We propose a microscopic mechanism for the incommensurate phase in TiOX compounds. The model includes the antiferromagnetic chains of Ti ions immersed in the phonon bath of the bilayer structure. Making use of the Cross-Fisher theory, we show that the geometrically frustrated character of the lattice is responsible for the structural instability which leads the chains to an incommensurate phase without an applied magnetic field. In the case of TiOCl, we show that our model is consistent with the measured phonon frequencies at $T=300K$ and the value of the incommensuration vector at the transition temperature. Moreover, we find that the dynamical structure factor shows a progressive softening of an incommensurate phonon near the zone boundary as the temperature decreases. This softening is accompanied by a broadening of the peak which gets asymmetrical as well when going towards the transition temperature. These features are in agreement with the experimental inelastic X-ray measurements.
We report on a detailed single crystal x-ray diffraction study of the unconventional spin-Peierls compound TiOCl. The intermediate phase of TiOCl is characterized by an incommensurate modulation which is virtually identical to that recently found in the homologue compound TiOBr. The first order phase transition between the spin-Peierls ground state and the incommensurate phase reveals the same kind of thermal hysteresis in both, its crystal structure and magnetic susceptibility. A weak, but significant magnetic field effect is found for this phase transition with a field induced shift of the t…
X-ray scattering measurements on single crystals of TiOCl reveal the presence of commensurate dimerization peaks within both the incommensurate spin-Peierls phase and the so-called pseudogap phase above T_c2. This scattering is relatively narrow in Q-space indicating long correlation lengths exceeding ~ 100 A below T* ~ 130 K. It is also slightly shifted in Q relative to that of the commensurate long range ordered state at the lowest temperatures, and it coexists with the incommensurate Bragg peaks below T_c2. The integrated scattering over both commensurate and incommensurate positions evolve…
The ground state of the spin-Peierls system TiOCl was probed using synchrotron x-ray diffraction on a single-crystal sample at T = 6 K. We tracked the evolution of the structural superlattice peaks associated with the dimerized ground state as a function of pressure. The dimerization along the b axis is rapidly suppressed in the vicinity of a first-order structural phase transition at Pc = 13.1(1) GPa. The high-pressure phase is characterized by an incommensurate charge density wave perpendicular to the original spin chain direction. These results show that the electronic ground state undergoe…
We report on the magnetic, thermodynamic and optical properties of the quasi-one-dimensional quantum antiferromagnets TiOCl and TiOBr, which have been discussed as spin-Peierls compounds. The observed deviations from canonical spin-Peierls behavior, e.g. the existence of two distinct phase transitions, have been attributed previously to strong orbital fluctuations. This can be ruled out by our optical data of the orbital excitations. We show that the frustration of the interchain interactions in the bilayer structure gives rise to incommensurate order with a subsequent lock-in transition to a …
In the present work we aim to characterize the lattice configurations and the magnetic behavior in the incommensurate phase of spin-Peierls systems. This phase emerges when the magnetic exchange interaction is coupled to the distortions of an underlying triangular lattice and has its experimental realization in the quasi-one dimensional compound family TiOX (X = Cl, Br). With a simple model of spin-1/2 chains inserted in a planar triangular geometry which couples them elastically, we are able to obtain the uniform-incommensurate and incommensurate-dimerized phase transitions seen in these comp…
Going beyond a recently proposed microscopic model for the incommensurate transition in the spin-Peierls TiOX (X=Cl, Br) compounds, in the present work we start by studying the thermodynamics of the model with XY spins and adiabatic phonons. We find that the system enters in an incommensurate phase by a first order transition at a low temperature $T_{c1}$. At a higher temperature $T_{c2}$ a continuous transition to a uniform phase is found. Furthermore, we study the magnetism in the incommensurate phase by Density Matrix Renormalization Group (DMRG) calculations on a 1D Heisenberg model where …
