We report high-pressure x-ray diffraction and magnetization measurements combined with ab-initio calculations to demonstrate that the high-pressure optical and transport transitions recently reported in TiOCl, correspond in fact to an enhanced Ti3+-Ti3+ dimerization existing already at room temperature. Our results confirm the formation of a metal-metal bond between Ti3+ ions along the b-axis of TiOCl, accompanied by a strong reduction of the electronic gap. The evolution of the dimerization with pressure suggests a crossover from the spin-Peierls to a conventional Peierls situation at high pressures.
We study TiOCl as an example of an S=1/2 layered Mott insulator. From our analysis of new susceptibility data, combined with LDA and LDA+U band structure calculations, we conclude that orbital ordering produces quasi-one-dimensional spin chains and that TiOCl is a new example of Heisenberg-chains which undergo a spin-Peierls transition. The energy scale is an order of magnitude larger than that of previously known examples. The effects of non-magnetic Sc impurities are explained using a model of broken finite chains.
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 …
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…
We combine high-resolution resonant inelastic x-ray scattering with cluster calculations utilizing a recently derived effective magnetic scattering operator to analyze the polarization, excitation energy, and momentum dependent excitation spectrum of the low-dimensional quantum magnet TiOCl in the range expected for orbital and magnetic excitations (0 - 2.5 eV). Ti 3d orbital excitations yield complete information on the temperature-dependent crystal-field splitting. In the spin-Peierls phase we observe a dispersive two-spinon excitation and estimate the inter- and intra-dimer magnetic exchang…
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…
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…
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…
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…
We report experimental results on the heat conductivity κof the S=1/2 spin chain compounds TiOBr and TiOCl for temperatures 5K<T<300K and magnetic fields up to 14. Surprisingly, we find no evidence of a significant magnetic contribution to κ, which is in stark contrast to recent results on S=1/2 spin chain cuprates. Despite this unexpected result, the thus predominantly phononic heat conductivity of these spin-Peierls compounds exhibits a very unusual behavior. In particular, we observe strong anomalies at the phase transitions Tc1 and Tc2. Moreover, we find an overall but anisotropic suppress…
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 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…
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…
The effect of the charge ordering on the spin-Peierls (SP) state has been examined by using a Peierls-Hubbard model at quarter-filling with dimerization, on-site and nearest-neighbor repulsive interactions. By taking account of the presence of dimerization, a bond distortion is calculated variationally with the renormalization group method based on bosonization. When the charge ordering appears at V=V_c with increasing the nearest-neighbor interaction (V), the distortion exhibits a maximum due to competition between the dimerization and the charge ordering. It is shown that the second-order ph…
We study the magnetic properties of a frustrated Heisenberg spin chain with a dynamic spin-phonon interaction. By Lanczos diagonalization, preserving the full lattice dynamics, we explore the non-adiabatic regime with phonon frequencies comparable to the exchange coupling energy which is e.g. the relevant limit for the spin-Peierls compound $CuGeO_3$. When compared to the static limit of an alternating spin chain the magnetic properties are strongly renormalized due to the coupled dynamics of spin and lattice degrees of freedom. The magnitude of the spin triplet excitation gap changes from a s…
We have studied the electronic structure of the spin-1/2 quantum magnet TiOCl by polarization-dependent momentum-resolved photoelectron spectroscopy. From that, we confirm the quasi-one-dimensional nature of the electronic structure along the crystallographic b-axis and find no evidence for sizable phonon-induced orbital fluctuations as origin for the non-canonical phenomenology of the spin-Peierls transition in this compound. A comparison of the experimental data to our own LDA+U and Hubbard model calculations reveals a striking lack of understanding regarding the quasi-one-dimensional electr…
