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Lattice thermal conductivity (kL) is a crucial physical property of crystals with applications in thermal management, such as heat dissipation, insulation, and thermoelectric energy conversion. However, accurately and rapidly determining kL poses a considerable challenge. In this study, we introduce an formula that achieves high precision (mean relative error=8.97%) and provides fast predictions, taking less than one minute, for kL across a wide range of inorganic binary and ternary materials. Our interpretable, dimensionally aligned and physical grounded formula forecasts kL values for 4,601 binary and 6,995 ternary materials in the Materials Project database. Notably, we predict undiscovered high kL values for AlBN2 (kL=101 W/ m/ K) and the undetectedlow kL Cs2Se (kL=0.98 W/ m/ K) at room temperature. This method for determining kL streamlines the traditionally time-consuming process associated with complex phonon physics. It provides insights into microscopic heat transport and facilitates the design and screening of materials with targeted and extreme kL values through the application of phonon engineering. Our findings offer opportunities for controlling and optimizing macroscopic transport properties of materials by engineering their bulk modulus, shear modulus, and Gruneisen parameter.

High thermoelectric properties are associated with the phonon-glass electron-crystal paradigm. Conventional wisdom suggests that the optimal bandgap of semiconductor to achieve the largest power factor should be between 6 and 10 kbT. To address challenges related to the bipolar effect and temperature limitations, we present findings on Zintl-type TlAgI2, which demonstrates an exceptionally low lattice thermal conductivity of 0.3 W m-1 K-1 at 300 K. The achieved figure of merit (ZT) for TlAgI2, featuring a 1.55 eV bandgap, reaches a value of 2.20 for p-type semiconductor. This remarkable ZT is attributed to the existence of extended antibonding states Ag-I in the valence band. Furthermore, the bonding hierarchy, influencing phonon anharmonicity, and coordination bonds, facilitating electron transfer between the ligand and the central metal ion, significantly contribute to electronic transport. This finding serves as a promising avenue for the development of high ZT materials with wide bandgaps at elevated temperatures.

Efficient and precise calculations of thermal transport properties and figure of merit, alongside a deep comprehension of thermal transport mechanisms, are essential for the practical utilization of advanced thermoelectric materials. In this study, we explore the microscopic processes governing thermal transport in the distinguished crystalline material Tl$_9$SbTe$_6$ by integrating a unified thermal transport theory with machine learning-assisted self-consistent phonon calculations. Leveraging machine learning potentials, we expedite the analysis of phonon energy shifts, higher-order scattering mechanisms, and thermal conductivity arising from various contributing factors like population and coherence channels. Our finding unveils an exceptionally low thermal conductivity of 0.31 W m$^{-1}$ K$^{-1}$ at room temperature, a result that closely correlates with experimental observations. Notably, we observe that the off-diagonal terms of heat flux operators play a significant role in shaping the overall lattice thermal conductivity of Tl$_9$SbTe$_6$, where the ultralow thermal conductivity resembles that of glass due to limited group velocities. Furthermore, we achieve a maximum $ZT$ value of 3.17 in the $c$-axis orientation for \textit{p}-type Tl$_9$SbTe$_6$ at 600 K, and an optimal $ZT$ value of 2.26 in the $a$-axis and $b$-axis direction for \textit{n}-type Tl$_9$SbTe$_6$ at 500 K. The crystalline Tl$_9$SbTe$_6$ not only showcases remarkable thermal insulation but also demonstrates impressive electrical properties owing to the dual-degeneracy phenomenon within its valence band. These results not only elucidate the underlying reasons for the exceptional thermoelectric performance of Tl$_9$SbTe$_6$ but also suggest potential avenues for further experimental exploration.

