The paper discusses the fundamental behavior of the dynamical lattice thermal conductivity k(W) of bulk cubic semiconductor crystals. The calculation approach is based on solving Boltzmann-Peierls Phonon Transport Equation in the frequency domain after excitation by a dynamical temperature gradient, within the framework of the single relaxation time approximation and using modified Debye-Callaway model. Our model allows us to obtain a compact expression for k(W) that captures the leading behavior of the dynamical thermal conduction by phonons. This expression fulfills the causality requirement and leads to a convolution type relationship between the heat flux density current and the temperature gradient in the real space-time domain in agreement with Gurtin-Pipkin theory. The dynamical behavior of k(W) is studied by changing ambient temperature as well as different intrinsic and extrinsic parameters including the effect of embedding semiconductor nanoparticles as extrinsic phonon scattering centers. The paper investigates also the applicability of Shastry Sum Rule and the possibility of existence and propagation of second sound in the frame work of Boltzmann theory.
Charge transport of topological semimetals has been in the focus of intensive investigations because of their non-trivial band topology. Heat transport of these materials, on the other hand, is largely unexplored and remains elusive. Here we report on an observation of unprecedented, giant magnetic quantum oscillations of thermal conductivity in the prototypical Weyl semimetal TaAs. The oscillations are antiphase with the quantum oscillating electronic density of states of a Weyl pocket, and their amplitudes amount to two orders of magnitude of the estimation based on the Wiedemann-Franz law. …
We report the calculation results of specific heat ($c_v$), and thermal conductivity ($κ$) by using Einstein, and Debye models about rock salt (NaCl), oxides: Na$_x$CoO$_2$, SrTiO$_3$, and LiNbO$_3$. In calculation, the longitudinal (L), and transverse (T) sound velocities ($v_T$, $v_L$) were estimated from acoustic phonons' dispersion's (~$ω$/$K$) in above materials, and the average sound velocities ($v_a$) were input into Debye model for $κ$ equation, and results were compared with that of Einstein model. In some oxides, $v_a$ is relatively reduced at slight high $v_T$ ($v_T$/$v_L$=0.3-0.5).…
Accelerated Discovery of Crystalline Materials with Record Ultralow Lattice Thermal Conductivity via a Universal Descriptor
Northwestern Polytechnical University（西北工业大学）；CRISMAT, CNRS, Normandie Univ, ENSICAEN, UNICAEN（诺曼底大学，卡昂国立高等工程学院，法国国家科学研究中心材料研究化学实验室）；Thayer School of Engineering, Dartmouth College（达特茅斯学院塔克工程学院）；Institute Laue Langevin（朗之万研究所）；FZU - Institute of Physics of the Czech Academy of Sciences（捷克科学院物理研究所）；ShanghaiTech Laboratory for Topological Physics & School of Physical Science and Technology, ShanghaiTech University（上海科技大学物理科学与技术学院拓扑物理实验室）；Université de Lorraine, CNRS, IJL（洛林大学，法国国家科学研究中心，界面与层析实验室）
A solid with larger sound speeds exhibits higher lattice thermal conductivity (k_{lat}). Diamond is a prominent instance where its mean sound speed is 14400 m s-1 and k_{lat} is 2300 W m-1 K-1. Here, we report an extreme exception that CuP2 has quite large mean sound speeds of 4155 m s-1, comparable to GaAs, but the single crystals show a very low lattice thermal conductivity of about 4 W m-1 K-1 at room temperature, one order of magnitude smaller than GaAs. To understand such a puzzling thermal transport behavior, we have thoroughly investigated the atomic structure and lattice dynamics by co…
We present a framework for quantifying the uncertainty that results from the choice of exchange-correlation (XC) functional in predictions of phonon properties and thermal conductivity that use density functional theory (DFT) to calculate the atomic force constants. The energy ensemble capabilities of the BEEF-vdW XC functional are first applied to determine an ensemble of interatomic force constants, which are then used as inputs to lattice dynamics calculations and a solution of the Boltzmann transport equation. The framework is applied to isotopically-pure silicon. We find that the uncertai…
