Modeling the thermal conductivities of the zinc antimonides ZnSb and Zn<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mrow /><mml:mn>4</mml:mn></mml:msub></mml:math>Sb<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mrow /><mml:mn>3</mml:mn></mml:msub></mml:math>

Bjerg, Lasse; Iversen, Bo B.; Madsen, Georg K. H.

doi:10.1103/physrevb.89.024304

Cited by 122 publications

(91 citation statements)

References 47 publications

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“…The according coefficients are listed in Table 1. Bjerg et al recently reported Debye temperatures which were derived from the DFT-calculated heat capacity of ZnSb employing the Slack definition [18]. The value specified for ZnSb (Θ D,Slack = 92 K) appears to be significantly lower than the experimental value of this study, which is derived from heat capacity measurements using a Debye-Einstein model (Θ D,Cp = 250 K), see above and Table 1.…”

Section: B Heat Capacity Measurementsmentioning

confidence: 68%

“…The presence of localized low energy optic modes as a consequence of multicenter bonded structural entities would provide a sound physical basis for the low thermal conductivity. This hypothesis has been put forward earlier [16], and recent theoretical investigations by Jund et al [17] and Bjerg et al [18] seem to confirm it, strongly questioning the empirical concept of "dumbbell" rattling recently pursued for Zn 4 Sb 3 [11].…”

Section: Introductionmentioning

confidence: 90%

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Thermal and vibrational properties of thermoelectric ZnSb: Exploring the origin of low thermal conductivity

et al. 2015

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The intermetallic compound ZnSb is an interesting thermoelectric material, largely due to its low lattice thermal conductivity. The origin of the low thermal conductivity has so far been speculative. Using multi-temperature single crystal X-ray diffraction (9 -400 K) and powder X-ray diffraction (300 -725 K) measurements we characterized the volume expansion and the evolution of structural properties with temperature and identify an increasingly anharmonic behavior of the Zn atoms. From a combination of Raman spectroscopy and first principles calculations of phonons we consolidate the presence of low-energy optic modes with wavenumbers below 60 cm -1 . Heat capacity measurements between 2 and 400 K can be well described by a Debye-Einstein model containing one Debye and two Einstein contributions with temperatures Θ D = 195K, Θ E1 = 78 K and Θ E2 = 277 K as well as a significant contribution due to anharmonicity above 150 K. The presence of a multitude of weakly dispersed low-energy optical modes (which couple with the acoustic, heat carrying phonons) combined with anharmonic thermal behavior provides an effective mechanism for low lattice thermal conductivity. The peculiar vibrational properties of ZnSb are attributed to its chemical bonding properties which are characterized by multicenter bonded structural entities. We argue that the proposed mechanism to explain the low lattice thermal conductivity of ZnSb might also control the thermoelectric properties of other electron poor semiconductors, such as Zn 4 Sb 3 , CdSb, Cd 4 Sb 3 , Cd 13-x In y Zn 10 , and Zn 5 Sb 4 In 2-δ .2

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Section: B Heat Capacity Measurementsmentioning

confidence: 68%

Section: Introductionmentioning

confidence: 90%

Thermal and vibrational properties of thermoelectric ZnSb: Exploring the origin of low thermal conductivity

et al. 2015

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“…5 below for a crystal with n atoms per unit cell and the atomic volume being a 3 [48][49][50] The parameter represents the total scattering time due to various resistive processes, Umklapp scattering (U), phonon-point-defect scattering (PD), phonon-boundary scattering (B), and etc. [32] In perfect insulators at high temperatures, U-processes [48,53,54].…”

Section: Relaxation-time Approximation (Rta) With the Debye Modelmentioning

confidence: 99%

The role of low-lying optical phonons in lattice thermal conductance of rare-earth pyrochlores: A first-principle study

2015

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Rare-earth pyrochlores, commonly exhibiting anomalously low lattice thermal conductivities, are considered as promising topcoat materials for thermal barrier coatings. However the structural origin underlying their low thermal conductivities remain unclear. In the present study, we investigated the phonon properties of two groups of RE pyrochlores, Ln2Zr2O7 (Ln = La, Nd, Sm, Gd) and Gd2T2O7 (T = Zr, Hf, Sn, Pb) employing density functional theory and quasi harmonic approximation.Through the relaxation time approximation (RTA) with Debye model, the thermal conductivities of those RE pyrochlores were predicted, showing good agreement with experimental measurements. The low thermal conductivities of RE pyrochlores were shown to largely come from the interference between the low-lying optical branches and acoustic branches. The structural origin underlying the low-lying optical branches was then clarified and the competition between scattering processes in transverse and longitude acoustic branches was discussed.

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“…7,17 Although QHA-based models overall improve accuracy of κ ' , they are far from the results obtained from calculating the anharmonic force constants and solving the associated Boltzmann transport equation (BTE). 8,18 To the best of our knowledge, solving the BTE is the optimal method for systematically and accurately calculating thermal conductivity.…”

Section: Introductionmentioning

confidence: 99%

An efficient and accurate framework for calculating lattice thermal conductivity of solids: AFLOW—AAPL Automatic Anharmonic Phonon Library

et al. 2017

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One of the most accurate approaches for calculating lattice thermal conductivity, κ ' , is solving the Boltzmann transport equation starting from third-order anharmonic force constants. In addition to the underlying approximations of ab-initio parameterization, two main challenges are associated with this path: high computational costs and lack of automation in the frameworks using this methodology, which affect the discovery rate of novel materials with ad-hoc properties. Here, the Automatic Anharmonic Phonon Library (AAPL) is presented. It efficiently computes interatomic force constants by making effective use of crystal symmetry analysis, it solves the Boltzmann transport equation to obtain κ ' , and allows a fully integrated operation with minimum user intervention, a rational addition to the current high-throughput accelerated materials development framework AFLOW. An "experiment vs. theory" study of the approach is shown, comparing accuracy and speed with respect to other available packages, and for materials characterized by strong electron localization and correlation. Combining AAPL with the pseudo-hybrid functional ACBN0 is possible to improve accuracy without increasing computational requirements.

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Modeling the thermal conductivities of the zinc antimonides ZnSb and Zn4Sb3

Cited by 122 publications

References 47 publications

Thermal and vibrational properties of thermoelectric ZnSb: Exploring the origin of low thermal conductivity

Thermal and vibrational properties of thermoelectric ZnSb: Exploring the origin of low thermal conductivity

The role of low-lying optical phonons in lattice thermal conductance of rare-earth pyrochlores: A first-principle study

An efficient and accurate framework for calculating lattice thermal conductivity of solids: AFLOW—AAPL Automatic Anharmonic Phonon Library

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