Distinct magnetic regimes through site-selective atom substitution in the frustrated quantum antiferromagnet Cs$_2$CuCl$_{4-x}$Br$_x$
P. T. Cong, B. Wolf, M. de Souza, N. Krueger, A. A. Haghighirad, S. Gottlieb- Schoenmeyer, F. Ritter, W. Assmus, I. Opahle, K. Foyevtsova, H. O. Jeschke, R. Val… 展开作者
P. T. Cong, B. Wolf, M. de Souza, N. Krueger, A. A. Haghighirad, S. Gottlieb- Schoenmeyer, F. Ritter, W. Assmus, I. Opahle, K. Foyevtsova, H. O. Jeschke, R. Valenti, L. Wiehl, M. Lang
We report on a systematic study of the magnetic properties on single crystals of the solid solution Cs$_2$CuCl$_{4-x}$Br$_x$ (0 $\leq$ x $\leq$ 4), which include the two known end-member compounds Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$, classified as quasi-two-dimensional quantum antiferromagnets with different degrees of magnetic frustration. By comparative measurements of the magnetic susceptibility $χ$($T$) on as many as eighteen different Br concentrations, we found that the inplane and out-of-plane magnetic correlations, probed by the position and height of a maximum in the magnetic susceptibility, respectively, do not show a smooth variation with x. Instead three distinct concentration regimes can be identified, which are separated by critical concentrations x$_{c1}$ = 1 and x$_{c2}$ = 2. This unusual magnetic behavior can be explained by considering the structural peculiarities of the materials, especially the distorted Cu-halide tetrahedra, which support a site-selective replacement of Cl- by Br- ions. Consequently, the critical concentrations x$_{c1}$ (x$_{c2}$) mark particularly interesting systems, where one (two) halidesublattice positions are fully occupied.
We investigate the electronic and magnetic properties of the frustrated triangular-lattice antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ in the framework of density functional theory. Analysis of the exchange couplings J and J' using the available X-ray structural data corroborates the values obtained from experimental results for Cs$_2$CuBr$_4$ but not for Cs$_2$CuCl$_4$. In order to understand this discrepancy, we perform a detailed study of the effect of structural optimization on the exchange couplings of Cs$_2$CuCl$_4$ employing different exchange-correlation functionals. We find tha…
We report $^{133}$Cs nuclear magnetic resonance (NMR) measurements on the 2D frustrated Heisenberg antiferromagnet Cs$_2$CuCl$_4$ down to 2 K and up to 15 T. We show that $^{133}$Cs NMR is a good probe of the magnetic degrees of freedom in this material. Cu spin degrees of freedom are sensed through a strong anisotropic hyperfine coupling. The spin excitation gap opens above the critical saturation field. The gap value was determined from the activation energy of the nuclear spin-lattice relaxation rate in a magnetic field applied parallel to the Cu chains (b axis). The values of the g-factor …
We report a detailed examination the magnetic structure of anhydrous cupric chloride CuCl2 carried out by powder neutron diffraction, magnetic susceptibility and specific heat measurements on polycrystalline and single crystal samples as well as an evaluation of the spin exchange interactions by first principles density functional theory (DFT) calculations. Anhydrous CuCl2 shows one dimensional antiferromagnetic behavior and long range antiferromagnetic ordering below a Neel temperature of 23.9 K. Neutron powder and single crystal diffraction reveal that, below 23.9K, CuCl2 undergoes a phase t…
We present a microscopic model of the spin-gap quantum magnet (CuCl)LaNb2O7 that was previously suggested as a realization of the spin-1/2 frustrated square lattice. Taking advantage of the precise atomic positions from recent crystal structure refinement, we evaluate individual exchange integrals and construct a minimum model that naturally explains all the available experimental data. Surprisingly, the deviation from tetragonal symmetry leads to the formation of spin dimers between fourth neighbors due to a Cu-Cl-Cl-Cu pathway with a leading antiferromagnetic exchange J4 ~ 25 K. The total in…
