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In the field of photocatalytic water splitting, no current studies have explicitly investigated the coexistence of multiple band-edge alignments in two-dimensional (2D) materials with intrinsic electric fields. In this Letter, we designed the ternary pentagonal CdSeTe monolayer, and proposed a novel concept called atom-valley locking, which could provide multiple band-edge positions. In the CdSeTe monolayer, two distinct valleys emerge in the electronic structure, one contributed by Se atoms and the other by Te atoms, with a spontaneous polarization of 187 meV between them. This phenomenon can be attributed to the localization of valley electrons and the breaking of four-fold rotational reflection symmetry, yet it does not rely on the breaking of time-reversal symmetry. Due to the atom-dependent valley distribution, two types of band-edge alignments can be identified. Moreover, selective switching between them can be achieved by strain engineering, thereby enabling precise control over the site of the hydrogen evolution reaction. Our findings open up new opportunities for exploring valley polarization and provide unique insights into the photocatalytic applications of 2D materials with intrinsic electric fields.

Mn3TeO6 (MTO) has been experimentally found to adopt a P21/n structure under high pressure, which exhibits a significantly smaller band gap compared to the atmospheric R-3 phase. In this study, we systematically investigate the magnetism, structural phase transition and electronic properties of MTO under high pressure through first-principles calculations. Both R-3 and P21/n phases of MTO are antiferromagnetic at zero temperature. The R-3 phase transforms to the P21/n phase at 7.58 GPa, accompanied by a considerable volume collapse of about 6.47%. Employing the accurate method that combines DFT+U and G0W0, the calculated band gap of R-3 phase at zero pressure is very close to the experimental values, while that of the P21/n phase is significantly overestimated. The main reason for this difference is that the experimental study incorrectly used the Kubelka-Munk plot for the indirect band gap to obtain the band gap of the P21/n phase instead of the Kubelka-Munk plot for the direct band gap. Furthermore, our study reveals that the transition from the R-3 phase to the P21/n phase is accompanied by a slight reduction in the band gap., Comment: 17 pages, 11 figures

Constitutive models are essential for describing the mechanical behavior of materials under high temperatures and pressures, among which the Steinberg-Guinan (SG) model is widely adopted. Recent work has discovered a peculiar dual anomaly of compression-induced softening and heating-induced hardening in the elasticity of compressed vanadium [Phys. Rev. B 104, 134102 (2021)], which is beyond the capability of the SG model to describe. In this work, a modified SG constitutive model is proposed to embody such an anomalous behavior. Elemental vanadium is considered as an example to demonstrate the effectiveness of this improved model in describing the dual anomalies of mechanical elasticity. This new variant of the SG model can also be applied to other materials that present an irregular variation in the mechanical elasticity, and is important to faithfully model and simulate the mechanical response of materials under extreme conditions., Comment: 14 pages, 4 figures

In this paper, the electrical transport, thermal transport, and thermoelectric properties of three new Janus STe$_{2}$, SeTe$_{2}$, and Se$_{2}$Te monolayers are systematically studied by first-principles calculations, as well as the comparative with available literature's results using different methods. It is found that the Seebeck coefficient and conductivity have opposite dependence on temperature, and we illustrate this phenomenon in detail. The decrease of the thermoelectric power factor (PF) with temperature originates from the decrease in conductivity. To obtain accurate and convergent lattice thermal conductivity, the root mean square (RMS) is calculated to obtain a reasonable cutoff radius for the calculation of third-order forces. Janus STe$_{2}$, SeTe$_{2}$, and Se$_{2}$Te monolayers exhibit ultra-low lattice thermal conductivity of 0.2, 0.133, and 4.81$\times10^{-4}$ W/mK at 300 K, which result from the strong coupling effect between the acoustic mode and the low-frequency optical branch, low phonon group velocity, small phonon lifetime, and large anharmonicity. Consequently, ultra-high $\textit{ZT}$ values of 2.11 (2.09), 3.28 (4.24), and 3.40 (6.51) for n-type(p-type) carrier doping of STe$_{2}$, SeTe$_{2}$, and Se$_{2}$Te are obtained, indicating that they are promising thermoelectric materials., Comment: 7 pages, 7 figures

