Materials based on cubic tetrahedrites (Cu$_{12}$Sb$_{4}$S$_{13}$) are useful thermoelectrics with unusual thermal and electrical transport properties, such as very low and nearly temperature-independent lattice thermal conductivity ($κ_{L}$). We explain the microscopic origin of the glass-like $κ_{L}$ in Cu$_{12}$Sb$_{4}$S$_{13}$ by explicitly treating anharmonicity up to quartic terms for both phonon energies and phonon scattering rates. We show that the strongly unstable phonon modes associated with trigonally coordinated Cu atoms are anharmonically stabilized above approximately $100$ K and continue hardening with increasing temperature, in accord with experimental data. This temperature induced hardening effect reduces scattering of heat carrying acoustic modes by reducing the available phase space for three-phonon processes, thereby balancing the conventional $\propto T$ increase in scattering due to phonon population and yielding nearly temperature-independent $κ_{L}$. Furthermore, we find that very strong phonon broadening lead to a qualitative breakdown of the conventional phonon-gas model and modify the dominant heat transport mechanism from the particle-like phonon wave packet propagation to incoherent tunneling described by off-diagonal terms in the heat-flux operator, which are typically prevailing in glasses and disordered crystals. Our work paves the way to a deeper understanding of glass-like thermal conductivity in complex crystals with strong anharmonicity.
The origin of the spin-glass state in (Fe,Sn)4N alloys is studied on the basis of a Heisenberg Hamiltonian with parameters derived from first principles within the magnetic force theorem applied in the framework of the disordered local moments method and local spin-density approximation. We show that in the alloy concentration range where the spin-glass state is stable only one Fe sublattice is intrinsically magnetic and the interatomic exchange magnetic interactions are essentially short ranged due to effects of chemical and magnetic disorder. The magnetic Fe atoms with well-localized spin mo…
The study of the ferrites YBaFe4-xGaxO7 shows that the substitution of Ga for Fe in YBaFe4O7 stabilizes the hexagonal symmetry for 0.40 < x < 0.70, at the expense of the cubic one. Using combined measurements of a. c. and d. c. magnetization, we establish that Ga substitution for Fe in YBaFe4O7 leads to an evolution from a geometrically frustrated spin glass (for x = 0) to a cationic disorder induced spin glass (x = 0.70). We also find an intermediate narrow range of doping where the samples are clearly phase separated having small ferrimagnetic clusters embedded in a spin glass matrix. The or…
A systematic investigation has been performed to elucidate effects of Rare-Earth (RE) type and local atomic configuration on magnetic properties of icosahedral quasicrystal (iQC) and their cubic approximants (2/1 and 1/1 ACs) in the ternary Cd-Mg-RE (RE = Gd, Tb, Dy, Ho, Er, and Tm) systems. At low temperatures, iQC and 2/1 ACs exhibit spin-glass-like freezing for RE = Gd, Tb, Dy, and Ho, while Er and Tm systems do not show freezing behaviour down to the base temperature ~ 2 K. The 1/1 ACs exhibit either spin-glass-like freezing or antiferromagnetic (AFM) ordering depending on their constituen…
Melting temperatures at ambient pressure of systems of isosceles Lennard-Jones trimers with angles ranging from 70 degrees to 100 degrees are determined. Two crystal structures are considered: a distorted body centered cubic structure and a distorted face centered cubic structure with preferred angles of 77 and 96 degrees, respectively. Liquid dynamics are slowed down when the angle is increased. A trimer angle of 83 degrees yields the largest distance between isochrones and the melting temperature, suggesting that this value gives the optimal glass-forming ability. It is conjectured that bett…
We combine the results of magnetic and transport measurements with Mossbauer spectroscopy and room-temperature diffraction data to construct the magnetic phase diagram of the new family of cubic perovskite manganites SrMn_1-xFe_xO_3. We have found antiferromagnetic ordering for lightly and heavily Fe-substituted material, while intermediate substitution leads to spin-glass behavior. Near the SrMn_0.5Fe_0.5O_3 composition these two types of ordering are found to coexist and affect one another. The spin glass behavior may be caused by competing ferro- and antiferromagnetic interactions among Mn^…
The low temperature behavior of densely packed interacting spherical single domain nanoparticles (MNP) is investigated by Monte Carlo simulations in the framework of an effective one spin model. The particles are distributed through a hard sphere like distribution with periodic boundary conditions and interact through the dipole dipole interaction (DDI) with an anisotropy energy including both cubic and uniaxial symmetry components. The cubic component is shown to play a sizable role on the value of the blocking temperature $T_b$ only when the MNP easy axes are parallel to the cubic easy direc…
An analysis of thermal transients from non-equilibrium ab initio molecular-dynamics simulations can be used to calculate the thermal conductivity of materials with a short phonon mean-free path. We adapt the approach-to-equilibrium methodology to the three-dimensional case of a simulation that consists of a cubic core region at higher temperature approaching thermal equilibrium with a thermostatted boundary. This leads to estimates of the lattice thermal conductivity for the glassy state of the phase-change memory material, Ge$_2$Sb$_2$Te$_5$, which are close to previously reported experimenta…
The nature of the cubic-like state in the lead-free piezoelectric ceramics 0.5K0.5Na0.5NbO3-0.5Na0.5Bi0.5TiO3 (KNN-50BNT) has been examined in detail by synchrotron x-ray diffraction (SD), selected area electron diffraction (SAED), neutron diffraction (ND), and temperature dependent dielectric characterization. The SD pattern of KNN-50BNT presents a pure perovskite structure with pseudocubic symmetry. However, superlattice reflections were observed by SAED and completely indexed by tetragonal symmetry with P4bm space group in ND pattern. The relaxor behavior of KNN-50BNT is compared with Pb-ba…