We analyze the effect of the phonon dynamics on a recently proposed model for the uniform-incommensurate transition seen in TiOX compounds. The study is based on a recently developed formalism for nonadiabatic spin-Peierls systems based on bosonization and a mean field RPA approximation for the interchain coupling. To reproduce the measured low temperature spin gap, a spin-phonon coupling quite bigger than the one predicted from an adiabatic approach is required. This high value is compatible with the renormalization of the phonons in the high temperature phase seen in inelastic x-ray experime…
We have performed x-ray scattering measurements on single crystals of the doped spin-Peierls compound Ti(1-x)Sc(x)OCl (x = 0, 0.01, 0.03). These measurements reveal that the presence of non-magnetic dopants has a profound effect on the unconventional spin-Peierls behavior of this system, even at concentrations as low as 1%. Sc-doping suppresses commensurate fluctuations in the pseudogap and incommensurate spin-Peierls phases of TiOCl, and prevents the formation of a long-range ordered spin-Peierls state. Broad incommensurate scattering develops in the doped compounds near Tc2 ~ 93 K, and persi…
We have studied the S=1/2 quasi-one-dimensional antiferromagnet TiOCl using single crystal x-ray diffraction and inelastic x-ray scattering techniques. The Ti ions form staggered spin chains which dimerize below Tc1 = 66 K and have an incommensurate lattice distortion between Tc1 and Tc2 = 92 K. Based on our measurements of the intensities, wave vectors, and harmonics of the incommensurate superlattice peaks, we construct a model for the incommensurate modulation. The results are in good agreement with a soliton lattice model, though some quantitative discrepancies exist near Tc2. The behavior…
On the basis of ab initio density functional theory (DFT) calculations, we derive the underlying microscopic model Hamiltonian for TiOCl, a unique system that shows two consecutive phase transitions from a Mott insulator to a spin-Peierls insulator through a structurally incommensurate phase. We show with our model that the presence of magnetic frustration in TiOCl leads to a competition with the spin-Peierls distortion, which results in the novel incommensurate phase. In addition, our calculations indicate that the spin-Peierls state is triggered by adiabatic phonons, which is essential for u…
The application of pressure can induce transitions between unconventional quantum phases in correlated materials. The inorganic compound TiOCl, composed of chains of S=1/2 Ti ions, is an ideal realization of a spin-Peierls system with a relatively simple unit cell. At ambient pressure, it is an insulator due to strong electronic interactions (a Mott insulator). Its resistivity shows a sudden decrease with increasing pressure, indicating a transition to a more metallic state which may coincide with the emergence of charge density wave order. Therefore, high pressure studies of the structure wit…
We present first principles density functional calculations and downfolding studies of the electronic and magnetic properties of the layered quantum spin system TiOCl. We discuss explicitely the nature of the exchange pathes and attempt to clarify the concept of orbital ordering in this material. An analysis of the electronic structure of slightly distorted structures according to the phononic modes allowed in this material suggests that this system is subject to large orbital fluctuations driven by the electron-phonon coupling. Based on these results, we propose a microscopic explanation of t…
The sequence of phase transitions and the symmetry of in particular the low temperature incommensurate and spin-Peierls phases of the quasi one-dimensional inorganic spin-Peierls system TiOX (TiOBr and TiOCl) have been studied using inelastic light scattering experiments. The anomalous first-order character of the transition to the spin-Peierls phase is found to be a consequence of the different symmetries of the incommensurate and spin-Peierls (P$2_{1}/m$) phases. The pressure dependence of the lowest transition temperature strongly suggests that magnetic interchain interactions play an impor…
The nickelate compound Y_{2}BaNiO_{5} is a spin-1 Haldane-gap antiferromagnet. The compound is doped with holes on replacing the off-chain Y^{3+} ions by Ca^{2+} ions. Inelastic neutron scattering (INS) experiments reveal the existence of sub-gap states on doping. A recent INS experiment provides evidence for an incommensurate double-peaked structure factor S(q) corresponding to the sub-gap states. In this paper, we formulate a microscopic theory for the origin of the incommensurate peak.
