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Register a new userEnhanced dimerization of TiOCl under pressure: spin-Peierls - to - Peierls transition
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Added by
Francisco Rivadulla Fernandez
Publication date
2008
fields
Physics
and research's language is
English
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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.
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We report experimental results on the heat conductivity kappa of 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 kappa, 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 suppression of kappa in the intermediate phase which extends even to temperatures higher than Tc2. An external magnetic field causes a slight downshift of the transition at Tc1 and enhances the suppression of kappa up to Tc2. We interprete our findings in terms of strong spin-phonon coupling and phonon scattering arising from spin-driven lattice distortions.
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 with x-rays are crucial in determining the ground-state physics in this quantum magnet. In ambient pressure, TiOCl exhibits a transition to an incommensurate nearly dimerized state at $T_{c2}=92$ K and to a commensurate dimerized state at $T_{c1}=66$ K. Here, we discover a rich phase diagram as a function of temperature and pressure using x-ray diffraction on a single crystal in a diamond anvil cell down to $T=4$ K and pressures up to 14.5 GPa. Remarkably, the magnetic interaction scale increases dramatically with increasing pressure, as indicated by the high onset temperature of the spin-Peierls phase. At $sim$7 GPa, the extrapolated onset of the spin-Peierls phase occurs above $T=300$ K, indicating a quantum singlet state exists at room temperature. Further comparisons are made with the phase diagrams of related spin-Peierls systems that display metallicity and superconductivity under pressure.
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-dimer physics in the high-pressure regime in a controlled fashion, having the potential to become an important model system representative of the class of dimerized transition metal oxides.
We investigated the infrared reflectivity of several Mg- and Si-substituted CuGeO3 single crystals. The temperature dependent b-axis and c-axis optical response is reported. For T<Tsp we detected the activation of zone-boundary phonons along the b axis of the crystal on the pure sample and for 1% Mg and 0.7% Si concentrations. From a detailed analysis of the phonon parameters the redshift of the B2u mode at 48 cm^-1 is observed and discussed in relation to the soft mode expected to drive the spin-Peierls phase transition in CuGeO3. Moreover, the polarization dependence of a magnetic excitation measured in transmission at 44 cm^-1 has been investigated.
We predict the new type of phase transition in quasi one-dimensional system of interacting electrons at high magnetic fields, the stabilization of a density wave which transforms a two dimensional open Fermi surface into a periodic chain of large pockets with small distances between them. We show that quantum tunneling of electrons between the neighboring closed orbits enveloping these pockets transforms the electron spectrum into a set of extremely narrow energy bands and gaps that decreases the total electron energy, thus leading to a emph{magnetic breakdown induced density wave} ground state analogous to the well-known instability of Peierls type.
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