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1. Spectral heat flux redistribution upon interfacial transmission

   https://doi.org/10.1088/1361-648X/ada660  

   Cui, Haoran; Maranets, Theodore; Ma, Tengfei; Wang, Yan (January 2025, Journal of Physics: Condensed Matter)

   Abstract In nonmetallic crystals, heat is transported by phonons of different frequencies, each contributing differently to the overall heat flux spectrum. In this study, we demonstrate a significant redistribution of heat flux among phonon frequencies when phonons transmit across the interface between dissimilar solids. This redistribution arises from the natural tendency of phononic heat to re-establish the bulk distribution characteristic of the material through which it propagates. Remarkably, while the heat flux spectra of dissimilar solids are typically distinct in their bulk forms, they can become nearly identical in superlattices or sandwich structures where the layer thicknesses are smaller than the phonon mean free paths. This phenomenon reflects that the redistribution of heat among phonon frequencies to the bulk distribution does not occur instantaneously at the interface, rather it develops over a distance on the order of phonon mean-free-paths. 

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2. Machine Learning a Universal Harmonic Interatomic Potential for Predicting Phonons in Crystalline Solids

   Lee, Huiju; Xia, Yi (March 2024, Applied physics letters)

   Grein, Christoph (Ed.)

   Phonons, as quantized vibrational modes in crystalline materials, play a crucial role in determining a wide range of physical properties, such as thermal and electrical conductivity, making their study a cornerstone in materials science. In this study, we present a simple yet effective strategy for deep learning harmonic phonons in crystalline solids by leveraging existing phonon databases and state-of-the-art machine learning techniques. The key of our method lies in transforming existing phonon datasets, primarily represented in interatomic force constants, into a force-displacement representation suitable for training machine learning universal interatomic potentials. By applying our approach to one of the largest phonon databases publicly available, we demonstrate that the resultant machine learning universal harmonic interatomic potential not only accurately predicts full harmonic phonon spectra but also calculates key thermodynamic properties with remarkable precision. Furthermore, the restriction to a harmonic potential energy surface in our model provides a way of assessing uncertainty in machine learning predictions of vibrational properties, essential for guiding further improvements and applications in materials science. 

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3. Hierarchy of Exchange-Correlation Functionals in Computing Lattice Thermal Conductivities of Rocksalt and Zincblende Semiconductors

   Wei, Jiacheng; Xia, Zhonghao; Xia, Yi; He, Jiangang (July 2024, Physical review B)

   Lattice thermal conductivity (κL) is a crucial characteristic of crystalline solids with significant implications for thermal management, energy conversion, and thermal barrier coating. The advancement of computational tools based on density functional theory (DFT) has enabled the effective utilization of phonon quasi-particle-based approaches to unravel the underlying physics of various crystalline systems. While the higher order of anharmonicity is commonly used for explaining extraordinary heat transfer behaviors in crystals, the impact of exchange-correlation (XC) functionals in DFT on describing anharmonicity has been largely overlooked. The XC functional is essential for determining the accuracy of DFT in describing interactions among electrons/ions in solids and molecules. However, most XC functionals in solid-state physics are primarily focused on computing the properties that only require small atomic displacements from the equilibrium (within the harmonic approximation), such as harmonic phonons and elastic constants, while anharmonicity involves larger atomic displacements. Therefore, it is more challenging for XC functionals to accurately describe atomic interactions at the anharmonicity level. In this study, we systematically investigate the room-temperature κL of 16 binary compounds with rocksalt and zincblende structures using var- ious XC functionals such as local density approximation (LDA), Perdew-Burke-Ernzerhof (PBE), revised PBE for solid and surface (PBEsol), optimized B86b functional (optB86b), revised Tao-Perdew-Staroverov-Scuseria (revTPSS), strongly constrained and appropriately normed functional (SCAN), regularized SCAN (rSCAN) and regularized-restored SCAN (r2SCAN) in combination with different perturbation orders, including phonon within harmonic approximation (HA) plus three- phonon scattering (HA+3ph), phonon calculated using self-consistent phonon theory (SCPH) plus three-phonon scattering (SCPH+3ph), and SCPH phonon plus three- and four-phonon scattering (SCPH+3,4ph). Our results show that the XC functional exhibits strong entanglement with perturbation order and the mean relative absolute error (MRAE) of the computed κL is strongly influenced by both the XC functional and perturbation order, leading to error cancellation or amplification. The minimal (maximal) MRAE is achieved with revTPSS (rSCAN) at the HA+3ph level, SCAN (r2SCAN) at the SCPH+3ph level, and PBEsol (rSCAN) at the SCPH+3,4ph level. Among these functionals, PBEsol exhibits the highest accuracy at the highest perturbation order. The SCAN- related functionals demonstrate moderate accuracy but are suffer from numerical instability and high computational costs. Furthermore, the different impacts of quartic anharmonicity on κL in rocksalt and zincblende structures are identified by all XC functionals, attributed to the distinct lattice anharmonicity in these two structures. These findings serve as a valuable reference for selecting appropriate functionals for describing anharmonic phonons and offer insights into high-order force constant calculations that could facilitate the development of more accurate XC functionals for solid materials. 

