Effect of disorder on the thermal transport and elastic properties in thermoelectric<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mi>Zn</mml:mi><mml:mn>4</mml:mn></mml:msub><mml:msub><mml:mi>Sb</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>

Bhattacharya, Sriparna; Hermann, Raphaël P.; Keppens, Veerle; Tritt, Terry M.; Snyder, G. Jeffrey

doi:10.1103/physrevb.74.134108

Cited by 68 publications

(49 citation statements)

References 24 publications

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“…Assuming that these phonon interactions are the dominant scattering term for the heat transport, a simple kinetic gas theory model yields a thermal conductivity c v v s l=3 13:2 mW K ÿ1 cm ÿ1 , where c v 1:68 J K ÿ1 cm ÿ3 is the specific heat (per unit volume) at 300 K, close to the Dulong-Petit limit. This estimation agrees favorably with the recently measured lattice thermal conductivity 13 mW K ÿ1 cm ÿ1 at 300 K obtained by the steady state method [10]. These results are at variance with an earlier lower estimation [11], obtained by thermal diffusivity, involving a smaller heat capacity, smaller sound velocity and a larger carrier concentration.…”

Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tosupporting

confidence: 90%

“…The measured heat capacity is identical to that reported in Ref. [10], except for a sharper signature of the first order phase transition at 250 K in the present sample.…”

supporting

confidence: 89%

“…These results are at variance with an earlier lower estimation [11], obtained by thermal diffusivity, involving a smaller heat capacity, smaller sound velocity and a larger carrier concentration. No abrupt change is seen in the thermal conductivity [10] near 255 K at the order-disorder transition involving Zn atoms [17]. Such a change would be expected if Zn disorder were playing a dominant role in the observed local mode.…”

Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tomentioning

confidence: 81%

“…The phonon damping related to the Lorentzian width results from interactions between local dimer phonon modes and the propagating acoustic phonon modes and corresponds to their very short phonon lifetime, @=ÿ 3:9 10 ÿ13 s at 300 K. With a mean sound velocity of v s 2:47 10 5 cm s ÿ1 (Ref. [10]), this lifetime yields the mean free path of the heat carrying acoustic phonons, l 0:96 nm, and is similar to unit cell dimensions. Assuming that these phonon interactions are the dominant scattering term for the heat transport, a simple kinetic gas theory model yields a thermal conductivity c v v s l=3 13:2 mW K ÿ1 cm ÿ1 , where c v 1:68 J K ÿ1 cm ÿ3 is the specific heat (per unit volume) at 300 K, close to the Dulong-Petit limit.…”

Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tomentioning

confidence: 99%

“…Among thermoelectric materials, zinc antimony, known in literature as Zn 4 Sb 3 , exhibits an outstanding figure of merit between 450 K and 670 K with ZT 1:3 at 670 K, owing to its particularly low thermal conductivity [10,11]. Sufficient electronic conductivity follows from a low electronic carrier concentration accompanied by high carrier mobility in this rather covalent material [12].…”

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confidence: 99%

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Dumbbell Rattling in Thermoelectric Zinc Antimony

et al. 2007

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Inelastic neutron scattering measurements on thermoelectric Zn 4 Sb 3 reveal a dominant soft local phonon mode at 5.3(1) meV. The form factor of this local mode is characteristic for dumbbells vibrating preferably along the dumbbell axis and can be related to a vibration of Sb dimers along the c axis. The Lorentzian width of the mode corresponds to short phonon lifetimes of 0.39(2) ps and yields an estimate of the thermal conductivity that agrees quantitatively with recent steady state measurements. Heat capacity measurements are consistent with an Einstein mode model describing the local Sb-dimer rattling mode with an Einstein temperature of 62(1) K. Our study suggests that soft localized phonon modes in crystalline solids are not restricted to cagelike structures and are likely to be a universal feature of good thermoelectric materials.