We report an experimental and theoretical study of the low-temperature specific heat $C$ and magnetic susceptibility $χ$ of the layered anisotropic triangular-lattice spin-1/2 Heisenberg antiferromagnets Cs$_2$CuCl$_{4-x}$Br$_x$ with $x$ = 0, 1, 2, and 4. We find that the ratio $J'/J$ of the exchange couplings ranges from 0.32 to $\approx 0.78$, implying a change (crossover or quantum phase transition) in the materials' magnetic properties from one-dimensional (1D) behavior for $J'/J < 0.6$ to two-dimensional (2D) behavior for $J'/J \approx 0.78$ behavior. For $J'/J < 0.6$, realized for $x$ = …
We investigate the electronic structure of Cs$_2$CuCl$_4$, a material discussed in the framework of a frustrated quantum antiferromagnet, by means of resonant inelastic x-ray scattering (RIXS) and Density Functional Theory (DFT). From the non-dispersive highly localized dd excitations, we resolve the crystal field splitting of the Cu$^{2+}$ ions in a strongly distorted tetrahedral coordination. This allows us to model the RIXS spectrum within the Crystal Field Theory (CFT), assign the dd orbital excitations and retrieve experimentally the values of the crystal field splitting parameters D$_q$,…
We present a computational study of the layered copper oxychloride [CuCl]LaNb(2)O(7) that has been recently proposed as a spin-1/2 frustrated square lattice compound. Our results evidence an orbitally degenerate ground state for the reported tetragonal crystal structure and reveal a Jahn-Teller-type structural distortion. This distortion heavily changes the local environment of copper -- CuO(2)Cl(2) plaquettes are formed instead of CuO(2)Cl(4) octahedra -- and restores the single-orbital scenario typical for copper oxides and oxyhalides. The calculated distortion is consistent with the availab…
Based on a realistic spin Hamiltonian for a frustrated quasi-two dimensional spin-1/2 antiferromagnet Cs$_{2}$CuCl$_{4}$, a three-dimensional spin ordering in the applied magnetic field $B$ near the saturation value $B_{c}$ is studied within the magnon Bose-Einstein condensation (BEC) scenario. With the use of a hard-core boson formulation of the spin model, a strongly anysotropic magnon dispersion in Cs$_{2}$CuCl$_{4}$ is calculated. In the dilute magnon limit near $B_{c}$, the hard-core boson constraint is resulted in an effective magnon interaction which is treated in the Hartree-Fock appro…
Periodic and cluster density-functional theory (DFT) calculations, including DFT+U and hybrid functionals, are applied to study magnetostructural correlations in spin-1/2 frustrated chain compounds CuX2: CuCl2, CuBr2, and a fictitious chain structure of CuF2. The nearest-neighbor and second-neighbor exchange integrals, J1 and J2, are evaluated as a function of the Cu-X-Cu bridging angle, theta, in the physically relevant range 80-110deg. In the ionic CuF2, J1 is ferromagnetic for theta smaller 100deg. For larger angles, the antiferromagnetic superexchange contribution becomes dominant, in acco…
The objective of the present work was to analyze the possibility of realization of quantum spin liquid in three volcanic minerals - averievite (Cu5O2(VO4)2(CuCl)), ilinskite (NaCu5O2(SeO3)2Cl3), and avdononite (K2Cu5Cl8(OH)4 2H2O - from the crystal chemistry point of view. Based on the structural data, the sign and strength of magnetic interactions have been calculated and the geometric frustrations serving as the main reason of the existence of spin liquids have been investigated. According to our calculations, the magnetic structures of averievite and ilinskite are composed of antiferromagne…
Motivated by the recent discovery of the spin tube [(CuCl$_2$tachH)$_3$Cl]Cl$_2$, we investigate the properties of a frustrated three-leg spin tube with antiferromagnetic intra-ring and inter-ring couplings. We pay special attention to the evolution of the properties from weak to strong inter-ring coupling and show on the basis of extensive density matrix renormalization group and exact diagonalization calculations that the system undergoes a first-order phase transition between a dimerized gapped phase at weak coupling that can be described by the usual spin-chirality model and a gapless crit…