We study the phase transition behavior of the ferroelectric BaTi$_{0.8}$Zr$_{0.2}$O$_3$ in the paraelectric region. The temperature dependencies of thermal, polar, elastic and dielectric properties indicate the presence of local structures above the paraelectric-ferroelectric transition temperature Tc = 292 K. The non-zero remnant polarization is measured up to a characteristic temperature T* ~350 K, which coincides with the temperature where the dielectric constant deviates from Curie-Weiss law. Resonant Piezoelectric Spectroscopy shows that DC field-cooling above Tc using fields smaller than the coercive field leads to an elastic response and remnant piezoelectricity below T*, which likely corresponds to the coherence temperature associated with polar nanostructures in ferroelectrics. The observed remnant effect is attributed to the reorientation of polar nanostructures above Tc., Comment: Accepted version in Applied Physics Letters. 13 pages; 4 figures. (Supp Material in version 1)

Noble gas atoms such as Kr and Xe are byproducts of nuclear fission in nuclear plants. How to trap and confine these volatile even radioactive gases is particularly challenging. Recent studies have shown that they can be trapped in nanocages of ultrathin silica. Here, we exhibit with self-consistent phonon theory and four-phonon (4ph) scattering where the adsorption of noble gases results in an anomalous increase in lattice thermal conductivity, while the presence of Cu atoms doping leads to a reduction in lattice thermal conductivity. We trace this behavior in host-guest 2D silica to an interplay of tensile strain, rattling phonon modes, and redistribution of electrons. We also find that 4ph scatterings play indispensable roles in the lattice thermal conductivity of 2D silica. Our work illustrates the microscopic heat transfer mechanism in 2D silica nanocages with the immobilization of noble gas atoms and inspires further exploring materials with the kagome and glasslike lattice thermal conductivity., Comment: 7 pages, 4 figures

Sb and Bi monolayers, as single-elemental ferroelectric materials with similar atomic structure, hold intrinsic piezoelectricity theoretically, which makes them highly promising for applications in functional nano-devices such as sensors and actuators. Here, using first-principles calculations, we systematically explore the piezoelectric response of Sb and Bi monolayers. Our findings reveal that Sb exhibits a negative piezoelectric response, whereas Bi displays a positive one. This discrepancy is attributed to the dominant role of different atomic internal distortions (internal-strain terms) in response to applied strain. Further electron-density distribution analysis reveals that the atomic bonding in Sb tends to be covalent, while the atomic bonding in Bi leans more towards ionic. Compared to the Sb monolayer, the Bi monolayer is distinguished by its more pronounced lone-pair orbitals electrons and associated larger Born effective charges. The Coulomb repulsions between lone-pair orbitals electrons and the chemical bonds lead to the Bi monolayer possessing more prominent atomic folds and, consequently, more significant atomic distortion in the z-direction under strain. These differences result in a considerable difference in internal-strain terms, ultimately leading to the reversed piezoelectric response between Sb and Bi monolayers. The present work provides valuable insights into the piezoelectric mechanism of 2D ferroelectric materials and their potential applications in nano-electronic devices.

We investigate the influence of three- and four-phonon scattering, perturbative anharmonic phonon renormalization, and off-diagonal terms of coherent phonons on the thermal conductivity of CsPbBr3 phase change perovskite, by using advanced implementations and first-principles simulations. Our study spans a wide temperature range covering the entire structural spectrum. Notably, we demonstrate that the interactions between acoustic and optical phonons result in contrasting trends of phonon frequency shifts for the high-lying optical phonons in orthorhombic and cubic CsPbBr3 as temperature varies. Our findings highlight the significance of wave-like tunneling of coherent phonons in ultralow and glass-like thermal conductivity in halide perovskites., Comment: 9 pages, 4 figures

One of the current challenges in nanoscience is tailoring phononic devices, such as thermal regulators and thermal computing. This has long been a rather elusive task because the thermal-switching ratio is not as high as electronic analogs. Mapping from a topological kirigami assembly, nitrogen-doped porous graphene metamaterials on the nanoscale are inversely designed with a thermal-switching ratio of 27.79, which is more than double the value of previous work. We trace this behavior to the chiral folding-unfolding deformation, resulting in a metal-insulator transition. This study provides a nanomaterial design paradigm to bridge the gap between kinematics and functional metamaterials that motivates the development of high-performance thermal regulators.