Studying the physical properties of materials under high pressure and temperature through experiments is difficult. Theoretical simulations can compensate for this deficiency. Currently, large-scale simulations using machine learning force fields are gaining popularity. As an important nuclear energy material, the evolution of the physical properties of uranium under extreme conditions is still unclear. Herein, we trained an accurate machine learning force field on alpha-U and predicted the lattice dynamics and elastic properties at high pressures and temperatures. The force field agrees well with the ab initio molecular dynamics (AIMD) and experimental results, and it exhibits higher accuracy than classical potentials. Based on the high-temperature lattice dynamics study, we first present the temperature-pressure range in which the Kohn anomalous behavior of the ${\Sigma}$4 optical mode exists. Phonon spectral function analysis showed that the phonon anharmonicity of alpha-U is very weak. We predict that the single-crystal elastic constants C44, C55, C66, polycrystalline modulus (E,G), and polycrystalline sound velocity ($C_L$,$C_S$) have strong heating-induced softening. All the elastic moduli exhibited compression-induced hardening behavior. The Poisson's ratio shows that it is difficult to compress alpha-U at high pressures and temperatures. Moreover, we observed that the material becomes substantially more anisotropic at high pressures and temperatures. The accurate predictions of alpha-U demonstrate the reliability of the method. This versatile method facilitates the study of other complex metallic materials., Comment: 21 pages, 9 figures, with Supplementary Material

Elasticity is one of the most fundamental mechanical properties of solid. In high-throughput design of advanced materials, there is an imperative demand for the capability to quickly calculate and screen a massive pool of candidate structures. A fully automatized pipeline with minimal human intervention is the key to provide high efficiency to achieve the goal. Here, we introduce a tool-kit MyElas that aims to address this problem by forging all pre-processing, elastic constant and other related property calculations, and post-processing into an integrated framework that automatically performs the assigned tasks to drive data flowing through parallelized pipelines from input to output. The core of MyElas is to calculate the second and third order elastic constants of a solid with the energy-strain method from first-principles. MyElas can auto-analyze the elastic constants, to derive other related physical quantities. Furthermore, the tool-kit also integrates a visualization function, which can, for example, plot the spatial anisotropy of elastic modulus and sound velocity of monocrystalline. The validity and efficiency of the toolkit are tested and bench-marked on several typical systems., Comment: 31 pages, 8 figures

A large bulk band gap is critical for the applications of quantum spin hall (QSH) insulators in spintronics at room temperature. Based on first-principles calculations, we predict that the methyl-functionalized III-Bi monolayers, namely III-Bi-(CH3)2 (III=Ga, In, Tl) thin films, own QSH states with band gap as large as 0.260, 0.304 and 0.843 eV, respectively, making them suitable for room-temperature applications. The topological characteristics are confirmed by s-px,y band inversion, topological invariant Z2, and the topologically protected edge states. Noticeably, for GaBi/InBi-(CH3)2 films, the s-px,y band inversion occurred in the progress of spin-orbital coupling (SOC), while for TlBi(CH3)2 film, the s-px,y band inversion happened in the progress of chemical bonding. Significantly, the QSH states in III-Bi-(CH3)2 films are robust against the mechanical strains and various methyl coverages, making these films particularly flexible to substrate choice for device applications. Besides, the h-BN substrate is an ideal substrate for III-Bi-(CH3)2 films to realize large gap nontrivial topological states.. These findings demonstrate that the methyl-functionalized III-Bi films may be good QSH effect platforms for topological electronic devices design and fabrication in spintronics.

The application of high pressure can fundamentally modify the crystalline and electronic structures of elements as well as their chemical reactivity, which could lead to the formation of novel materials. Here, we explore the reactivity of lithium with sodium under high pressure, using a swarm structure searching techniques combined with first-principles calculations, which identify a thermodynamically stable LiNa compound adopting an orthorhombic oP8 phase at pressure above 355 GPa. The formation of LiNa may be a consequence of strong concentration of electrons transfer from the lithium and the sodium atoms into the interstitial sites, which also leads to opening a relatively wide band gap for LiNa-op8. This is substantially different from the picture that share or exchange electrons in common compounds and alloys. In addition, lattice-dynamic calculations indicate that LiNa-op8 remains dynamically stable when pressure decompresses down to 70 GPa., Comment: 14 pages, 6 figures