We present a theoretical and experimental study of a quasi-one-dimensional zigzag antiferromagnet (N_2H_5)CuCl_3, which can be viewed as weakly coupled Heisenberg chains with a frustrated interaction. We first discuss generic features of the magnetic properties of the zigzag spin chain between the nearly single chain case and the nearly double chain case, on the basis of the finite temperature density-matrix renormalization group (DMRG) calculations. We next show the experimental results for the magnetic susceptibility and the high-field magnetization of a single crystal of (N_2H_5)CuCl_3 abov…
We present a comprehensive review of nuclear magnetic resonance (NMR) studies performed on three nanoscale molecular magnets with different configurations of geometrically frustrated antiferromagnetic (AFM) triangles, new spin frustration systems with different novel structures: (1) the isolated single AFM triangle K$_6$[V$_{15}$As$_6$O$_{42}$(H$_2$O)]$\cdot$8H$_2$O (in short V15), (2) the spin ball [Mo$_{72}$Fe$_{30}$O$_{252}$(Mo$_2$O$_7$(H$_2$O))$_2$ (Mo$_2$O$_8$H$_2$(H$_2$O))(CH$_3$COO)$_{12}$(H$_2$O)$_{91}$]$\cdot$150H$_2$O (in short Fe30 spin ball), and (3) the twisted triangular spin tub…
Effects of Fe-substitution on the crystal structure and magnetic correlations of the geometrically frustrated antiferromagnets YBaCo4-xFexO7+δ (x = 0, 0.2, 0.4, 0.5, 0.6, and 0.8) have been studied by neutron diffraction, Mössbauer spectroscopy, and ac susceptibility. The compounds YBaCo4-xFexO7+δ have a special layered-type crystal structure with an alternating Kagomé (6c site) and triangular (2a site) layers along the c axis. Fe3+ ions are found to be substituted at both the crystallographic 2a and 6c sites of Co ions. Mössbauer results show a high spin state of Fe3+ ions in a tetrahedral co…
Motivated by the crystal structures of [(CuCl2tachH)3Cl]Cl2 and Ca3Co2O6, we develop a low-energy effective theory using the bosonization technique for a spin-1/2 frustrated three-leg spin tube with trigonal prism units in two limit cases. The features obtained with the effective theory are numerically elucidated by the density matrix renormalization group method. Three different quantum phases in the ground state of the system, say, one gapped dimerized phase and two distinct gapless phases, are identified, where the two gapless phases are found to have the conformal central charge c=1 and 3/…
We present the temperature dependence of the uniform susceptibility of spin-half quantum antiferromagnets on spatially anisotropic triangular-lattices, using high temperature series expansions. We consider a model with two exchange constants, $J_1$ and $J_2$ on a lattice that interpolates between the limits of a square-lattice ($J_1=0$), a triangular-lattice ($J_2=J_1$), and decoupled linear chains ($J_2=0$). In all cases, the susceptibility which has a Curie-Weiss behavior at high temperatures, rolls over and begins to decrease below a peak temperature, $T_p$. Scaling the exchange constants t…
We report muon spin relaxation ($μ$SR) and magnetic susceptibility measurements on Cu(Cl,Br)La(Nb,Ta)$_{2}$O$_{7}$, which demonstrate: (a) the absence of static magnetism in (CuCl)LaNb$_{2}$O$_{7}$ down to 15 mK confirming a spin-gapped ground state; (b) phase separation between partial volumes with a spin-gap and static magnetism in (CuCl)La(Nb,Ta)$_{2}$O$_{7}$; (c) history-dependent magnetization in the (Nb,Ta) and (Cl,Br) substitution systems; (d) a uniform long-range collinear antiferromagnetic state in (CuBr)LaNb$_{2}$O$_{7}$; and (e) a decrease of Néel temperature with decreasing Br conc…
