Dual-frequency resonant phonon scattering in BaxRyCo4Sb12 (R=La, Ce and Sr)

Low temperature transport properties of polycrystalline dual-element-filled skutterudites BaxRyCo4Sb12 (R=La, Ce, and Sr) are reported. Remarkably the combination of Ba and La or Ba and Ce is much more effective in reducing lattice thermal conductivity (κL) than Ba and Sr. The density-functional theory calculations and experimental data suggest that multiple-filled skutterudites using filler elements of different chemical natures, such as the rare earths, the alkaline earths, or the alkalines provide a broader range of resonant phonon scattering. The thermoelectric figure of merit of filled skutterudites can likely be improved by means of such multiple-element void filling.

[1]  Ctirad Uher,et al.  Chapter 5 Skutterudites: Prospective novel thermoelectrics , 2001 .

[2]  Kresse,et al.  Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. , 1996, Physical review. B, Condensed matter.

[3]  G. Meisner,et al.  Strain field fluctuation effects on lattice thermal conductivity of ZrNiSn-based thermoelectric compounds , 2004 .

[4]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[5]  Randeria,et al.  Low-temperature properties of a model glass. II. Specific heat and thermal transport. , 1990, Physical review. B, Condensed matter.

[6]  M. Wagner INFLUENCE OF LOCALIZED MODES ON THERMAL CONDUCTIVITY , 1963 .

[7]  B. Sales,et al.  Lattice dynamics and reduced thermal conductivity of filled skutterudites , 1999, cond-mat/9906028.

[8]  O. Leupold,et al.  Strongly decoupled europium and iron vibrational modes in filled skutterudites , 2005 .

[9]  P. Klemens Thermal Conduction In Solids , 1976 .

[10]  C. Uher,et al.  Transmission of phonons through grain boundaries in diamond films , 1993 .

[11]  C. Uher,et al.  Effect of Sn substituting for Sb on the low-temperature transport properties of ytterbium-filled skutterudites , 2003 .

[12]  Terry M. Tritt,et al.  Recent trends in thermoelectric materials research , 2001 .

[13]  R. K. Williams,et al.  Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials , 1996, Science.

[14]  B. Sales,et al.  FILLED SKUTTERUDITE ANTIMONIDES : ELECTRON CRYSTALS AND PHONON GLASSES , 1997 .

[15]  M. Wagner Resonance Scattering of Phonons by Molecular Impurity Centers , 1964 .

[16]  E. F. Steigmeier,et al.  Scattering of Phonons by Electrons in Germanium-Silicon Alloys , 1964 .

[17]  G. A. Slack,et al.  Nonmetallic crystals with high thermal conductivity , 1973 .

[18]  H. Matsunami,et al.  Phonon‐electron scattering in single crystal silicon carbide , 1993 .

[19]  R. Pohl Thermal Conductivity and Phonon Resonance Scattering , 1962 .

[20]  P. Klemens The Scattering of Low-Frequency Lattice Waves by Static Imperfections , 1955 .

[21]  T. Geballe,et al.  Isotopic and Other Types of Thermal Resistance in Germanium , 1958 .

[22]  G. A. Slack,et al.  Thermal Conductivity and Phonon Scattering by Magnetic Impurities in CdTe , 1964 .

[23]  C. Uher Thermal conductivity of high-Tc superconductors , 1990 .

[24]  S. Kanzaki,et al.  Hot Isostatic Pressing to Increase Thermal Conductivity of Si_3N_4 Ceramics , 1999 .

[25]  P. Klemens Thermal Conductivity and Lattice Vibrational Modes , 1958 .

[26]  G. Kresse,et al.  Ab initio molecular dynamics for liquid metals. , 1993 .

[27]  P. Klemens,et al.  The thermal conductivity of dielectric solids at low temperatures (Theoretical) , 1951, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[28]  B. Sales,et al.  Structural, magnetic, thermal, and transport properties of X{sub 8}Ga{sub 16}Ge{sub 30} (X=Eu,Sr,Ba) single crystals , 2001 .

[29]  C. Uher,et al.  Influence of electron-phonon interaction on the lattice thermal conductivity of Co1-xNixSb3 , 2002 .

[30]  B. Abeles Lattice Thermal Conductivity of Disordered Semiconductor Alloys at High Temperatures , 1963 .

[31]  Donald T. Morelli,et al.  Low temperature properties of the filled skutterudite CeFe4Sb12 , 1995 .

[32]  E. J. Freeman,et al.  Localized vibrational modes in metallic solids , 1998, Nature.

[33]  George S. Nolas,et al.  Semiconducting Ge clathrates: Promising candidates for thermoelectric applications , 1998 .