Materials Science (cond-mat.mtrl-sci)

Abstract: Artificial intelligence (AI) has emerged as a powerful tool in the discovery and optimization of novel battery materials. However, the adoption of AI in battery cathode representation and discovery is still limited due to the complexity of optimizing multiple performance properties and the scarcity of high-fidelity data. In this study, we present a comprehensive machine-learning model (DRXNet) for battery informatics and demonstrate the application in discovery and optimization of disordered rocksalt (DRX) cathode materials. We have compiled the electrochemistry data of DRX cathodes over the past five years, resulting in a dataset of more than 30,000 discharge voltage profiles with 14 different metal species. Learning from this extensive dataset, our DRXNet model can automatically capture critical features in the cycling curves of DRX cathodes under various conditions. Illustratively, the model gives rational predictions of the discharge capacity for diverse compositions in the Li--Mn--O--F chemical space and high-entropy systems. As a universal model trained on diverse chemistries, our approach offers a data-driven solution to facilitate the rapid identification of novel cathode materials, accelerating the development of next-generation batteries for carbon neutralization.

Abstract: A combined study employing density functional theory (DFT) using the experimentally determined modulated structures and bulk-sensitive hard x-ray photoelectron spectroscopy on single-crystalline Ni$_2$MnGa is presented in this work. For the aforementioned modulated structures, all of the characteristic features in the experimental valence band (VB) are in excellent agreement with the theoretical VB calculated from DFT, evincing that it is the true representation of Ni$_2$MnGa in the martensite phase. We establish the existence of a charge density wave (CDW) state in the martensite phase from the shape of the VB near $E_F$ that shows a transfer of spectral weight in excellent agreement with DFT. Furthermore, presence of a pseudogap is established by fitting the near $E_F$ region with a power law function predicted theoretically for the CDW phase. Thus, the present work emphasizes that the atomic modulation plays an important role in hosting the CDW phase in bulk stoichiometric Ni$_2$MnGa.

Abstract: Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high performance donor-acceptor systems. Here, we probe the origin of field-dependent free charge generation and photoluminescence in non-fullerene acceptor (NFA) based organic solar cells using the polymer PM6 and NFA Y5 - a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of samples with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artefacts from non-geminate recombination of photogenerated- and dark charge carriers near the electrodes. We then correlate free charge generation with steady state photoluminescence intensity, and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low offset system is entirely controlled by the field dependent exciton dissociation into charge transfer states.

Abstract: We study monochromatic linearly-polarized laser-induced band structure modifications in material systems with valley (graphene and hexagonal-Boron-Nitride), and topological (Dirac and Weyl semimetals), properties. We find that for Dirac-like linearly-dispersing bands, the laser dressing effectively moves the Dirac nodes away from their original position by up to ~10% of the Brillouin zone (opening a large pseudo-gap in their original position). The direction of the movement can be fully controlled by rotating the laser polarization axis. We prove that this effect originates from band nonlinearities away from the Dirac nodes (without which the effect completely vanishes, and which are often neglected). We demonstrate that this physical mechanism is applicable beyond two-dimensional Dirac semimetals, and can move the positions of the valley minima in hexagonal materials to tune valley selectivity, split and move Weyl cones in higher-order Weyl semimetals, and merge Dirac nodes in three-dimensional topological Dirac semimetals. The model results are validated with ab-initio time-dependent density functional theory calculations. Our results directly affect theoretical and experimental efforts for exploring light-dressed electronic-structure, suggesting that one can benefit from band nonlinearity for tailoring material properties. They also highlight the importance of describing the full band structure in nonlinear optical phenomena in solids.

Abstract: Material deformation and failure under impact loading is a subject of active investigation in space science and often requires very specialized equipment for testing. In this work, we present the design, operational analysis and application of a low-velocity ($\sim 100$ m/s) projectile impact framework for evaluating the deformation and failure of space-grade materials. The system is designed to be modular and easily adaptable to various test geometries, while enabling accurate quantitative evaluation of plastic flow. Using coupled numerical methods and experimental techniques, we first establish an operating procedure for the system. Following this, its performance in two complementary impact configurations is demonstrated using numerical and experimental analysis. In the first, a Taylor impact test is performed for predicting the deformed shape of a cylindrical projectile impinging on a rigid substrate. In the second, deformation of a plate struck by a rigid projectile is evaluated. In both cases, physics-based models are used to interpret the resulting fields. We present a discussion of how the system may be used both for material property estimation (e.g., dynamic yield strength) as well as for failure evaluation (e.g., perforation and fracture) in the same projectile impact configuration.

