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Register a new userStudy of spin-Peierls transition in alpha--NaV2O5 by infrared reflectivity
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Polarized infrared reflectivity measurements have been performed on single crystals of the spin-Peierls compound alpha-NaV2O5 in the temperature range 20-300 K. Pronounced spectral features associated with the formation of the dimerized phase were detected both in the a- and b-polarizations (perpendicular and parallel to the spin-1/2 chains, respectively). The temperature dependence of a salient spectral line at 718 cm^-1 sharply rising below the transition temperature T_SP obeys a (1-T/T_SP)^(2beta) law with T_SP simeq 34.3$K and beta simeq 0.25. In addition, a continuum signal is observed in the whole temperature range in the a-polarized optical conductivity spectra. In order to interpret these results, calculations of the static dimerization and of the optical conductivity based on a mean-field and a dynamical treatment of the lattice respectively are proposed.
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Infrared reflectance of alpha-NaV2O5 single crystals in the frequency range from 50 cm-1 to 10000 cm-1 was studied for a, b and c-polarisations. In addition to phonon modes identification, for the a-polarised spectrum a broad continuum absorption in the range of 1D magnetic excitation energies was found. The strong near-IR absorption band at 0.8 eV shows a strong anisotropy with vanishing intensity in c-polarisation. Activation of new phonons due to the lattice dimerisation were detected below 35K as well as pretransitional structural fluctuations up to 65K.
At room-temperature NaV2O5 was found to have the centrosymmetric space group Pmmn. This space group implies the presence of only one kind of V site in contrast with previous reports of the non-centrosymmetric counterpart P21mn. This indicates a non-integer valence state of vanadium. Furthermore, this symmetry has consequences for the interpretation of the transition at 34 K, which was ascribed to a spin-Peierls transition of one dimensional chains of V4+.
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 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 investigate the temperature dependent optical properties of NaV2O5, in the energy range 4meV-4eV. The symmetry of the system is discussed on the basis of infrared phonon spectra. By analyzing the optically allowed phonons at temperatures below and above the phase transition, we conclude that a second-order change to a larger unit cell takes place below 34 K, with a fluctuation regime extending over a broad temperature range. In the high temperature undistorted phase, we find good agreement with the recently proposed centrosymmetric space group Pmmn. On the other hand, the detailed analysis of the electronic excitations detected in the optical conductivity, provides direct evidence for a charge disproportionated electronic ground-state, at least on a locale scale: A consistent interpretation of both structural and optical conductivity data requires an asymmetrical charge distribution on each rung, without any long range order. We show that, because of the locally broken symmetry, spin-flip excitations carry a finite electric dipole moment, which is responsible for the detection of direct two-magnon optical absorption processes for E parallel to the a axis. The charged-magnon model, developed to interpret the optical conductivity of NaV2O5, is described in detail, and its relevance to other strongly correlated electron systems, where the interplay of spin and charge plays a crucial role in determining the low energy electrodynamics, is discussed.
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