We have performed $^{75}$As and $^{23}$Na nuclear magnetic resonance (NMR) measurements on a single crystal of NaFe$_{0.9835}$Co$_{0.0165}$As and found microscopic coexistence of superconductivity with a two-component spin density wave (SDW). Using $^{23}$Na NMR we measured the spatial distribution of local magnetic fields. The SDW was found to be incommensurate with a major component having magnetic moment ($\sim0.2\,μ_B$/Fe) and a smaller component with magnetic moment ($\sim0.02\,μ_B$/Fe). Spin lattice relaxation experiments reveal that this coexistence occurs at a microscopic level.
We analyze the excitation spectra of a spin-phonon coupled chain in the presence of a soliton. This is taken as a microscopic model of a Spin-Peierls material placed in a high magnetic field. We show, by using a semiclassical approximation in the bosonized representation of the spins that a trapped magnetic state obtained in the adiabatic approximation is destroyed by dynamical phonons. Low energy states are phonons trapped by the soliton. When the magnetic gap is smaller than the phonon frequencies the only low energy state is a mixed magneto-phonon state with the energy of the gap. We emphas…
Mechanism of Incommensurate Magnetic Order in $\mathrm{BaCo_2(AsO_4)_2}$: Interplay of Frustrated Further-Neighbor Exchanges and Bond-Directional Anisotropy
Qom University of Technology（库姆理工大学）；University of Toronto（多伦多大学）；Shahrekord University（沙赫里克尔德大学）
We present a theoretical study of the response of $β$-$\text{Li}_2\text{IrO}_3$ under external magnetic fields in the $ab$, $bc$ and $ac$ crystallographic planes. The results are based on the minimal nearest-neighbor $J$-$K$-$Γ$ model and reveal a rich intertwining of field-induced phases and magnetic phase transitions with distinctive signatures that can be probed directly via torque magnetometry. Most saliently, we observe: i) an unusual reentrance of the incommensurate counter-rotating order for fields in the $ab$-plane, and ii) a set of abrupt torque discontinuities which are particularly …
The pressure ($p$) -- temperature ($T$) phase diagram for microscopic magnetism in the multiferroic compound HoMn$_{2}$O$_{5}$ was established using neutron diffraction measurements under a hydrostatic pressure up to 1.25 GPa. At ambient pressure, incommensurate--commensurate--incommensurate magnetic phase transitions occur successively with decreasing temperature. Upon applying pressure, the incommensurate phase at the lowest temperature almost decreases and the commensurate phase appears. The $p$ -- $T$ phase diagram established shows excellent agreement with the recently reported $p$ -- $T$…
Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map at atomic resolution the nature of incommensurate order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ($\sim$ 93K). In diffraction, the ordering wavevector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the underlying ordered state is lattice-comme…
Motivated by recent experimental measurements on pressure-driven phase transitions in Mott-insulators as well as the new iron pnictide superconductors, we show that first principles Car-Parrinello molecular dynamics calculations are a powerful method to describe the microscopic origin of such transitions. We present results for (i) the pressure-induced insulator to metal phase transition in the prototypical Mott insulator TiOCl as well as (ii) the pressure-induced structural and magnetic phase transitions in the family of correlated metals $A$Fe$_2$As$_2$ ($A$=Ca,Sr,Ba). Comparison of our pred…
In the metallic magnet Nb$_{1-y}$Fe$_{2+y}$, the low temperature threshold of ferromagnetism can be investigated by varying the Fe excess $y$ within a narrow homogeneity range. We use elastic neutron scattering to track the evolution of magnetic order from Fe-rich, ferromagnetic Nb$_{0.981}$Fe$_{2.019}$ to approximately stoichiometric NbFe$_2$, in which we can, for the first time, characterise a long-wavelength spin density wave state burying a ferromagnetic quantum critical point. The associated ordering wavevector $\mathbf{q}_{\rm SDW}=$(0,0,$l_{\rm SDW}$) is found to depend significantly on…