A model of disordered spin-Peierls system is considered, where domain walls are randomly distributed as a telegraph noise. For this realization of the disorder in an XX spin chain, we calculate exactly the density of states as well as several thermodynamic quantities. The resulting physical behavior should be qualitatively unchanged even for an XXZ chain, up to the isotropic XXX point. For weak disorder, besides a high energy regime where the behavior of a pure spin-Peierls system is recovered, there is a cross-over to a low energy regime with singular thermodynamic properties and enhanced ant…
Using Car-Parrinello molecular dynamics calculations we investigate the behavior of the low-dimensional multiorbital Mott insulator TiOCl under pressure. We show that the system undergoes {\it two} consecutive phase transitions, first at $P_\text{c}$ from a Mott-insulator to a metallic phase in the $ab$ plane with a strong Ti-Ti dimerization along $b$. At a pressure $P'_\text{c} > P_\text{c}$ the dimerization disappears and the system behaves as a uniform metal. This second transition has not yet been reported experimentally. We show that the insulator-to-metal transition at $P_\text{c}$ is dr…
Electronic structure calculations on the low dimensional spin-1/2 compound TiOCl were performed at several pressures in the orthorhombic phase, finding that the structure is quasi-one-dimensional. The Ti3+ (d1) ions have one t2g orbital occupied (dyz) with a large hopping integral along the b direction of the crystal. The most important magnetic coupling is Ti-Ti along the b axis. The transition temperature (Tc) has a linear evolution with pressure, and at about 10 GPa this Tc is close to room temperature, leading to a room temperature spin-Peierls insulator-insulator transition, with an impor…
We report on a zero-field 63Cu nuclear quadrupole resonance (NQR) study of nonmagnetic Mg impurity substituted Cu1-xMgxGeO3 (single crystals; the spin-Peierls transition temperature Tsp~14, 13.5, and 11 K for x=0, 0.0043, and 0.020) in a temperature range from 4.2 K to 250 K. We found that below T*~77 K, Cu NQR spectra are broadened and nonexponential Cu nuclear spin-lattice relaxation increases for undoped and more remarkably for Mg-doped samples. The results indicate that random lattice distortion and impurity-induced spins appear below T*, which we associate with a precursor of the spin-Pei…
We have performed detailed x-ray scattering measurements on single crystals of the spin-Peierls compound TiOBr in order to study the critical properties of the transition between the incommensurate spin-Peierls state and the paramagnetic state at Tc2 ~ 48 K. We have determined a value of the critical exponent beta which is consistent with the conventional 3D universality classes, in contrast with earlier results reported for TiOBr and TiOCl. Using a simple power law fit function we demonstrate that the asymptotic critical regime in TiOBr is quite narrow, and obtain a value of beta_{asy} = 0.32…
Pressure-dependent transmittance and reflectance spectra of TiOBr and TiOCl single crystals at room temperature suggest the closure of the Mott-Hubbard gap, i.e., the gap is filled with additional electronic states extending down to the far-infrared range. According to pressure-dependent x-ray powder diffraction data the gap closure coincides with a structural phase transition. The transition in TiOBr occurs at slightly lower pressure ($p$=14 GPa) compared to TiOCl ($p$=16 GPa) under hydrostatic conditions, which is discussed in terms of the chemical pressure effect. The results of pressure-de…
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 investigate the Peierls transition in the one-dimensional Peierls-Hubbard model at half filling in the adiabatic approximation for the lattice. Depending on the value of the electron-lattice coupling constant g the equilibrium dimerization can be either enhanced or suppressed by the Hubbard interaction U. Applying second order perturbation theory we determine the critical value g_c = 0.689348 below which the Hubbard interaction enhances the dimerization.
