Novel rattling of K atoms in aluminium-doped defect pyrochlore tungstate.

نویسندگان

  • Elvis Shoko
  • Gordon J Kearley
  • Vanessa K Peterson
  • Hannu Mutka
  • Michael M Koza
  • Jun-ichi Yamaura
  • Zenji Hiroi
  • Gordon J Thorogood
چکیده

Rattling dynamics have been identified as fundamental to superconductivity in defect pyrochlore osmates and aluminium vanadium intermetallics, as well as low thermal conductivity in clathrates and filled skutterudites. Combining inelastic neutron scattering (INS) measurements and ab initio molecular dynamics (MD) simulations, we use a new approach to investigate rattling in the Al-doped defect pyrochlore tungstates: AAl0.33W1.67O6 (A = K, Rb, Cs). We find that although all the alkali metals rattle, the rattling of the K atoms is unique, not only among the tungstates but also among the analogous defect osmates, KOs2O6 and RbOs2O6. Detailed analysis of the MD trajectories reveals that two unique features set the K dynamics apart from the rest, namely, (1) quasi one-dimensional local diffusion within a cage, and (2) vibration at a range of frequencies. The local diffusion is driven by strongly anharmonic local potentials around the K atoms exhibiting a double-well structure in the direction of maximum displacement, which is also the direction of local diffusion. On the other hand, vibration at a range of frequencies is a consequence of the strong anisotropy in the local potentials around the K atoms as revealed by directional magnitude spectra. We present evidence to show that it is the smaller size rather than the smaller mass of the K rattler which leads to the unusual dynamics. Finally, we suggest that the occurrence of local diffusion and vibration at a range of frequencies in the dynamics of a single rattler, as found here for the K atoms, may open new possibilities for phonon engineering in thermoelectric materials.

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

منابع مشابه

Novel vortex distribution in the β-pyrochlore superconductor KOs2O6

By utilizing the micro-Hall probe array, we study the superconducting and the vortex states in a single crystal of KOs2O6 near the first-order transition at Tp ∼ 8 K, which is associated with a change in the rattling motion of K ions. We show that below the first-order transition, the lower critical field exhibits a distinct decrease, suggesting that the electron-phonon coupling is weakened bel...

متن کامل

Tm-doped TiO2 and Tm2Ti2O7 pyrochlore nanoparticles: enhancing the photocatalytic activity of rutile with a pyrochlore phase

Tm-doped TiO2 nanoparticles were synthesized using a water-controlled hydrolysis reaction. Analysis was performed in order to determine the influence of the dopant concentration and annealing temperature on the phase, crystallinity, and electronic and optical properties of the resulting material. Various characterization techniques were utilized such as X-ray diffraction, Raman spectroscopy, X-...

متن کامل

Fast ion conductivity in strained defect-fluorite structure created by ion tracks in Gd2Ti2O7

The structure and ion-conducting properties of the defect-fluorite ring structure formed around amorphous ion-tracks by swift heavy ion irradiation of Gd2Ti2O7 pyrochlore are investigated. High angle annular dark field imaging complemented with ion-track molecular dynamics simulations show that the atoms in the ring structure are disordered, and have relatively larger cation-cation interspacing...

متن کامل

Preparation of Camera-ready Typescript:

The potassium double tungstates KGd(WO4)2, KY(WO4)2, and KLu(WO4)2 are excellent candidates for solid-state lasers, see Ref. [1] and Refs. therein, because of their high refractive index of ~2.02.1, the large transition cross-sections of rare-earth (RE) ions doped into these hosts, the possibility to incorporate very large concentrations of RE 3+ ions, reaching the stoichiometric structure KRE(...

متن کامل

ذخیره در منابع من


  با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

عنوان ژورنال:
  • Journal of physics. Condensed matter : an Institute of Physics journal

دوره 26 30  شماره 

صفحات  -

تاریخ انتشار 2014