Electronic-liquid-crystal phases, in which part of the spatial symmetries are broken spontaneously, are considered to play a vital role in interpreting the structure-property relation in strongly-correlated materials. Although electronic-liquid-crystal phases have been inferred in studies of a wide range of materials, the nature of the transition between such phases has received little experimental attention. Here we report the direct observation of an electronic smectic-nematic phase transition in a doped manganite utilizing transmission electron microscopic techniques. We show that, in this …
We investigate numerically the zero-temperature physics of the one-dimensional Bose-Hubbard model in an incommensurate cosine potential, recently realized in experiments with cold bosons in optical superlattices L. Fallani et al., Phys. Rev. Lett. 98, 130404, (2007)]. An incommensurate cosine potential has intermediate properties between a truly periodic and a fully random potential, displaying a characteristic length scale (the quasi-period) which is shown to set a finite lower bound to the excitation energy of the system at special incommensurate fillings. This leads to the emergence of gapp…
We have performed synchrotron radiation X-ray and neutron diffraction measurements on magnetoelectric multiferroic CuFe1-xAlxO2 (x=0.0155), which has a proper helical magnetic structure with incommensurate propagation wave vector in the ferroelectric phase. The present measurements revealed that the ferroelectric phase is accompanied by lattice modulation with a wave number 2q, where q is the magnetic modulation wave number. We have calculated the Fourier spectrum of the spatial modulations in the local electric polarization using a microscopic model proposed by Arima [T. Arima, J. Phys. Soc. …
We present a microscopic theory for the low temperature metamagnetic phase diagram of HoNi_2B_2C that agrees well with experiments.For the same model we determined the zero field ground state as a function of temperature and find the $c$-axis commensurate to incommensurate transition in the expected temperature range. The complex behaviour of the system originates from the competition between the crystalline electric field and the Ruderman-Kittel-Kasuya-Yosida interaction, whose effective form is obtained. No essential influence of superconductivity has to be invoked to understand the magnetic…
We use variable-temperature x-ray thermal diffuse scattering and inelastic scattering to investigate the lattice dynamics in single crystals of multiferroic CaMn7O12 which undergo a series of orbital and magnetic transitions at low temperatures. Upon approaching the charge and orbital ordering temperature To=250 K from above, we observe intense diffuse scattering features and a pronounced optical phonon softening centered around the superstructure reflections of the incommensurately modulated structure. The phonon anomaly appears well above To and continuously increases upon cooling, following…
We have performed simultaneous measurements of magnetic chirality by using polarized neutrons and electric polarization along the b-axis of single crystals of YMn$^{4+}$(Mn$_{1-x}$Ga$_{x}$)$^{3+}$O$_{5}$ with $x=0.047$ and 0.12, in which nonmagnetic Ga-ions dilute Mn$^{3+}$ spins. The $x=0.047$ sample exhibits high-temperature incommensurate (HT-ICM), commensurate (CM), and low-temperature incommensurate (LT-ICM) magnetic phases in order of decreasing temperature, whereas the $x=0.12$ sample exhibits only HT-ICM and LT-ICM phases. Here, the CM and LT-ICM phases are ferroelectric and weak-ferro…
We report an $^{75}$As NMR study of BaFe$_2$As$_2$ in both single crystals and polycrystal forms. We find that Sn impurities in the single crystal dramatically alter the low energy spin fluctuations and suppress the ordering temperature from 138 K to 85 K. In contrast to Sn-free samples, we find that the temperature dependence of the $^{75}$As NMR spectra and spin lattice relaxation rates reveal a second order phase transition to a state of incommensurate magnetic order.