We present inelastic neutron scattering and thermodynamic measurements characterizing the magnetic excitations in a disordered non-magnetic substituted spin-liquid antiferromagnet. The parent compound Ba3Mn2O8 is a dimerized, quasi-two-dimensional geometrically frustrated quantum disordered antiferromagnet. We substitute this compound with non-magnetic vanadium for the S = 1 manganese atoms, Ba3(Mn1-xVx)2O8, and find that the singlet-triplet excitations which dominate the spectrum of the parent compound persist for the full range of substitution examined, x = 0.02 to 0.3. We also observe addit…
We have systematically investigated the influence of gradual replacement of Ca by Gd on the magnetic and complex dielectric properties of the well-known geometrically frustrated spin-chain system, Ca3Co2O6 (T_N= 24 K with additional magnetic transitions below 12K), by studying the series, Ca3-xGdxCo2O6 (x less than 0.7), down to 1.8K. Heat capacity measurements establish that the reduction of T_N with Gd substitution is much less as compared to that by Y substitution. The magnetic moment data reveal that there are changes in the oxidation state of Co as well, unlike for Y-substitution, beyond …
The effect of chemical substitution on the ground state of the geometrically frustrated antiferromagnet CsCrF$_4$ has been investigated through a neutron powder diffraction experiment. Magnetic Fe-substituted CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$ and nonmagnetic Al-substituted CsCr$_{0.98}$Al$_{0.02}$F$_{4}$ samples are measured, and magnetic Bragg peaks are clearly observed in both samples. Magnetic structure analysis revealed a 120$^{\circ}$ structure having a magnetic propagation vector $\mathbf{k}_{\rm mag}=(0,0,1/2)$ in CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$. For CsCr$_{0.98}$Al$_{0.02}$F$_{4}$, a qua…
Spin-1/2 Heisenberg antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ with distorted triangular-lattice structures are studied by means of electron spin resonance spectroscopy in magnetic fields up to the saturation field and above. In the magnetically saturated phase, quantum fluctuations are fully suppressed, and the spin dynamics is defined by ordinary magnons. This allows us to accurately describe the magnetic excitation spectra in both materials and, using the harmonic spin-wave theory, to determine their exchange parameters. The viability of the proposed method was proven by applying it…
In this paper, we investigate the properties of frustrated three-leg spin tubes under a magnetic field. We concentrate on two kind of geometries for these tubes, one of which is relevant for the compound $\mathrm{[(CuCl_2tachH)_3Cl]Cl_2}$. We combine an analytical path integral approach with a strong coupling approach, as well as large-scale Density Matrix Renormalization Groups (DMRG) simulations, to identify the presence of plateaux in the magnetization curve as a function of the value of spin $S$. We also investigate the issue of gapless non-magnetic excitations on some plateaux, dubbed chi…
Magnetic insulators have proven to be usable as quantum simulators for itinerant interacting quantum systems. In particular the compound (C$_{5}$H$_{12}$N)$_{2}$CuBr$_{4}$ (short (Hpip)$_{2}$CuBr$_{4}$) was shown to be a remarkable realization of a Tomonaga-Luttinger liquid (TLL) and allowed to quantitatively test the TLL theory. Substitution weakly disorders this class of compounds and allows thus to use them to tackle questions pertaining to the effect of disorder in TLL as well, such as the formation of the Bose glass. As a first step in this direction we present in this paper a study of th…
We present detailed calculations of the magnetic ground state properties of Cs$_2$CuCl$_4$ in an applied magnetic field, and compare our results with recent experiments. The material is described by a spin Hamiltonian, determined with precision in high field measurements, in which the main interaction is antiferromagnetic Heisenberg exchange between neighboring spins on an anisotropic triangular lattice. An additional, weak Dzyaloshinkii-Moriya interaction introduces easy-plane anisotropy, so that behavior is different for transverse and longitudinal field directions. We determine the phase di…