Compound phases often display properties that are symmetry-forbidden relative to their nominal, average crystallographic symmetry, even if extrinsic reasons (defects, strain, imperfections) are not apparent. Here, we investigate macroscopic inversion symmetry breaking in nominally centrosymmetric materials and measure Resonant Piezoelectric Spectroscopy (RPS) and Resonant Ultrasound Spectroscopy (RUS) in 15 compounds, 18 samples, and 21 different phases, including unpoled ferroelectrics, paraelectrics, relaxors, ferroelastics, incipient ferroelectrics, and isotropic materials with low defect concentrations, i.e. NaCl,cfused silica, and CaF2. We exclude the flexoelectric effect as a source of the observed piezoelectricity yetcobserve piezoelectricity in all nominally cubic phases of these samples. By scaling the RPS intensities with those of RUS, we calibrate the effective piezoelectric coefficients using single crystal quartz as standard. Using this scaling we determine the effective piezoelectric modulus in nominally non-piezoelectric phases, finding that the "symmetry-forbidden" piezoelectric effect ranges from 1 pm/V to 10E-5 pm/V. The values for unpoled ferroelectric phases are only slightly higher than those in the paraelectric phase of the same material. The lowest coefficients are well below the detection limit of conventional piezoelectric measurements and demonstrate RPS as an ultra-highly sensitive method to measure piezoelectricity. We suggestt hat symmetry-breaking piezoelectricity in nominally centrosymmetric materials and disordered, unpoled ferroelectrics is ubiquitous.

Two-dimensional materials with ferroelectric properties break the size effect of conventional ferroelectric materials and unlock unprecedented potentials of ferroelectric-related application at small length scales. In this work, using density functional theory (DFT) calculations, we discover a tribo-ferroelectricity behavior in a group of bilayer group-IV monochalcogenides (MX, with M = Ge, Sn and X = S, Se). Upon interlayer sliding over an in-plane unit cell length, the top layer exhibits a reversible intralayer ferroelectric switching, leading to a reversible transition between the ferroelectric (electric polarization of 40$\mu$C/cm$^2$) and antiferroelectric states in the bilayer MXs. Our results show that the interlayer van der Waals interaction, which is usually considered to be weak, can actually generate an in-plane lattice distortion and thus cause the breaking/forming of intralayer covalent bonds in the top layer, leading to the observed tribo-ferroelectricity phenomenon. This unique property has several advantages for energy harvesting over existing piezoelectric and triboelectric nanogenerators. The interlayer sliding-induced polarization change is as high as 40$\mu$C/cm$^2$, which can generate an open-circuit voltage two orders of magnitude higher than that of MoS$_2$-based nanogenerators. The polarization change occurs over a time period for interlayer sliding over a unit-cell length, leading to an ultrahigh polarization changing rate and thus an ultrahigh short-circuit current. The theoretical prediction of power output for the tribo-ferroelectric bilayer MXs at a moderate sliding speed 1 m/s is four orders of magnitude higher than the MoS$_2$ nanogenerator, indicating great potentials in energy harvesting applications., Comment: Manuscript: 19 pages including 4 figures

The relationship between material properties and independent variables such as temperature, external field or time, is usually represented by a curve or surface in a multi-dimensional space. Determining such a curve or surface requires a series of experiments or calculations which are often time and cost consuming. A general strategy uses an appropriate utility function to sample the space to recommend the next optimal experiment or calculation within an active learning loop. However, knowing what the optimal sampling strategy to use to minimize the number of experiments is an outstanding problem. We compare a number of strategies based on directed exploration on several materials problems of varying complexity using a Kriging based model. These include one dimensional curves such as the fatigue life curve for 304L stainless steel and the Liquidus line of the Fe-C phase diagram, surfaces such as the Hartmann 3 function in 3D space and the fitted intermolecular potential for Ar-SH, and a four dimensional data set of experimental measurements for BaTiO3 based ceramics. We also consider the effects of experimental noise on the Hartmann 3 function. We find that directed exploration guided by maximum variance provides better performance overall, converging faster across several data sets. However, for certain problems, the trade-off methods incorporating exploitation can perform at least as well, if not better than maximum variance. Thus, we discuss how the choice of the utility function depends on the distribution of the data, the model performance and uncertainties, additive noise as well as the budget., Comment: 15 pages and 15 figures,submitted to Physical Review Materials