Below 1 K, the specific heat Cp of glasses depends approximately linearly on temperature T, in contrast with the cubic dependence observed in crystals, and which is well understood in terms of the Debye theory. That linear contribution has been ascribed to the existence of two-level systems as postulated by the Tunnelling Model. Therefore, a least-squares linear fit Cp = C_1 T + C_3 T^3 has been traditionally used to determine the specific-heat coefficients, though systematically providing calorimetric cubic coefficients exceeding the elastic coefficients obtained from sound-velocity measureme…
Type-I clathrate compounds have attracted a great deal of interest in connection with the search for efficient thermoelectric materials. These compounds constitute networked cages consisting of nano-scale tetrakaidecahedrons (14 hedrons) and dodecahedrons (12 hedrons), in which the group 1 or 2 elements in the periodic table are encaged as the so-called rattling guest atom. It is remarkable that, though these compounds have crystalline cubic-structure, they exhibit glass-like phonon thermal conductivity over the whole temperature range depending on the states of rattling guest atoms in the tet…
Ultrasound velocity measurements of the orbital-degenerate frustrated spinel MgV$_2$O$_4$ are performed in the high-purity single crystal which exhibits successive structural and antiferromagnetic phase transitions, and in the disorder-introduced single crystal which exhibits spin-glass-like behavior. The measurements reveal that two-types of unusual temperature dependence of the elastic moduli coexist in the cubic paramagnetic phase, which are resolved by magnetic-field and disorder sensitivities: huge Curie-type softening with decreasing temperature, and concave temperature dependence with a…
Dynamical magnetism in the disordered cubic lattice material $γ$-${\rm Ba}_{3}{\rm CoNb}_{2}{\rm O}_{9}$
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH（柏林赫尔姆霍兹材料与能源有限公司）；Technische Universität Berlin（柏林工业大学）；University of Oslo（奥斯陆大学）；Freie Universität Berlin（柏林自由大学）；PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢勒研究所中子与μ子科学中心）；Helmholtz-Zentrum Dresden-Rossendorf (HZDR)（德累斯顿-罗斯多夫赫尔姆霍兹中心）；Diamond Light Source（钻石光源实验室）；Institut Laue-Langevin（朗之万研究所）
Nanocrystalline ribbons of inverse Heusler alloy Mn2Ni1.6Sn0.4 have been synthesised by melt spinning of the arc melted bulk precursor. The single phase ribbons crystallize into a cubic structure and exhibit very fine crystallite size of < 2 nm. Temperature dependent magnetization (M-T) measurements reveal that austenite (A)-martensite (M) phase transition begins at T~248 K and finishes at T~238 K during cooling cycle and these values increase to T~267 K and T~259 K while warming. In cooling cycle, the A-phase shows ferromagnetic (FM) ordering with a Curie temperature T~267 K, while both the F…
We report complex magnetic, magnetoresistance (MR) and magnetocaloric properties of Gd4RhAl and Tb4RhAl forming in the Gd4RhIn type cubic structure. Though the synthesis of the compounds was reported long ago, to our knowledge, no attempt was made to investigate the properties of these compounds. The present results of ac and dc magnetization, electrical resistivity and heat-capacity measurements down to 1.8 K establish that these compounds undergo antiferromagnetic order initially, followed by complex spin-glass features with decreasing temperature. These characteristic temperatures are: For …
Phonon spectrum of cubic barium zirconate is calculated from first principles using the density functional theory. Unstable phonon mode with the $R_{25}$ symmetry in the phonon spectrum indicates an instability of the cubic structure with respect to rotations of the oxygen octahedra. It is shown that the ground-state structure of the crystal is $I4/mcm$. In order to find the manifestations of the predicted instability, EXAFS measurements at the Ba $L_{\rm III}$-edge are used to study the local structure of BaZrO$_3$ at 300 K. An enhanced value of the Debye-Waller factor for the Ba-O atomic pai…
We report the synthesis, structure, and magnetic and transport properties of a new ternary intermetallic compound PrRhSn3 which crystallizes in LaRuSn3-type cubic structure (space group Pm-3n). At low applied fields the dc magnetic susceptibility exhibits a sharp anomaly below 6~K with an irreversible behavior in zero field cooled (ZFC) and field cooled (FC) susceptibility below 5.5 K. The ac susceptibility exhibits a frequency dependent anomaly revealing a spin-glass behavior with a freezing temperature, T_f = 4.3 K. The observation of spin-glass behavior is further supported by a very slow d…
Solid He-4 is viewed as a nearly perfect Debye solid. Yet, recent calorimetry measurements by the PSU group (J. Low Temp. Phys. 138, 853 (2005) and Nature 449, 1025 (2007)) indicate that at low temperatures the specific heat has both cubic and linear contributions. These features appear in the same temperature range where measurements of the torsional oscillator period suggest a supersolid transition. We analyze the specific heat and compare the measured with the estimated entropy for a proposed supersolid transition with 1% superfluid fraction and find that the observed entropy is too small. …
It has been known for decades that thermal conductivity of insulating crystals becomes proportional to the inverse of temperature when the latter is comparable to or higher than the Debye temperature. This behavior has been understood as resulting from Umklapp scattering among phonons. We put under scrutiny the magnitude of the thermal diffusion constant in this regime and find that it does not fall below a threshold set by the square of sound velocity times the Planckian time ($τ_p=\hbar/k_BT$). The conclusion, based on scrutinizing the ratio in cubic crystals with high thermal resistivity, a…
