Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userAnharmonic inter-layer bonding leads to intrinsically low thermal conductivity of bismuth oxychalcogenides
112
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
The anharmonicity of phonons in solid is ultimately rooted in the chemical bonding. However, the direct connection between phonon anharmoncity and chemical bonding is difficult to make experimentally or theoretically, due mainly to their complicated lattice structures. Here, with the help of density functional theory based calculations, we discovery that electrostatic inter-layer coupling in Bi$_2$O$_2$X (X=S,Se,Te) leads to intrinsically low lattice thermal conductivity. We explain our discovery by the strong anharmonic chemical bonding between Bi and chalcogen atoms. Our results shed light on the connection between inter-layer chemical bonding and phonon anharmonicity, which could be explored in a wide range of layered materials.
rate research
Read More
Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this work, we present an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles and develop a high-efficiency approach of discovering low $kappa_{rm L}$ materials by screening the local coordination environments of crystalline compounds. The followed first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from thirteen prototype crystal structures contained in the inorganic crystal structure database. Furthermore, we demonstrate an approach of rationally designing high-performance thermoelectrics by additionally incorporating cations with stereochemically active lone-pair electrons. Our results not only provide fundamental insights into the physical origin of the low lattice thermal conductivity in a large family of copper-based compounds but also offer an efficient approach to discovery and design materials with targeted thermal transport properties.
Half-Heusler compounds usually exhibit relatively higher lattice thermal conductivity that is undesirable for thermoelectric applications. Here we demonstrate by first-principles calculations and Boltzmann transport theory that the BiBaK system is an exception, which has rather low thermal conductivity as evidenced by very small phonon group velocity and relaxation time. Detailed analysis indicates that the heavy Bi and Ba atoms form a cage-like structure, inside which the light K atom rattles with larger atomic displacement parameters. In combination with its good electronic transport properties, the BiBaK shows a maximum n-type ZT value of 1.9 at 900 K, which outperforms most half-Heusler thermoelectric materials.
The low-temperature thermal conductivity in polycrystalline graphene is theoretically studied. The contributions from three branches of acoustic phonons are calculated by taking into account scattering on sample borders, point defects and grain boundaries. Phonon scattering due to sample borders and grain boundaries is shown to result in a $T^{alpha}$-behaviour in the thermal conductivity where $alpha$ varies between 1 and 2. This behaviour is found to be more pronounced for nanosized grain boundaries. PACS: 65.80.Ck, 81.05.ue, 73.43.Cd
Recently there has been paid much attention to phenomena caused by local anharmonic vibrations of the guest ions encapsulated in polyhedral cages of materials such as pyrochlore oxides, filled skutterdites and clathrates. We theoretically investigate the optical conductivity solely due to these so-called rattling phonons in a one-dimensional anharmonic potential model. The dipole interaction of the guest ions with electric fields induces excitations expressed as transitions among vibrational states with non-equally spaced energies, resulting in a natural line broadening and a shift of the peak frequency as anharmonic effects. In the case of a single well potential, a softening of the peak frequency and an asymmetric narrowing of the line width with decreasing temperature are understood as a shift of the spectral weight to lower level transitions. On the other hand, the case of a double minima potential leads to a multi-splitting of a spectral peak in the conductivity spectrum with decreasing temperature.
The optical conductivity and the spectral weight of four topological insulators with increasing chemical compensation (Bi2Se3, Bi2-xCaxSe3, Bi2Se2Te, Bi2Te2Se) have been measured from 5 to 300 K and from sub-THz to visible frequencies. The effect of compensation is clearly observed in the infrared spectra, through the suppression of an extrinsic Drude term and the appearance of strong absorption peaks, that we assign to electronic transitions among localized states. From the far-infrared spectral weight of the most compensated sample (Bi2Te2Se) one can estimate a density of charge-carriers in the order of 10^17/cm^3 in good agreement with transport data. Those results demonstrate that the low-energy electrodynamics in single crystals of topological insulators, even at the highest degree of compensation presently achieved, is still affected by extrinsic charge excitations.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