Time-domain magneto-THz spectroscopy is utilized to study the frustrated magnet averievite Cu$_{5-x}$Zn$_x$V$_2$O$_{10}$(CsCl). Pronounced THz resonances are observed in unsubstituted samples ($x=0$) when cooling below the onset of short-range magnetic correlations. The influence of external magnetic effects confirms the magnetic origin of these resonances. Increasing Zn substitution suppresses the resonances, as frustration effects dominate, reflecting the non-magnetic phases for $x> 0.25$ compounds. The temperature evolution of the THz spectra is complemented with electron spin resonance spe…
Impurity effects on the triangular antiferromagnets Ni$_{1-x}M_x$Ga$_2$S$_4$ ($M=$ Mn, Fe, Co and Zn) are studied. The 2D frozen spin-disordered state of NiGa$_2$S$_4$ is stable against the substitution of Zn$^{2+}$ ($S=0$) and Heisenberg Fe$^{2+}$ ($S=2$) spins, and exhibits a $T^2$-dependent magnetic specific heat, scaled by the Weiss temperature. In contrast, the substitutions with Co$^{2+}$ ($S=3/2$) spin with Ising-like anisotropy and Heisenberg Mn$^{2+}$ ($S=5/2$) spin induce a conventional spin glass phase. From these comparisons, it is suggested that integer size of Heisenberg spins is…
For temperatures below 0.6 K the geometrically frustrated layered quantum antiferromagnet Cs$_2$CuCl$_4$ in a magnetic field perpendicular to the layers orders magnetically in a so-called cone state, where the magnetic moments have a finite component in the field direction while their projection onto the layers forms a spiral. Modeling this system by a two-dimensional spatially anisotropic quantum Heisenberg antiferromagnet with Dzyaloshinskii-Moriya interaction, we find that even for vanishing temperature the usual spin-wave expansion is plagued by infrared divergencies which are due to the c…
Dielectric and magnetic properties have been studied for poly-crystalline samples of quasi-one-dimensional frustrated spin-1/2 system Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$(M=Ni and Zn) which does not exhibit a three-dimensional magnetic transition due to quantum spin fluctuation and low dimensionality. A broad peak in the magnetic susceptibility - temperature curves originated from a short range helical ordering at low temperature is suppressed by the Ni and Zn substitution for Cu sites. The capacitance is found to anomalously increase with decreasing T below ~50 K, which is also s…
We report the magnetic properties of $A$-site spinel compound MnSc$_2$Se$_4$. The macroscopic magnetic measurements uncovers successive magnetic transitions at $T_{\rm{N1}}$= 2.04 K, followed by two further transitions at $T_{\rm{N2}}$=1.8 K and $T_{\rm{N3}}$=1.6 K. Neutron powder diffraction reveals that both, $T_{\rm{N2}} < T < T_{\rm{N1}}$ and $T <T_{\rm{N3}}$, orders are associated with the propagation vector $k$=(3/4 3/4 0), while the magnetic structures are collinear amplitude modulated and helical, respectively. Using neutron powder spectroscopy we demonstrated the effect of substitutio…
$^7$Li and $^{29}$Si NMR, $μ$SR and magnetization measurements in Li$_2$V$_{1-x}$OTi$_x$SiO$_4$, for $0 \leq x \leq 0.2$, are presented. The $x=0$ compound is a prototype of frustrated two-dimensional Heisenberg antiferromagnet on a square-lattice with competing nearest ($J_1$) and next-nearest ($J_2$) neighbour exchange interactions. Ti$^{4+}$ (S=0) for V$^{4+}$ (S=1/2) substitution yields the spin dilution of the antiferromagnetic layers. The analysis of the magnetization and of the nuclear spin-lattice relaxation rate shows that spin dilution not only reduces the spin-stiffness by a factor …
Using neutron powder diffraction and Monte-Carlo simulations we show that a spin-liquid regime emerges at $all compositions in the diamond-lattice antiferromagnets Co(Al1-xCox)2O4. This spin-liquid regime induced by frustration due to the second-neighbour exchange coupling J2, is gradually superseded by antiferromagnetic collinear long-range order (k=0) at low temperatures. Upon substitution of Al3+ by Co3+ in the octahedral B-site the temperature range occupied by the spin-liquid regime narrows and TN increases. To explain the experimental observations we considered magnetic anisotropy D or t…