Typical ferroelectrics possess a large spontaneous polarization Ps but simultaneously a large remnant polarization Pr as well, resulting in an inferior energy storage density.A mechanism that can reduce the Pr while maintain the Ps is demanded to enhance the energy storage property of ferroelectrics.In the present study, it is shown that after acceptor doping and aging treatment, the domain switching in ferroelectrics becomes reversible, giving rise to a pinched double hysteresis loop. The pinched loop with a large Ps and a small Pr thus results in an enhanced energy storage density. The physics behind is a defect induced internal field that provides a restoring force for the domains to switch back.The idea is demonstrated through a time-dependent Ginzburg-Landau simulation as well as experimental measurements in BaTiO$_3$ based single crystal and ceramics. The mechanism is general and can be applied to various ferroelectrics, especially the environment-friendly ones., Comment: under submission to RCS JMCA

Stacking fault energy (SFE) plays an important role in deformation mechanisms and mechanical properties of face-centered cubic (fcc) metals and alloys. In metastable fcc alloys, the SFEs determined from density functional theory (DFT) calculations and experimental methods often have opposite signs. Here, we show that the negative SFE by DFT reflects the thermodynamic instability of the fcc phase relative to the hexagonal close-packed one; while the experimentally determined SFEs are restricted to be positive by the models behind the indirect measurements. We argue that the common models underlying the experimental measurements of SFE fail in metastable alloys. In various concentrated solid solutions, we demonstrate that the SFEs obtained by DFT calculations correlate well with the primary deformation mechanisms observed experimentally, showing a better resolution than the experimentally measured SFEs. Furthermore, we believe that the negative SFE is important for understanding the abnormal behaviors of partial dislocations in metastable alloys under deformation. The present work advances the fundamental understanding of SFE and its relation to plastic deformations, and sheds light on future alloy design by physical metallurgy.

Lateral heterostructures of two-dimensional (2D) materials, integrating different phases or materials into a single piece of nanosheet, have attracted intensive research interests in the past few years for high-performance electronic and optoelectronic devices. It also holds promises to significantly improve the performance and enable new functions of spintronic devices. It is imperative to have a 2D material possessing diverse electronic and magnetic properties that are required in spintronics. In this work, using density functional theory calculations, we surveyed all IV, V and VI group transition metal dichalcogenides (TMDs) and discovered that CrS2 has the most diverse electronic and magnetic properties: antiferromagnetic (AFM) metallic 1T phase, nonmagnetic (NM) semiconductor 2H phase, and ferromagnetic (FM) semiconductor 1T_prime phase with a Curie temperature of ~1000 K. More interestingly, we found that a tensile or compressive strain could turn 1T_prime phase into a spin-up or spin-down half metal. Such a unique feature enables designing strain-controlled spintronic devices using a single piece of CrS2 crystal with improved energy efficiency, which remains a challenge in miniaturization of spintronic devices. In-depth analysis attributed the unique strain tunability to the interplay between strain-induced lattice deformation and different spatial orientation of the spin-up/spin-down electronic orbitals. A prototypical design of a simple spin-valve logic device operated by strain is also presented., Comment: 40 pages, 6 figures in main text, 17 figures in SI

The 1T_prime phase of transition metal dichalcogenides (TMDs) is a low symmetry charge density wave (CDW) phase, which can be regarded as a periodically distorted structure (Peierls distortion) of the high symmetry 1T phase. In this paper, using density functional theory (DFT) calculations, we report that the positive charge (hole) injection is an effective method to modulate the Peierls distortion of MoS2 1T_prime for new CDW phase and superior electromechanical properties. A new stable CDW phase is discovered at hole doping level of ~ 0.10h+/atom, named as 1Tt_prime. The hole charging and discharging can induce a reversible phase transition of MoS2 among the three phases, 1T, 1T_prime and 1Tt_prime. Such reversible phase transition leads to superior electromechanical properties including a strain output as high as -5.8% with a small hysteresis loop, multi-step super-elasticity, and multi-shape memory effect, which are valuable in active electromechanical device designs at nanoscale. In-depth analysis on the change of electronic structure under hole doping was performed to understand the new CDW phase and the observed phase transition. Using charge doping to modulate the Peierls distortion in two-dimensional materials can serve as a general concept for nano-active material designs., Comment: 28 pages, 5 figures in main text, 10 figures in supporting information