We consider the ground state and the elementary excitations of an array of spin-Peierls chains coupled by elastic and magnetic interactions. It is expected that the effect of the magnetic interchain coupling will be to reduce the dimerization amplitude and that of the elastic coupling will be to confine the spin one-half solitons corresponding to each isolated chain. We show that this is the case when these interactions are not frustrated. On the other hand, in the frustrated case we show that the amplitude of dimerization in the ground state is independent of the strength of the interchain ma…
We study the unoccupied electronic structure of the spin-1/2 quantum magnet TiOCl by x-ray absorption near-edge spectroscopy (XANES) at the Ti L and O K edges. Data is acquired both in total electron and fluorescence yield mode (TEY and FY, respectively). While only the latter allows to access the unconventional low-temperature spin-Peierls (SP) phase of TiOCl the signal is found to suffer from significant self-absorption in this case. Nevertheless, we conclude from FY data that effects of the SP distortion on the electronic structure are absent within experimental accuracy. The similarity of …
We consider a chain of atoms that are bound together by a harmonic force. Spin-1/2 electrons that move between neighboring chain sites (Hückel model) induce a lattice dimerization at half band filling (Peierls effect). We supplement the Hückel model with a local Hubbard interaction and a long-range Ohno potential, and calculate the average bond-length, dimerization, and optical phonon frequencies for finite straight and zig-zag chains using the density-matrix renormalization group (DMRG) method. We check our numerical approach against analytic results for the Hückel model. The Hubbard interact…
We demonstrate that a Peierls dimerization can occur in ferromagnetic spin chains activated by thermal fluctuations. The dimer order parameter and entanglement measures are studied as functions of the modulation of the magnetic exchange interaction and temperature, using a spin-wave theory and the density-matrix renormalization group. We discuss the case where a periodic modulation is caused by spin-phonon coupling and the case where electronic states effectively induce such a modulation. The importance of the latter for a number of transition metal oxides is highlighted.
The spin$-1/2$ chain with ferromagnetic exchange $J_1 < 0$ between first neighbors and antiferromagnetic $J_2 > 0$ between second neighbors supports two spin-Peierls (SP) instabilities depending on the frustration $α= J_2/\vert J_1\vert$. Instead of chain dimerization with two spins per unit cell, $J_1-J_2$ models with $α> 0.65$ and linear spin-phonon coupling are unconditionally unstable to sublattice dimerization with four spins per unit cell. Unequal $J_1$ to neighbors to the right and left extends the model to gapped ($γ> 0$) chains with conditional SP transitions at $T_{SP}$ to dimerized …
The two-dimensional Peierls-Hubbard model is studied at half-filling within both Hartree-Fork and Kotliar-Ruckenstein slave-boson theory. The interplay between two types of long-range order, bond-order wave (BOW) and antiferromagnetism (AFM), is analysed for two representative dimerization patterns, corresponding both to the same wavevector $(π,π)$. For each pattern, the Peierls dimerization (and associated BOW) is weakened and finally suppressed with increasing Hubbard on-site interaction, and correspondingly AFM is gradually enhanced. In particular, a coexistence regime with both BOW and AFM…
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 …
The spin-$1/2$ chain with antiferromagnetic exchange $J_1$ and $J_2 = αJ_1$ between first and second neighbors, respectively, has both gapless and gapped ($Δ(α) > 0$) quantum phases at frustration $0 \le α\le 3/4$. The ground state instability of regular ($δ= 0$) chains to dimerization ($δ> 0$) drives a spin-Peierls transition at $T_{SP}(α)$ that varies with $α$ in these strongly correlated systems. The thermodynamic limit of correlated states is obtained by exact treatment of short chains followed by density matrix renormalization calculations of progressively longer chains. The doubly degene…
We use exact diagonalization combined with mean-field theory to investigate the phase diagram of the spin-orbital model for cubic vanadates. The spin-orbit coupling competes with Hund's exchange and triggers a novel phase, with the ordering of $t_{2g}$ orbital magnetic moments stabilized by the tilting of VO$_6$ octahedra. It explains qualitatively spin canting and reduction of magnetization observed in YVO$_3$. At finite temperature an orbital Peierls instability in the $C$-type antiferromagnetic phase induces modulation of magnetic exchange constants even in absence of lattice distortions. T…
TiPO$_4$ is a Mott insulator and one of few inorganic compounds featuring a spin-Peierls phase at low temperature. Recent experimental studies have suggested the presence of spin-Peierls dimerization also at ambient temperature though at high pressure. Here, we present a combined experimental and theoretical study of the energetics of the high-pressure phase. We analyse dimerization properties and their coupling to spin degrees of freedom. Most importantly, we argue that TiPO$_4$ resents a direct analogue to the celebrated binary transition metal oxide VO$_2$. TiPO$_4$ allows to assess spin-di…