In the design of materials with low lattice thermal conductivity, compounds with high density, low speed of sound, and complexity at either the atomic, nano- or microstructural level are preferred. The layered compound Mg$_3$Sb$_2$ defies these prevailing paradigms, exhibiting lattice thermal conductivity comparable to PbTe and Bi$_2$Te$_3$, despite its low density and simple structure. The excellent thermoelectric performance ($zT$ $\sim$ 1.5) in $n$-type Mg$_3$Sb$_2$ has thus far been attributed to its multi-valley conduction band, while its anomalous thermal properties have been largely ove…
The temperature dependence of the thermal conductivity of amorphous solids is markedly different from that of their crystalline counterparts, but exhibits universal behaviour. Sound attenuation is believed to be related to this universal behaviour. Recent computer simulations demonstrated that in the harmonic approximation sound attenuation $Γ$ obeys quartic, Rayleigh scattering scaling for small wavevectors $k$ and quadratic scaling for wavevectors above the Ioffe-Regel limit. However, simulations and experiments do not provide a clear picture of what to expect at finite temperatures where an…
Thermal conductivity of amorphous carbon thin films
用$3ω$方法测量了非晶碳薄膜在80- 400 K温度范围内的热导率$Λ$。样品薄膜的范围从通过远程等离子体沉积制备的软a-C：H（室温下的$Λ= 0.20$ W m $^{-1}$ K $^{-1}$）到具有大部分从过滤弧源沉积的$sp^3$键合碳的非晶金刚石（$Λ= 2.2$ W m $^{-1}$ K $^{-1}$）。连续介质理论提供了电导率随质量密度变化的唯象描述。热导率与由测量的原子密度和纵向声速计算的最小热导率吻合得很好。
An ultralow lattice thermal conductivity of 0.14 W$\cdot$ m$^{-1} \cdot$ K$^{-1}$ along the $\vec b$ axis of As$_2$Se$_3$ single crystals was obtained at 300 K by first-principles calculations involving the density functional theory and the resolution of the Boltzmann transport equation. This ultralow lattice thermal conductivity arises from the combination of two mechanisms: 1) a cascade-like fall of the low-lying optical modes, which results in avoided crossings of these with the acoustic modes, low sound velocities and increased scattering rates of the acoustic phonons; and 2) the repulsion…
Different types of graphene-related materials (GRM) are industrially available and have been exploited for thermal conductivity enhancement in polymers. These include materials with very different features, in terms of thickness, lateral size and composition, especially concerning the oxygen to carbon ratio and the possible presence of surface functionalization. Due to the variability of GRM properties, the differences in polymer nanocomposites preparation methods and the microstructures obtained, a large scatter of thermal conductivity performance is found in literature. However, detailed cor…
The transparent semiconductor In$_{2}$O$_{3}$ is a technologically important material. It combines optical transparency in the visible frequency range and sizeable electric conductivity. We present a study of thermal conductivity of In$_{2}$O$_{3}$ crystals and find that around 20 K, it peaks to a value as high as 5,000 WK$^{-1}$m$^{-1}$, comparable to the peak thermal conductivity in silicon and exceeded only by a handful of insulators. The amplitude of the peak drastically decreases in presence of a type of disorder, which does not simply correlate with the density of mobile electrons. Annea…
A fundamental understanding of the phonon transport mechanism is important for optimizing the efficiency of thermoelectric devices. In this study, we investigate the thermal transport properties of the oxidized form of phosphorene called phosphorene oxide (PO) by solving phonon Boltzmann transport equation based on first-principles density functional theory. We reveal that PO exhibits a much lower thermal conductivity (2.42-7.08 W/mK, at 300 K) than its pristine counterpart as well as other two-dimensional materials. To comprehend the physical origin of such low thermal conductivity, we scruti…
A simple vibrational model of heat transfer in two-dimensional (2D) fluids relates the heat conductivity coefficient to the longitudinal and transverse sound velocities, specific heat, and the mean interatomic separation. This model is demonstrated not to contradict the available experimental and numerical data on heat transfer in 2D complex plasma layers. Additionally, the heat conductivity coefficient of a 2D one-component plasma with a logarithmic interaction is evaluated.