The influence of negative chemical pressure induced by gradual replacement of Ca by Sr as well as of external pressure (up to 10 kbar) on the magnetism of Ca3CoRhO6 has been investigated by magnetization studies. It is found that the solid solution, Ca(3-x)Sr(x)CoRhO6, exists at least till about x= 1.0 without any change in the crystal structure. Apart from insensitivity of the spin-chain feature to volume expansion, the characteristic features of geometrical frustration interestingly appear at the same temperatures for all compositions, in sharp contrast to the response to Y substitution for …
The effect of disorder is studied on the field-induced quantum phase transition in the frustrated spin-ladder compound H8C4SO2Cu2(Cl[1-x]Brx)4 using bulk magnetic and thermodynamic measurements. The parent material (x=0) is a quantum spin liquid, which in applied fields is known to form a magnon condensate with long-range helimagnetic order. We show that bond randomness introduced by a chemical substitution on the non-magnetic halogene site destroys this phase transition at very low concentrations, already for x=0.01. The extreme fragility of the magnon condensate is attributed to random frust…
We report nuclear magnetic resonance (NMR) studies in the antiferromagnetic state of the quasi-two-dimensional (CuBr)LaNb2O7. The NMR spectra at zero magnetic field and 4.2 K indicate a unique Cu and Br sites with an internal field of 5.7 T (at Cu) and 16.4 T (at Br), confirming a magnetic order. For the large internal field at the Br sites to be compatible with the collinear antiferromagnetic order observed by neutron diffraction experiments (N. Oba et al., J. Phys. Soc. Jpn. 75, (2006) 113601), the Br atoms must move significantly off the center of the square of the Cu sublattice so that the…
We present a study on the impact of Mn$^{3+}$ substitution in the geometrically frustrated Ising garnet Ho$_3$Ga$_5$O$_{12}$ using bulk magnetic measurements and low temperature powder neutron diffraction. We find that the transition temperature, $T_N$ = 5.8 K, for Ho$_3$MnGa$_4$O$_{12}$ is raised by almost 20 when compared to Ho$_3$Ga$_5$O$_{12}$. Powder neutron diffraction on Ho$_3$Mn$_x$Ga$_{5-x}$O$_{12}$ ($x$ = 0.5, 1) below $T_N$ shows the formation of a long range ordered ordered state with $\mathbf{k}$ = (0,0,0). Ho$^{3+}$ spins are aligned antiferromagnetically along the six crystallog…
We study the evolution of the single-hole spectral function when the ground state of the anisotropic-triangular-lattice antiferromagnet changes from the incommensurate magnetically-ordered phase to the spin-liquid state. In order to describe both of the ground states on equal footing, we use the large-N approach where the transition between these two phases can be obtained by controlling the quantum fluctuations via an 'effective' spin magnitude. Adding a hole into these ground states is described by a t-J type model in the slave-fermion representation. Implications of our results to possible …
The geometrically-frustrated, triangular antiferromagnet GGG exhibits a rich mix of short-range order and isolated quantum states. We investigate the effects of up to 1% Neodymium substitution for Gallium on the ac magnetic response at temperatures below 1 K in both the linear and nonlinear regimes. Substitutional disorder actually drives the system towards a more perfectly frustrated state, apparently compensating for the effect of imperfect Gadolinium/Gallium stoichiometry, while at the same time more closely demarcating the boundaries of isolated, coherent clusters composed of hundreds of s…
Intrinsic Magnetic Excitations and Heavy-Fermion Formation in the Frustrated Mn Pyrochlore System YMn$_{2+δ}$Zn$_{20-x}X_x$ ($X$ = In and Al) Revealed by Nuclear Magnetic Resonance and Nuclear Quadrupole Resonance Measurements
