Optical properties and electronic structure of Ca-doped alpha'-NaV2O5

The dielectric function of alpha'-Na(1-x)Ca(x)V2O5 (0 < x < 20%) was measured for the a and b axes in the photon energy range 0.8-4.5 eV at room temperature. By varying the Ca-concentration we control the relative abundancy of V4+ and V5+. We observe that the intensity of the main optical absorption peak at 1 eV is proportional to the number of V5+ ions. This rules out the interpretation as a V4+ d-d excitation, and it establishes that this is the on-rung bonding-antibonding transition.Comment: 6 pages, ReVTeX, 5 figures in encapsulated postscript forma

Investigation of thermal and magnetic properties of defects in a spin-gap compound NaV2O5

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.Comment: 6 pages, 8 figure

Orthorhombic versus monoclinic symmetry of the charge-ordered state of NaV2O5

High-resolution X-ray diffraction data show that the low-temperature superstructure of alpha-NaV2O5 has an F-centered orthorhombic 2a x 2b x 4c superlattice. A structure model is proposed, that is characterized by layers with zigzag charge order on all ladders and stacking disorder, such that the averaged structure has space group Fmm2. This model is in accordance with both X-ray scattering and NMR data. Variations in the stacking order and disorder offer an explanation for the recently observed devils staircase of the superlattice period along c.Comment: REVTEX, 4 pages including 2 figures, shortened, submitted to PR

X-ray anomalous scattering investigations on the charge order in α′\alpha^\prime-NaV2_2O5_5

Anomalous x-ray diffraction studies show that the charge ordering in $\alpha^\prime$-NaV$_2$O$_5$ is of zig-zag type in all vanadium ladders. We have found that there are two models of the stacking of layers along \emph{c-}direction, each of them consisting of 2 degenerated patterns, and that the experimental data is well reproduced if the 2 patterns appears simultaneously. We believe that the low temperature structure contains stacking faults separating regions corresponding to the four possible patterns.Comment: Submitted to Phys. Rev. Lett., 4 pages, 4 eps figures inserted in the tex

Charge-ordering phase transition and order-disorder effects in the Raman spectra of NaV2O5

In the ac polarized Raman spectra of NaV2O5 we have found anomalous phonon broadening, and an energy shift of the low-frequency mode as a function of the temperature. These effects are related to the breaking of translational symmetry, caused by electrical disorder that originates from the fluctuating nature of the V {4.5+} valence state of vanadium. The structural correlation length, obtained from comparisons between the measured and calculated Raman scattering spectra, diverges at T< 5 K, indicating the existence of the long-range charge order at very low temperatures, probably at T=0 K.Comment: 8 pages, 4 figures, new version, to appear in PR

Dzyaloshinskii-Moriya interaction in NaV2_2O5_5: a microscopic study

We present a unified account of magnetic exchange and Raman scattering in the quasi-one-dimensional transition-metal oxide NaV$_2$O$_5$. Based on a cluster-model approach explicit expressions for the exchange integral and the Raman-operator are given. It is demonstrated that a combination of the electronic-structure and the Dzyaloshinskii-Moriya interaction, allowed by symmetry in this material, are responsible for the finite Raman cross-section giving rise to both, one- and two-magnon scattering amplitudes.Comment: 7 pages, 1 figur

Lattice vibrations of alpha'-NaV_2O_5 in the low-temperature phase. Magnetic bound states?

We report high resolution polarized infrared studies of the quarter-filled spin ladder compound alpha'-NaV_2O_5 as a function of temperature (5K <= T <= 300K). Numerous new modes were detected below the temperature T_c=34K of the phase transition into a charge ordered nonmagnetic state accompanied by a lattice dimerization. We analyse the Brillouin zone (BZ) folding due to lattice dimerization at T_c and show that some peculiarities of the low-temperature vibrational spectrum come from quadruplets folded from the BZ point (1/2, 1/2, 1/4). We discuss an earlier interpretation of the 70, 107, and 133cm-1 modes as magnetic bound states and propose the alternative interpretation as folded phonon modes strongly interacting with charge and spin excitations.Comment: 15 pages, 13 Postscript figure

Optical spectroscopic study of the interplay of spin and charge in NaV2O5

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.Comment: Revtex, 19 pages, 16 postscript pictures embedded in the text, submitted to PRB. Find more stuff at http://www.stanford.edu/~damascel/andreaphd.html or http://www.ub.rug.nl/eldoc/dis/science/a.damascelli

Photonic band gaps in materials with triply periodic surfaces and related tubular structures

We calculate the photonic band gap of triply periodic bicontinuous cubic structures and of tubular structures constructed from the skeletal graphs of triply periodic minimal surfaces. The effect of the symmetry and topology of the periodic dielectric structures on the existence and the characteristics of the gaps is discussed. We find that the C(I2-Y**) structure with Ia3d symmetry, a symmetry which is often seen in experimentally realized bicontinuous structures, has a photonic band gap with interesting characteristics. For a dielectric contrast of 11.9 the largest gap is approximately 20% for a volume fraction of the high dielectric material of 25%. The midgap frequency is a factor of 1.5 higher than the one for the (tubular) D and G structures

A microscopic model for the structural transition and spin gap formation in alpha'-NaV2O5

We present a microscopic model for alpha'-NaV2O5. Using an extended Hubbard model for the vanadium layers we derive an effective low-energy model consisting of pseudospin Ising chains and Heisenberg chains coupled to each other. We find a ``spin-Peierls-Ising'' phase transition which causes charge ordering on every second ladder and superexchange alternation on the other ladders. This transition can be identified with the first transition of the two closeby transitions observed in experiment. Due to charge ordering the effective coupling between the lattice and the superexchange is enhanced. This is demonstrated within a Slater-Koster approximation. It leads to a second instability with superexchange alternation on the charge-ordered ladders due to an alternating shift of the O sites on the rungs of that ladder. We can explain within our model the observed spin gap, the anomalous BCS ratio, and the anomalous shift of the critical temperature of the first transition in a magnetic field. To test the calculated superstructure we determine the low-energy magnon dispersion and find agreement with experiment.Comment: 32 pages, 12 figures include