The effect of correlation on Peierls transition, which is accompanied by a dimerization, t_d, of a bond alternation for transfer energy, has been examined for a half-filled one-dimensional electron system with on-site repulsive interaction (U). By applying the renormalization group method to the interaction of the bosonized Hamiltonian, the dimerization has been calculated variationally and self-consistently with a fixed electron-phonon coupling constant (λ) and it is shown that t_d takes a maximum as a function of U. The result is examined in terms of charge gap and spin gap and is compared w…
Impurity-induced magnetic order has been observed in many quasi-1D systems including doped variants of the spin-Peierls system CuGeO3. TiOCl is another quasi-1D quantum magnet with a spin-Peierls ground state, and the magnetic Ti sites of this system can be doped with non-magnetic Sc. To investigate the role of non-magnetic impurities in this system, we have performed both zero field and longitudinal field muSR experiments on polycrystalline Ti1-xScxOCl samples with x = 0, 0.01, and 0.03. We verified that TiOCl has a non-magnetic ground state, and we found no evidence for spin freezing or magn…
We investigate the microscopic dynamics at the initial stage of photoinduced phase transitions in tetrathiafulvalene-$p$-chloranil by exact diagonalization. We first show that the one-dimensional extended Peierls-Hubbard model exhibits a neutral phase with small ionicity and negligible dimerization and an ionic phase with moderate ionicity and dimerization. Aside from these phases, we find a doubly ionized phase with strong dimerization that we call the "dipole" phase. These ground-state phases are characterized by various order parameters and the Zak phase, which is relevant to electronic pol…
The spin-Peierls transition in the ground state of a quasi-one-dimensional spin-1/2 Heisenberg model coupled to adiabatic bond phonons is studied using a quantum Monte Carlo (QMC) method. The transition from a gapless Neel state to a spin-gapped Peierls state is explored in the parameter space spanned by the spatial anisotropy and the strength of spin-lattice coupling. It is found that for any finite inter-chain coupling, the transition to a dimerized Peierls ground state occurs only when the spin-lattice coupling exceeds a finite, non-zero critical value. This is in contrast to the pure 1D mo…
ESR of the pure monocrystals of CuGeO3 is studied in the frequency range 9-75 GHz and in the temperature interval 1.2-25 K. The splitting of the ESR line into several spectral components is observed below 5 K, in the temperature range where the magnetic susceptibility is suppressed by the spin-Peierls dimerization. The analysis of the magnetic resonance signals allows one to separate the signals of the S=1/2- and S=1 defects of the spin-Peierls phase. The value of g-factor of these signals is close to that of the Cu-ion. The additional line of the magnetic resonance is characterized by an anom…
Using {\it ab initio} density functional theory and single-orbital Hubbard model calculations via the density matrix renormalization group method, we systematically studied the monolayer VOI$_2$ with a $3d^1$ electronic configuration. Our phonon calculations indicate that the orthorhombic $Pmm2$ FE-II phase is the most likely ground state, involving a ferroelectric distortion along the $a$-axis and V-V dimerization along the $b$-axis. Specifically, the "pseudo Jahn-Teller" effect caused by the coupling between empty V ($d_{xz/yz}$ and $d_{3z^2-r^2}$) and O $2p$ states is proposed as the mechan…
We add a Heisenberg interaction term $\proptoλ$ in the one-dimensional SU(2)$\otimes$XY spin-orbital model introduced by B. Kumar. At $λ=0$ the spin and orbital degrees of freedom can be separated by a unitary transformation leading to an exact solution of the model. We show that a finite $λ>0$ leads to spontaneous dimerization of the system which in the thermodynamic limit becomes a smooth phase transition at $λ\to 0$, whereas it remains discontinuous within the first order perturbation approach. We present the behavior of the entanglement entropy, energy gap and dimerization order parameter …
We investigate the effect of dipolar interactions in one-dimensional systems in connection with the possibility of observing exotic many-body effects with trapped atomic and molecular dipolar gases. By combining analytical and numerical methods, we show how the competition between short- and long-range interactions gives rise to frustrating effects which lead to the stabilization of spontaneously dimerized phases characterized by a bond-ordering. This genuine quantum order is sharply distinguished from Mott and spin-density wave phases, and can be unambiguously probed by measuring non local or…
We consider the one-dimensional extended Hubbard model in the presence of an explicit dimerization $δ$. For a sufficiently strong nearest neighbour repulsion we establish the existence of a quantum phase transition between a mixed bond-order wave and charge-density wave phase from a pure bond-order wave phase. This phase transition is in the universality class of the two-dimensional Ising model.