Shastry-Sutherland lattice was observed as alternative ground state in Rare Earth intermetallic with Mo$_2$B$_2$Fe and U$_2$Pt$_2$Sn anisotropic structures where magnetic frustration is favored. In the case of Ce$_2$Pd$_2$Sn, it was shown that such phase can be suppressed by the application of magnetic field and, in this work, its stability is studied as a function of the electronic concentration by doping the Sn(4+) lattice with In(3+) atoms. Magnetic and specific heat measurements show that around 50\% substitution the Shastry Sutherland lattice vanishes in a critical point. This result conf…
Ba$_3$Mn$_2$O$_8$ is a geometrically frustrated spin dimer compound. We investigate the effect of site disorder on the zero field phase diagram of this material by considering the solid solution Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$, where nonmagnetic V$^{5+}$ ions partially substitute magnetic Mn$^{5+}$ ions. This substitution results in unpaired $S=1$ moments for half-substituted dimers, which are ungapped and therefore susceptible to types of magnetic order not present in the parent compound. AC susceptibility measurements of compositions between $x=0.046$ and $x=0.84$ show a sharp frequ…
We present a successful synthesis method of the series Ga$_{x}$Cu$_{4-x}$(OD)$_{6}$Cl$_{2}$ with substitutions up to $x=0.8$. The compound remains a frustrated kagome system with an insulating ground state similar to herbertsmithite for these substitutions, as the additional charge of Ga$^{3+}$ is most likely bound to additional OH$^{-}$ and Cl$^{-}$. Besides infrared measurements, we present magnetic and specific-heat data down to 2 K for selected samples with $0\leq x\leq0.8$. With increasing $x$ the long-range magnetic order is suppressed, similar to what was observed in the series Zn$_{x}$…
CeFe$_2$ is a geometrically frustrated ferromagnet that lies close to an instability at which a subtle change in the lattice symmetry couples to a transition to antiferromagnetism. We use x-ray diffraction, diamond-anvil-cell techniques, and numerical simulation to identify the ground states and to quantitatively illustrate effects of competing magnetic energy scales and geometrical frustration on the magnetic phase diagram. Comparison of phase transitions under both chemical substitution and applied pressure suggests a general solution to the physics of pyrochlore rare earth inter-metallic ma…
Spin correlations in the geometrically frustrated RBaCo4O7 compounds, usually described as an alternating stacking of Kagome and triangular layers on a hexagonal lattice, have been studied by mean-field approach and by Monte-Carlo simulations. The behavior of the system was modelled with an isotropic Heisenberg Hamiltonian as a function of the relevant parameter Jout/Jin, representing the ratio between exchange integrals inside the Kagome layers, Jin, and between Kagome and triangular layers, Jout. This ratio can be varied in real systems by appropriate chemical substitutions. At the mean-fiel…
We report the remarkably robust ferroelectric state in the multiferroic compound Mn$_{1-x}$Zn$_x$WO$_4$. The substitution of the magnetic Mn$^{2+}$ with nonmagnetic Zn$^{2+}$ reduces the magnetic exchange and provides control of the various magnetic and multiferroic states of MnWO$_4$. Only 5 % of Zn substitution results in a complete suppression of the frustrated collinear (paraelectric) low temperature phase. The helical magnetic and ferroelectric phase develops as the ground state. The multiferroic state is stable up to a high level of substitution of more than 50 %. The magnetic, thermodyn…
The Fe sublattice in the compound ZrFe$_4$Si$_2$ features geometrical frustration and quasi-one-dimensionality. We therefore investigated the magnetic behavior in ZrFe$_4$Si$_2$ and its evolution upon substituting Ge for Si and under the application of hydrostatic pressure using structural, magnetic, thermodynamic, and electrical-transport probes. Magnetic measurements reveal that ZrFe$_4$Si$_2$ holds paramagnetic Fe moments with an effective moment $μ_{\rm eff}= 2.18~μ_{B}$. At low temperatures the compound shows a weak short-range magnetic order below 6 K. Our studies demonstrate that substi…
