanced mechanical properties and superconductivity.

cond-mat.mtrl-sci↗

arXiv2013

Two energy scales of spin dimers in clinoclase Cu3(AsO4)(OH)3

Magnetic susceptibility and microscopic magnetic model of the mineral clinoclase Cu3(AsO4)(OH)3 are reported. This material can be well described as a combination of two nonequivalent spin dimers with the sizable magnetic couplings of J about 700 K and J(D2) about 300 K. Based on density functional theory calculations, we pinpoint the location of dimers in the crystal structure. Surprisingly, the largest coupling operates between the structural Cu2O6 dimers. We investigate magnetostructural correlations in Cu2O6 structural dimers, by considering the influence of the hydrogen position on the magnetic coupling. Additionally, we establish the hydrogen positions that were not known so far and analyze the pattern of hydrogen bonding.

cond-mat.str-el↗

arXiv2013

Square-lattice magnetism of diaboleite Pb2Cu(OH)4Cl2

We report on the quasi-two-dimensional magnetism of the natural mineral diaboleite Pb2Cu(OH)4Cl2 with a tetragonal crystal structure, which is closely related to that of the frustrated spin-1/2 magnet PbVO3. Magnetic susceptibility of diaboleite is well described by a Heisenberg spin model on a diluted square lattice with the nearest-neighbor exchange of J~35 K and about 5% of non-magnetic impurities. The dilution of the spin lattice reflects the formation of Cu vacancies that are tolerated by the crystal structure of diaboleite. The weak coupling between the magnetic planes triggers the long-range antiferromagnetic order below TN~11 K. No evidence of magnetic frustration is found. We also analyze the signatures of the long-range order in heat-capacity data, and discuss the capability of identifying magnetic transitions with heat-capacity measurements.

cond-mat.mtrl-sci↗