Systematic experimental and theoretical research on the role of microstructure and interface thermal resistance on the thermal conductivity of the PbTe-CoSb3 bulk polycrystalline composite is presented. In particular, the correlation between the particle size of the dispersed phase and interface thermal resistance (R_{int}) on the phonon thermal conductivity (κ_{ph}) is discussed. With this aim, a series of PbTe-CoSb_3 polycrystalline composite materials with the different particle sizes of CoSb_3 was prepared. The structural (XRD) and microstructural analysis (SEM/EDXS) confirmed assumed chem…
Silicon carbide has excellent physical properties, such as high stability, thermal conductivity, and mechanical strength. It has been widely used in high-power devices, catalysis, material processing, and other fields and is of great significance in basic discipline research. We used crystal structure search and first principles calculation to predict four new silicon carbide structures stabilized within 3TPa. Pnma (SiC) replaces B1 (SiC) above 2.6TPa, and the new component Si3C2 becomes the most stable after 2.5TPa. P4/mbm phase Si3C2 under high pressure has electrode characteristics. The sil…
Intrinsically ultralow thermal conductivity in all-inorganic superatomic bulk crystals
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所北京凝聚态物理国家实验室）；School of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电技术学院）；Department of Energy and Resources Engineering, Peking University（北京大学能源与资源工程系）；Center for High Pressure Science and Technology Advanced Research（高压科学和技术先进研究中心）；Key Laboratory of Quantum Materials under Extreme Conditions in Shandong Province, School of Physics and Physical Engineering, Qufu Normal University（曲阜师范大学物理与物理工程学院山东省极端条件量子材料重点实验室）
研究通过生长Re6Se8Te7和Re6Te15超原子单晶，发现其在室温下热导率分别为0.32和0.53 W m-1 K-1，归因于高Grüneisen参数和低声速，验证了无序声子传输的存在。
Balanced electron and phonon heat transport in metallic $\varepsilon$-TaN
Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin（德克萨斯大学奥斯汀分校奥登计算工程与科学学院）；Department of Physics, The University of Texas at Austin（德克萨斯大学奥斯汀分校物理系）；Texas Materials Institute, The University of Texas at Austin（德克萨斯大学奥斯汀分校德州材料研究所）；Walker Department of Mechanical Engineering, The University of Texas at Austin（德克萨斯大学奥斯汀分校沃克机械工程系）
We present an ab-initio study of the temperature dependent elastic constants of BAs, a semiconductor that exhibits ultra-high thermal conductivity and is under investigation for thermal management in electronics. We test the consistency of our predictions by computing the temperature dependent sound velocity of the longitudinal acoustic mode along the $[111]$ direction and comparing with experiment. Furthermore, as a byproduct, we present the room temperature phonon dispersions, and the temperature dependent thermal expansion, isobaric heat capacity, and average Grüneisen parameter comparing w…
Applications of commodity polymers are often hindered by their low thermal conductivity. In these systems, going from the standard polymers dictated by weak van der Waals interactions to biocompatible hydrogen bonded smart polymers, the thermal transport coefficient k varies between 0.1 - 0.4 W/Km. Combining all-atom molecular dynamics simulations with some experiments, we study thermal transport and its link to the elastic response of commodity plastics. We find that there exists a maximum attainable stiffness (or sound wave velocity), thus providing an upper bound of k for these solid polyme…
We present a study of thermal conductivity, $κ$, in undoped and doped strontium titanate in a wide temperature range (2-400 K) and detecting different regimes of heat flow. In undoped SrTiO$_{3}$, $κ$ evolves faster than cubic with temperature below its peak and in a narrow temperature window. Such a behavior, previously observed in a handful of solids, has been attributed to a Poiseuille flow of phonons, expected to arise when momentum-conserving scattering events outweigh momentum-degrading ones. The effect disappears in presence of dopants. In SrTi$_{1-x}$Nb$_{x}$O$_{3}$, a significant redu…
The orthorhombic monochalcogenide SnSe has attracted much attention in recent years as a promising high-temperature thermoelectric material. We present a study of its thermal conductivity and specific heat of SnSe between 2~K and 300~K and quantify its anisotropic thermal diffusivity, $D$. For both crystallographic orientations, thermal diffusivity remains above the recently identified Planckian limit ($D > v_s^2 τ_P$, where $v_s$ is the sound velocity and $τ_P= \hbar/k_BT$) and its anisotropy in $D$ is set by the anisotropy of $v_s$. Comparison with cubic members of the IV-VI family leads to …
Heat conduction in dielectric crystals originates from the propagation of atomic vibrations, whose microscopic dynamics is well described by the linearized phonon Boltzmann transport equation. Recently, it was shown that thermal conductivity can be resolved exactly and in a closed form as a sum over relaxons, $\mathit{i.e.}$ collective phonon excitations that are the eigenvectors of Boltzmann equation's scattering matrix [Cepellotti and Marzari, PRX $\mathbf{6}$ (2016)]. Relaxons have a well-defined parity, and only odd relaxons contribute to the thermal conductivity. Here, we show that the co…
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…
We present a detailed density functional theory based calculations of the structural, elastic, lattice dynamical, thermophysical, and optoelectronic properties of ternary semiconductors CaZn$_2$X$_2$ (X = N, P, As) in this paper. The obtained lattice parameters are in excellent agreement with the experimental values and other theoretical findings. These elastic constants satisfy the mechanical stability criteria. Moreover, many thermophysical parameters of these compounds are estimated, including the Debye temperature, average sound velocity, melting temperature, heat capacity, lattice thermal…