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Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tosupporting

confidence: 90%

“…The measured heat capacity is identical to that reported in Ref. [10], except for a sharper signature of the first order phase transition at 250 K in the present sample.…”

supporting

confidence: 89%

Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tomentioning

confidence: 81%

Section: -2 Axis Model (Ii) or (Iii) Possible Correlations Tomentioning

confidence: 99%

mentioning

confidence: 99%

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Dumbbell Rattling in Thermoelectric Zinc Antimony

et al. 2007

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Phase Transformation Contributions to Heat Capacity and Impact on Thermal Diffusivity, Thermal Conductivity, and Thermoelectric Performance

2019

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Although direct measurements of κ are possible, [2] it is more frequent in measurement above room temperature to calculate thermal conductivity through the relation (Note S1, Supporting Information)Here, D [m 2 s −1 ] is the thermal diffusivity and ρc p = (∂H/∂T) p is the constant pressure heat capacity [J m −3 K −1 ] typically calculated from experimental bulk density, ρ [kg m −3 ] and the mass specific heat c p [J kg −1 K −1 ]. Equation (1) is utilized largely because measurements of thermal diffusivity, D, are accurate (within ≈3%) and easily accessible. [2] Thus, the uncertainty in calculating κ (often 10% or more) is frequently attributed to measurement of heat capacity. [2,3] Due to the uncertainty in the absolute magnitude of high temperature heat capacity measurements, it is often more accurate to use a model. Usually, the temperature independent Dulong-Petit heat capacity is a good approximation (within ≈5%) near room temperature. At higher temperatures, a model that incorporates a linear temperature dependence may be appropriate. [2,4,5] However, an incomplete understanding of heat capacity measurements and models can lead to inaccurate estimations of κ in some systems, especially those having substantial latent heats (e.g., during phase transitions). The recent debate surrounding the thermoelectric material, Cu 2 Se, is an excellent example. [6][7][8][9][10][11] In this material, and others, [12][13][14] the thermal diffusivity drops markedly as the material undergoes a phase transition. Depending on the heat capacity used to calculate κ, a maximum zT between 0.6 [7] and 2.3 [6] has been reported due to the superionic phase transition in Cu 2 Se. As exemplified in Figure 1, the choice of heat capacity can have a drastic impact on zT values.To properly characterize the behavior of thermal conductivity through a phase transition, it is paramount to understand the concurrent behavior of heat capacity. Recognizing that the total capacity of a material to absorb heat includes both the intrinsic heat capacity of the phases present and the enthalpy (heat) of transformation ΔH that is required to maintain equilibrium (characterized by the order parameter φ) as the temperature is changedThe accurate characterization of thermal conductivity κ, particularly at high temperature, is of paramount importance to many materials, thermoelectrics in particular. The ease and access of thermal diffusivity D measurements allows for the calculation of κ when the volumetric heat capacity, ρc p , of the material is known. However, in the relation κ = ρc p D, there is some confusion as to what value of c p should be used in materials undergoing phase transformations. Herein, it is demonstrated that the Dulong-Petit estimate of c p at high temperature is not appropriate for materials having phase transformations with kinetic timescales relevant to thermal transport. In these materials, there is an additional capacity to store heat in the material through the enthalpy of transformation ΔH. This can be described using a generalize...

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Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

et al. 2023

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The elastic behavior of a material can be a powerful tool to decipher thermal transport. In thermoelectrics, measuring the elastic moduli-directly tied to sound velocity-is critical to understand trends in lattice thermal conductivity, as well as study bond anharmonicity and phase transitions, given the sensitivity of elastic moduli to the chemical bonding. In this review, we introduce the basics of elasticity and explain the origin of high-temperature lattice softening from a bonding perspective. We then review elasticity data throughout classes of thermoelectrics, and explore trends in sound velocity, anharmonicity, and thermal conductivity. We reveal how experimental sound velocities can improve the accuracy of common thermal conductivity models and present a critical discussion of Grüneisen parameter estimates from elastic moduli. Readers will be equipped with tools to leverage elasticity measurements or calculations to accurately interpret thermal transport trends.

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Effect of disorder on the thermal transport and elastic properties in thermoelectricZn4Sb3

Cited by 68 publications

References 24 publications

Dumbbell Rattling in Thermoelectric Zinc Antimony

Dumbbell Rattling in Thermoelectric Zinc Antimony

Phase Transformation Contributions to Heat Capacity and Impact on Thermal Diffusivity, Thermal Conductivity, and Thermoelectric Performance

Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

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