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4. Hierarchical Coherent Phonons in a Superatomic Semiconductor

   https://doi.org/10.1002/adma.201903209  

   Lee, Kihong; Maehrlein, Sebastian_F; Zhong, Xinjue; Meggiolaro, Daniele; Russell, Jake_C; Reed, Douglas_A; Choi, Bonnie; De_Angelis, Filippo; Roy, Xavier; Zhu, Xiaoyang (July 2019, Advanced Materials)

   Abstract The coupling of phonons to electrons and other phonons plays a defining role in material properties, such as charge and energy transport, light emission, and superconductivity. In atomic solids, phonons are delocalized over the 3D lattice, in contrast to molecular solids where localized vibrations dominate. Here, a hierarchical semiconductor that expands the phonon space by combining localized 0D modes with delocalized 2D and 3D modes is described. This material consists of superatomic building blocks (Re₆Se₈) covalently linked into 2D sheets that are stacked into a layered van der Waals lattice. Using transient reflectance spectroscopy, three types of coherent phonons are identified: localized 0D breathing modes of isolated superatom, 2D synchronized twisting of superatoms in layers, and 3D acoustic interlayer deformation. These phonons are coupled to the electronic degrees of freedom to varying extents. The presence of local phonon modes in an extended crystal opens the door to controlling material properties from hierarchical phonon engineering. 

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5. High frequency atomic tunneling yields ultralow and glass-like thermal conductivity in chalcogenide single crystals

   https://doi.org/10.1038/s41467-020-19872-w  

   Sun, Bo; Niu, Shanyuan; Hermann, Raphael P.; Moon, Jaeyun; Shulumba, Nina; Page, Katharine; Zhao, Boyang; Thind, Arashdeep S.; Mahalingam, Krishnamurthy; Milam-Guerrero, JoAnna; et al (December 2020, Nature Communications)

   null (Ed.)

   Abstract Crystalline solids exhibiting glass-like thermal conductivity have attracted substantial attention both for fundamental interest and applications such as thermoelectrics. In most crystals, the competition of phonon scattering by anharmonic interactions and crystalline imperfections leads to a non-monotonic trend of thermal conductivity with temperature. Defect-free crystals that exhibit the glassy trend of low thermal conductivity with a monotonic increase with temperature are desirable because they are intrinsically thermally insulating while retaining useful properties of perfect crystals. However, this behavior is rare, and its microscopic origin remains unclear. Here, we report the observation of ultralow and glass-like thermal conductivity in a hexagonal perovskite chalcogenide single crystal, BaTiS 3 , despite its highly symmetric and simple primitive cell. Elastic and inelastic scattering measurements reveal the quantum mechanical origin of this unusual trend. A two-level atomic tunneling system exists in a shallow double-well potential of the Ti atom and is of sufficiently high frequency to scatter heat-carrying phonons up to room temperature. While atomic tunneling has been invoked to explain the low-temperature thermal conductivity of solids for decades, our study establishes the presence of sub-THz frequency tunneling systems even in high-quality, electrically insulating single crystals, leading to anomalous transport properties well above cryogenic temperatures. 

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