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Register a new userInversion symmetry in the spin-Peierls compound NaV2O5
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Authors
A. Meetsma
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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+.
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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.
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.
We discuss the symmetry of NaV2O5 in the high temperature phase on the basis of optical conductivity data. Conclusive information cannot be obtained by studying the optically allowed lattice vibrations. However, intensity and polarization of the electronic excitations give a direct indication for a broken-parity electronic ground-state. This is responsible for the detection of charged bi-magnons in the optical spectrum.
The specific heat, magnetic susceptibility and ESR signals of a Na-deficient vanadate Na_xV_2O_5 (x=1.00 - 0.90) were studied in the temperature range 0.07 - 10 K, well below the transition point to a spin-gap state. The contribution of defects provided by sodium vacancies to the specific heat was observed. It has a low temperature part which does not tend to zero till at least 0.3 K and a high temperature power-like tail appears above 2 K. Such dependence may correspond to the existence of local modes and correlations between defects in V-O layers. The magnetic measurements and ESR data reveal S=1/2 degrees of freedom for the defects, with their effective number increasing in temperature and under magnetic field. The latter results in the nonsaturating magnetization at low temperature. No long-range magnetic ordering in the system of defects was found. A model for the defects based on electron jumps near vacancies is proposed to explain the observed effects. The concept of a frustrated two-dimensional correlated magnet induced by the defects is considered to be responsible for the absence of magnetic ordering.
Polarized far-infrared (FIR) spectroscopic measurements and FIR magneto-optical studies were performed on the inorganic spin-Peierls compound CuGeO_3. An absorption line, which was found at 98 cm$^{-1}$ in the dimerized phase (D phase), was assigned to a folded phonon mode of B$_{3u}$ symmetry. The splitting of the folded mode into two components in the incommensurate phase (IC phase) has been observed for the first time. A new broad absorption centered at 63 cm$^{-1}$ was observed only in the ${bf E}parallel b$ axis polarization, which was assigned to a magnetic excitation from singlet ground state to a continuum state.
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