We report a synchrotron x-ray scattering study of the diluted spin-Peierls (SP) material Cu_{1-x}Mg_xGeO_3. In a recent paper we have shown that the SP dimerization attains long-range order only for x < x_c = 0.022(0.001). Here we report that the SP transition is reentrant in the vicinity of the critical concentration x_c. This is manifested by broadening of the SP dimerization superlattice peaks below the reentrance temperature, T_r, which may mean either the complete loss of the long-range SP order or the development of a short-range ordered component within the long-range ordered SP state. …
We reexamine the dimerization, the charge and the spin gaps of a half-filled Peierls-Hubbard chain by means of the incremental expansion technique. Our numerical findings are in significant quantitative conflict with recently obtained results by M. Sugiura and Y. Suzumura [J. Phys. Soc. Jpn. v. 71 (2002) 697] based on a bosonization and a renormalization group method, especially with respect to the charge gap. Their approach seems to be valid only in the weakly correlated case.
The spin-Peierls transition is modeled in the dimer phase of the spin-$1/2$ chain with exchanges $J_1$, $J_2 = αJ_1$ between first and second neighbors. The degenerate ground state generates an energy cusp that qualitatively changes the dimerization $δ(T)$ compared to Peierls systems with nondegenerate ground states. The parameters $J_1 = 160$ K, $α= 0.35$ plus a lattice stiffness account for the magnetic susceptibility of CuGeO$_3$, its specific heat anomaly, and the $T$ dependence of the lowest gap.
We report the presence of spin dimerization in the ground state of the one dimensional Kondo lattice model at quarter filling. The emergence of this new phase of the Kondo lattice can be traced to the form of the RKKY interaction between the localized moments and provides the first example of dimerization induced indirectly by itinerant electrons. We propose this dimer ordering as the driving mechanism of the spin-Peierls phase observed in the quasi-one-dimensional organic compounds (Per)$_{2}$M(mnt)$_{2}$ (M=Pt, Pd). Moreover, this suggests that a richer phase diagram than the Doniach paradig…
We have calculated the magnetic excitation spectrum in frustrated and dimerized spin 1/2 Heisenberg chains for model parameters which describe the thermodynamics and low frequency spin dynamics in the spin--Peierls system $CuGeO_{3}$. As a test the chosen model is found to reproduce the lowest Raman excitation energy near $30 cm^{-1}$ in the dimerized phase. We establish the elementary triplet and singlet excitation branches below the continuum and estimate the interchain coupling effects on the dimerization parameter.
We use the two cut-off renormalization group (RG) method to study the spin-Peierls model in one-dimension for the entire phonon frequency range. We integrate out the phonon and solve the effective Fermion system via mean field and RG methods. We make use of the symmetry that the Neel, dimerization, and spin current order parameters form an SU(2) triplet based on resolving the Fermion into left and right movers. We present the phase diagram and discuss its implications for the organic charge-transfer salt (TMTTF)$_2$PF$_6$.