Electronic Coherence Evolution at the Nearly Commensurate Incommensurate CDW Boundary of 1T-TaS2
Xiamen University Malaysia（厦门大学马来西亚分校）；University of Connecticut（康涅狄格大学）；Institute of Materials Science, Storrs, University of Connecticut（康涅狄格大学斯托尔斯材料科学研究所）；Center for Functional Nanomaterials, Brookhaven National Lab（布鲁克海文国家实验室功能纳米材料中心）；Synchrotron Light Research Institute (Public Organization), Ministry of Higher Education Science Research and Innovation（高等教育、科学研究与创新部同步光研究所）；National Synchrotron Light Source II, Brookhaven National Lab（布鲁克海文国家实验室国家同步光源二号设施）；Xiamen University（厦门大学）
We report thermodynamic properties, magnetic ground state, and microscopic magnetic model of the spin-1 frustrated antiferromaget Li$_{2}$NiW$_{2}$O$_{8}$ showing successive transitions at $T_{\rm N1}\simeq 18$ K and $T_{\rm N2}\simeq 12.5$ K in zero field. Nuclear magnetic resonance and neutron diffraction reveal collinear and commensurate magnetic order with the propagation vector $\mathbf k=(\frac12,0,\frac12)$ below $T_{\rm N2}$. The ordered moment of 1.8 $μ_B$ at 1.5 K is directed along $[0.89(9),-0.10(5),-0.49(6)]$ and matches the magnetic easy axis of spin-1 Ni$^{2+}$ ions, which is det…
We construct a microscopic model of electron interactions which gives rise to both superconductivity and antiferromagnetism, and which admits an approximate SO(5) symmetry that relates these two phases. The symmetry can be exact, or it may exist only in the long-wavelength limit, depending on the detailed form of the interactions. We compute the macroscopic Landau-Ginzburg free energy for this model as a function of temperature and doping, by explicitly integrating out the fermions. We find that the resulting phase diagram can resemble that observed for the cuprates, with the antiferromagnetis…
The magnetic phase transitions reported below 230 K in cupric oxide are analyzed theoretically at the macroscopic and microscopic levels. The incommensurate multiferroic and lock-in commensurate phases are shown to realize an inverted sequence of symmetry-breaking mechanisms with respect to the usual sequence occurring in low temperature multiferroic compounds. The higher temperature spin-spiral phase results from coupled order-parameters which decouple at the lock-in transition to the commensurate ground state phase. Expressing the order-parameters in function of the magnetic spins allows det…
By combining neutron four-circle diffraction and polarized neutron diffraction techniques we have determined the complex spin structures of a multiferroic, YMn2O5, that exhibits two ferroelectric phases at low temperatures. The obtained magnetic structure has spiral components in both the low temperature ferroelectric phases that are magnetically commensurate and incommensurate, respectively. Among proposed microscopic theories for the magneto-electric coupling, our results are consistent with both the spin-current model that requires a magnetic transverse (cycloidal) spiral structure in order…
Macroscopic magnetic properties and microscopic magnetic structure of Rb$_2$Mn$_3$(MoO$_4$)$_3$(OH)$_2$ (space group $Pnma$) are investigated by magnetization, heat capacity and single-crystal neutron diffraction measurements. The compound's crystal structure contains bond-alternating [Mn$_3$O$_{11}$]$^{\infty}$ chains along the $b$-axis, formed by isosceles triangles of Mn ions occupying two crystallographically nonequivalent sites (Mn1 site on the base and Mn2 site on the vertex). These chains are only weakly linked to each other by nonmagnetic oxyanions. Both SQUID magnetometry and neutron …
The anisotropic d=3 tJ model is studied by renormalization-group theory, yielding the evolution of the system as interplane coupling is varied from the isotropic three-dimensional to quasi-two-dimensional regimes. Finite-temperature phase diagrams, chemical potential shifts, and in-plane and interplane kinetic energies and antiferromagnetic correlations are calculated for the entire range of electron densities. We find that the novel tau phase, seen in earlier studies of the isotropic d=3 tJ model, and potentially corresponding to the superconducting phase in high-T_c materials, persists even …
Microscopic magnetic phase evolution in the Weyl semimetal Mn$_3$Sn revealed by $μ^+$SR
KTH Royal Institute of Technology（皇家理工学院）；Uppsala University（乌普萨拉大学）；PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢勒研究所中子与μ子科学中心）；University of Luxembourg（卢森堡大学）；Forschungszentrum Jülich GmbH（于利希研究中心有限公司）；TRIUMF（特利昂夫实验室）；Institut Laue-Langevin（朗之万-桂良研究所）；RWTH Aachen（亚琛工业大学）
We present a microscopic study of the interlayer spacing d versus in-plane magnetic field $B_\parallel$ phase diagram for bilayer quantum Hall (QH) pseudo-ferromagnets. In addition to the interlayer charge balanced commensurate and incommensurate states analyzed previously, we address the corresponding interlayer charge unbalanced "canted" QH states. We predict a large anomaly in the bilayer capacitance at the canting transition and the formation of dipole stripe domains with periods exceeding 1 micron in the canted state.