Orthorhombic GdFeO$_3$ has attracted considerable attention in recent years because its magnetic structure is similar to that in the well-known BiFeO$_3$ material. We investigate electronic structure, magnetism, and optical properties of the orthorhombic GdFeO$_3$ in terms of density-functional-theory calculations. The modified Becke-Johnson (mBJ) exchange potential is adopted to improve on the description of the electronic structure. Our calculation show that the G-type antiferromagnetic (G-AFM ordering of Fe spins) phase of orthorhombic GdFeO$_3$ is stable compared to other magnetic phases. The semiconductor gap calculated with mBJ, substantially larger than that with GGA, is in good agreement with recent experimental values. Besides, we also investigate effect of the spin-orbit coupling on the electronic structure, and calculate with mBJ the complex dielectric functions and other optical functions of photon energy. The magnetic exchange interactions are also investigated, which gives a Neel temperature close to experimental observation. For comparison towards supporting our results, we study the electronic structure of rhombohedral (R3c) BiFeO$_3$ with mBJ. These lead to a satisfactory theoretical understanding of the electronic structure, magnetism, and optical properties of orthorhombic GdFeO$_3$ and can help elucidate electronic structures and optical properties of other similar materials., Comment: 8 pages, 5 figures

Chemical functionalization is an effective means to tune electronic and crystal structure of two-dimensional material, which may be crucial for moder microelectronics industry. Based on the first-principle calculation and an iterative solution of Boltzmann transport equation, we find that antimony films are potential excellent thermoelectrical materials with rather low thermal conductivities $k$ ($<$ 2.5 W/mK). The chemical functionalization can induce the reduction in $k$ to some extent, which is mainly due to the reduction of phonon lifetimes limited by the anharmonic scattering. More interesting, the origin of the reduction in $k$ is not the anharmonic interaction but the harmonic interaction from the depressed phonon spectrum mechanism, and for some chemical functional atom in halogen, the flat modes appearing in the low frequency range play also a key factor in the reduction of $k$ by significantly increasing the three-phonon scattering channels. Our work analyzes the reduction mechanism in $k$ from the chemical functionalization for antimonene, and provides a new view to adjust the thermal conductivity which can benefit thermoelectric material design., Comment: 6 pages, 4 figures

By the generalized gradient approximation in framewok of density functional theory, we investigate a 2D topological insulator of new silicon allotrope (call dumbbell silicene synthesized recently by Cahangirov et al) through tuning external compression strain, and find a topological quantum phase transition from normal to topological insulator, i.e., the dumbbell silicene can turn a two-dimensional topological insulator with an inverted band gap. The obtained maximum topological nontrivial band gap about 12 meV under isotropic strain is much larger than that for previous silicene, and can be further improved to 36 meV by tuning anisotropic strain, which is sufficiently large to realize quantum spin Hall effect even at room-temperature, and thus is beneficial to the fabrication of high-speed spintronics devices. Furthermore, we confirm that the boron nitride sheet is an ideal substrate for the experimental realization of the dumbbell silicene under external strain, maintaining its nontrivial topology. These properties make the two-dimensional dumbbell silicene a good platform to study novel quantum states of matter, showing great potential for future applications in modern silicon-based microelectronics industry., Comment: 7 pages, 5 figures

Quantum spin Hall (QSH) state of matter has a charge excitation bulk bandgap and a pair of gapless spin-filtered edge-states, which can support backscattering-free transport. Bilayer phosphorene possesses a large tunable bandgap and high carrier mobilities, and therefore has the widely potential applications in nanoelectronics and optics. Here, we demonstrate an strain-induced electronic topological phase transition from a normal to QSH state in bilayer phosphorene accompanying by a band inversion that changes $\mathbbm{Z}_{2}$ from 0 to 1, which is highly dependent on the interlayer stacking. When the bottom layer is shifted by 1/2 unit cell along axial direction with respect to the top layer, the topological bandgap reaches up to 92.5 meV, which is sufficiently large to realize the QSH effect at room temperature. Its optical absorption spectrum becomes broadened, and even extends to the far-infra-red region leading to a wider range of brightness, which is highly desirable in optic devices., Comment: 33 pages, 6 figures