We study the effects of opening of the band gap on the double exchange ferromagnetism. Applying the density-matrix renormalization group method and an analytical expansion from the dimer limit to the one-dimensional double exchange model, we demonstrate for a relevant region of the exchange coupling that, in the weak dimerization regime, the Peierls gap opens in the fully spin-polarized conduction band without affecting its ferromagnetism, whereas in the strong dimerization regime, the ferromagnetism is destroyed and the Mott gap opens instead, leading the system to the antiferromagnetic quasi…
We study the formation of antiferromagnetic correlations induced by impurity doping in anisotropic two-dimensional spin-Peierls systems. Using a mean-field approximation to deal with the inter-chain magnetic coupling, the intra-chain correlations are treated exactly by numerical techniques. The magnetic coupling between impurities is computed for both adiabatic and dynamical lattices and is shown to have an alternating sign as a function of the impurity-impurity distance, hence suppressing magnetic frustration. An effective model based on our numerical results supports the coexistence of antif…
A theory of the metal-insulator transition in vanadium dioxide from the high-temperature rutile to the low- temperature monoclinic phase is proposed on the basis of cluster dynamical mean field theory, in conjunction with the density functional scheme. The interplay of strong electronic Coulomb interactions and structural distortions, in particular the dimerization of vanadium atoms in the low temperature phase, plays a crucial role. We find that VO2 is not a conventional Mott insulator, but that the formation of dynamical V-V singlet pairs due to strong Coulomb correlations is necessary to tr…
The electronic properties of quarter-filled organic materials showing spin-Peierls transition are investigated theoretically. By studying the one-dimensional extended Peierls-Hubbard model analytically as well as numerically, we find that there is a competition between two different spin-Peierls states due to the tetramized lattice distortion in the strongly correlated regime. One is accompanied by lattice dimerization which can be interpreted as a spontaneous Mott insulator, while the other shows the existence of charge order of Wigner crystal-type. Results of numerical density matrix renorma…
A simple intuitive picture of spin-Peierls antiferromagnets arises from regarding the elementary excitations as S=1/2 solitons. In a strictly one-dimensional system these excitations are assumed not to form bound-states and to be repelled by impurities. Couplings to the three-dimensional lattice are assumed to produce an effective confining potential which binds solitons to antisolitons and to impurities, with the number of bound-states increasing as the interchain coupling goes to 0. We investigate these various assumptions numerically in a phononless model where spontaneous dimerization aris…
Photoinduced dynamics of charge density and lattice displacements is calculated by solving the time-dependent Schrödinger equation for a one-dimensional extended Peierls-Hubbard model with alternating potentials for the mixed-stack organic charge-transfer complex, TTF-CA. A pulse of oscillating electric field is incorporated into the Peierls phase of the transfer integral. The frequency, the amplitude, and the duration of the pulse are varied to study the nonlinear and cooperative character of the photoinduced transition. When the dimerized ionic phase is photoexcited, the threshold behavior i…
Using exact diagonalizations we consider self-consistently the lattice distortions in odd Peierls-Hubbard and spin-Peierls periodic rings in the adiabatic harmonic approximation. From the tails of the inherent spin soliton the dimerization d_\infty of regular even rings is found by extrapolations to infinite ring lengths. Considering a wide region of electron-electron onsite interaction values U>0 compared with the band width 4t_0 at intermediately strong electron-phonon interaction g, known relationships obtained by other methods are reproduced and/or refined within one unified approach: such…
The spin-Peierls transition at $T_{SP}$ of spin-$1/2$ chains with isotropic exchange interactions has previously been modeled as correlated for $T > T_{SP}$ and mean field for $T < T_{SP}$. We use correlated states throughout in the $J_1-J_2$ model with antiferromagnetic exchange $J_1$ and $J_2 = αJ_1$ between first and second neighbors, respectively, and variable frustration $0 \leq α\leq 0.50$. The thermodynamic limit is reached at high $T$ by exact diagonalization of short chains and at low $T$ by density matrix renormalization group calculations of progressively longer chains. In contrast …
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…
We report here on physical properties and lattice distortion in the new quasi-one-dimensional spin system TiOBr by x-ray diffraction experiment using synchrotoron radiation. Comparing the crystal structure between TiOBr and TiOCl, the difference of b-axis length plays a key role for physical properties in both systems. By using single crystal of TiOBr, superlattice reflections were observed at (0 1.5 0) and (0 2.5 0). The temperature dependence of superlattice reflections imply the first order transition at $T_{c1}$=27K. We analyzed the data using the simple dimerization model.
Dynamical properties of the novel inorganic spin-Peierls compound α'--NaV2O5 are investigated using a one-dimensional dimerized Heisenberg model. By exact diagonalizations of chains with up to 28 sites, supplemented by a finite-size scaling analysis, the dimerization parameter δis determined by requiring that the model reproduces the experimentally observed spin gap Δ. The dynamical and static spin structure factors are calculated. As for CuGeO3, the existence of a low energy magnon branch separated from the continuum is predicted. The present calculations also suggest that a large magnetic Ra…