The effects of substituting nonmagnetic Mg2+ and Zn2+ ions for the Mn2+ (S = 5/2) ions on the structural, magnetic and dielectric properties of the multiferroic frustrated antiferromagnet MnWO4 were investigated. Polycrystalline samples of Mn1-xMgxWO4 and Mn1-xZnxWO4 (0<x<0.3) solid solutions were prepared by a solid-state route and characterized via X-ray and neutron diffraction, magnetization, and dielectric permittivity measurements. Mg and Zn substitutions give rise to very similar effects. The Neel temperature TN, the AF3-to-AF2 magnetic phase transition temperature T2, and the critical f…
Quantum magnetic properties in a geometrically frustrated lattice of spin-1/2 magnet, such as quantum spin liquid or solid and the associated spin fractionalization, are considered key in developing a new phase of matter. The feasibility of observing the quantum magnetic properties, usually found in geometrically frustrated lattice of spin-1/2 magnet, in a perovskite material with controlled disorder is demonstrated. It is found that the controlled chemical disorder, due to the chemical substitution of Ru ions by Co-ions, in a simple perovskite CaRuO3 creates a random prototype configuration o…
We report susceptibility, specific heat, and neutron diffraction measurements on NaCu$_2$O$_2$, a spin-1/2 chain compound isostructural to LiCu$_2$O$_2$, which has been extensively investigated. Below 13 K, we find a long-range ordered, incommensurate magnetic helix state with a propagation vector similar to that of LiCu$_2$O$_2$. In contrast to the Li analogue, substitutional disorder is negligible in NaCu$_2$O$_2$. We can thus rule out that the helix is induced by impurities, as was claimed on the basis of prior work on LiCu$_2$O$_2$. A spin Hamiltonian with frustrated longer-range exchange …
Anisotropic Kitaev Spin Glass in Li$_{2}$Ru$_{x}$Ir$_{1-x}$O$_{3}$
University of California, San Diego（加州大学圣迭戈分校）；Institute of Science and Technology Austria（奥地利科学技术研究所）；TRIUMF（特利昂夫实验室）；Argonne National Laboratory（阿贡国家实验室）；Brookhaven National Laboratory（布鲁克海文国家实验室）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Brigham Young University（杨百翰大学）；University of California, Berkeley（加州大学伯克利分校）
We study the $3d$ substitution in $4d$ transition metal oxides in the cases of $3d^3$ doping at either $3d^2$ or $4d^4$ sites which realize orbital dilution. We derive the effective $3d-4d$ (or $3d-3d$) superexchange in a Mott insulator with different ionic valencies, underlining the emerging structure of the spin-orbital coupling between the impurity and the host sites and demonstrate that it is qualitatively different from that encountered in the host itself. This derivation shows that the interaction between the host and the impurity depends in a crucial way on the type of doubly occupied $…
The ground state magnetic behaviour of Ce2(Pd0.8Ag0.2)2In and Ce2(Pd0.5Ag0.5)2In, found in the ferromagnetic branch of Ce2Pd2In, has been investigated by neutron powder diffraction at low temperature. Ce2(Pd0.8Ag0.2)2In is characterized by a ferromagnetic structure with the Ce moments aligned along the c-axis and values of 0.96(2) mB. The compound retains the P4/mbm throughout the magnetic transition, although the magnetic ordering is accompanied by a significant decrease of the lattice strain along [00l], suggesting a magnetostructural contribution. The magnetic behaviour of Ce2(Pd0.5Ag0.5)2I…
Quantum spin systems such as magnetic insulators usually show classical magnetic order, but such classical states can give way to quantum liquids with exotic entanglement through two known mechanisms of frustration: geometric frustration in lattices with triangle motifs, and spin-orbit-coupling frustration in the exactly solvable quantum liquid of Kitaev's honeycomb lattice. Here we present the experimental observation of a new kind of frustrated quantum liquid arising in an unlikely place: the magnetic insulator Ba4Ir3O10 where Ir3O12 trimers form an unfrustrated square lattice. Experimentall…