In order to study the phase diagram from a microscopic viewpoint, we have measured wTF- and ZF-$μ^+$SR spectra for the Sr$_{1-x}$Ca$_x$Co$_2$P$_2$ powder samples with $x=0$, 0.2, 0.4, 0.5, 0.6, 0.8, and 1. Due to a characteristic time window and spatial resolution of $μ^+$SR, the obtained phase diagram was found to be rather different from that determined by magnetization measurements. That is, as $x$ increases from 0, a Pauli-paramagnetic phase is observed even at the lowest $T$ measured (1.8~K) until $x=0.4$, then, a spin-glass like phase appears at $0.5\leq x\leq0.6$, and then, a phase with…
Electronic phases with symmetry properties matching those of conventional liquid crystals have recently been discovered in transport experiments on semiconductor heterostructures and metal oxides at milli-Kelvin temperatures. We report the spontaneous onset of a onedimensional, incommensurate modulation of the spin system in the high-temperature superconductor YBa2Cu3O6.45 upon cooling below ~150 K, while static magnetic order is absent above 2 K. The evolution of this modulation with temperature and doping parallels that of the in-plane anisotropy of the resistivity, indicating an electronic …
The space and time symmetry breaking at magnetic phase transitions in multiferroics results in a number of strongly pronounced optical effects. Our high-resolution spectroscopic study of 3d- excitons in a complex multi-sublattice magnetoelectric CuB2O4 demonstrates that, among those, a large antiferromagnetic linear dichroism is observed which is highly sublattice-sensitive to subtle changes in the spin subsystems. We prove that the discovered linear dichroism is related microscopically to the magnetic Davydov splitting of the exciton states. We announce a novel magnetic phase transition and a…
Magnetoelectric phase diagrams of the rare-earth (R) Mn perovskites RMnO3 are theoretically studied by focusing on crucial roles of the symmetric magnetostriction or the Peierls-type spin-phonon coupling through extending our previous work [M. Mochizuki et al., Phys. Rev. Lett. 105, 037205 (2010)]. We first construct a microscopic classical Heisenberg model for RMnO3 including the frustrated spin exchanges, single-ion anisotropy, and Dzyaloshinskii-Moriya interaction. We also incorporate the lattice degree of freedom coupled to the Mn spins via the Peierls-type magnetostriction. By analyzing t…
Isotropic and anisotropic magnetic behavior of the frustrated spin chain compound $β$-TeVO$_4$ is reported. Three magnetic transitions observed in zero magnetic field are tracked in fields applied along different crystallographic directions using magnetization, heat capacity, and magnetostriction measurements. Qualitatively different temperature-field diagrams are obtained below 10 T for the field applied along $a$ or $b$ and along $c$, respectively. In contrast, a nearly isotropic high-field phase emerges above 18 T and persists up to the saturation that occurs around 22.5 T. Upon cooling in …