Abstract: Efficient generation and manipulation of spin signals in a given material without invoking external magnetism remain one of the challenges in spintronics. The spin Hall effect (SHE) and Rashba-Edelstein effect (REE) are well-known mechanisms to electrically generate spin accumulation in materials with strong spin-orbit coupling (SOC), but the exact role of the strength and type of SOC, especially in crystals with low symmetry, has yet to be explained. In this study, we investigate REE in two different families of non-magnetic chiral materials, elemental semiconductors (Te and Se) and semimetallic disilicides (TaSi$_2$ and NbSi$_2$), using an approach based on density functional theory (DFT). By analyzing spin textures across the full Brillouin zones and comparing them with REE magnitudes calculated as a function of chemical potential, we link specific features in the electronic structure with the efficiency of the induced spin accumulation. Our findings show that magnitudes of REE can be increased by: (i) the presence of purely radial (Weyl-type) spin texture manifesting as the parallel spin-momentum locking, (ii) high spin polarization of bands along one specific crystallographic direction, (iii) low band velocities. By comparing materials possessing the same crystal structures, but different strengths of SOC, we conclude that larger SOC may indirectly contribute to the enhancement of REE. It yields greater spin-splitting of bands along specific crystallographic directions, which prevents canceling the contributions from the oppositely spin-polarized bands over wider energy regions and helps maintain larger REE magnitudes. We believe that these results will be useful for designing spintronics devices and may aid further computational studies searching for efficient REE in materials with different symmetries and SOC strengths.

Abstract: As a recent successfully exfoliated non van der Waals layered material, AgCrS2 has received a lot of attentions. Motivated by its structure related magnetic and ferroelectric behavior, a theoretical study on its exfoliated monolayer AgCr2S4 has been carried out in the present work. Based on density functional theory, the ground state and magnetic order of monolayer AgCr2S4 have been determined. The centrosymmetry emerges upon two-dimensional confinement and thus eliminates the bulk polarity. Moreover, two-dimensional ferromagnetism appears in the CrS2 layer of AgCr2S4 and can persist up to room temperature. The surface adsorption has also been taken into consideration, which shows a nonmonotonic effect on the ionic conductivity through ion displacement of the interlayer Ag, but has little impact on the layered magnetic structure.

Abstract: Confronting the unveiled sophisticated multiscale structural and physical characteristics of hysteresis simulation of permanent magnets, notably samarium-cobalt (Sm-Co) alloy, a novel scheme is proposed linking physics-based micromagnetics on the nanostructure level and magnetostatic homogenization on the mesoscale polycrystal level. Thereby the micromagnetics-informed surrogate hysteron is the key to bridge the scales of nanostructure and polycrystal structure. This hysteron can readily emulate the local magnetization reversal with the nanoscale mechanisms considered, such as nucleation of domains, and domain wall migration and pinning. The overall hysteresis, based on a sintered Sm-Co polycrystal, considering both mesoscale and nanoscale characteristics, is simulated and discussed.

Abstract: KTaO${}_{3}$ presents a rich hyper-Raman spectrum originating from two-phonon processes at the Brillouin zone boundary, indicating the possibility of driving these phonon modes using intense midinfrared laser sources. We obtained the coupling of light to the highest-frequency longitudinal optic phonon mode $Q_{\rm{HY}}$ at the $X$ $(0,0, \frac{1}{2})$ point by first principles calculations of the total energy as a function of the phonon coordinate $Q_{\rm{HY}}$ and electric field $E$. We find that the energy curve as a function of $Q_{\rm{HY}}$ softens for finite values of electric field, indicating the presence of $Q_{\rm{HY}}^2 E^2$ nonlinearity with negative coupling coefficient. We studied the feasibility of utilizing this nonlinearity to transiently break the translation symmetry of the material by making the $Q_{\rm{HY}}$ mode unstable with an intense midinfrared pump pulse. We also considered the possibility that nonlinear phonon-phonon couplings can excite the lowest-frequency phonon coordinates $Q_{\rm{LZ}}$ and $Q_{\rm{LX}}$ at $X$ when the $Q_{\rm{HY}}$ mode is externally driven. The nonlinear phonon-phonon couplings were also obtained from first principles via total-energy calculations as a function of the phonon coordinates, and these were used to construct the coupled classical equations of motion for the phonon coordinates in the presence of an external pump term on $Q_{\rm{HY}}$. We numerically solved them for a range of pump frequencies and amplitudes and found three regimes where the translation symmetry is broken: i) rectification of the lowest-frequency coordinates due to large amplitude oscillation of the $Q_{\rm{HY}}$ coordinate about its equilibrium position, ii) rectification of only the $Q_{\rm{HY}}$ coordinate without displaced oscillations of the lowest-frequency coordinates, and iii) rectification of all three coordinates.

Abstract: Ni-Mn-based Heusler alloys like Ni-Mn-Sn show an elastocaloric as well as magnetocaloric effect during the magneto-structural phase transition, making this material interesting for solid-state cooling application. Material processing by additive manufacturing can overcome difficulties related to machinability of the alloys, caused by their intrinsic brittleness. Since the magnetic properties and transition temperature are highly sensitive to the chemical composition, it is essential to understand and monitoring these properties over the entire processing chain. In the present work the microstructural and magnetic properties from gas-atomized powder to post-processed Ni-Mn-Sn alloy are investigated. Direct energy deposition was used for processing, promoting the evolution of a polycrystalline microstructure being characterized by elongated grains along the building direction. A complete and sharp martensitic transformation can be achieved after applying a subsequent heat treatment at 1173 K for 24 h. The Mn-evaporation of 1.3 at. % and the formation of Mn-oxide during DED-processing lead to an increase of the transition temperature of 45 K and a decrease of magnetization, clearly pointing at the necessity of controlling the composition, oxygen partial pressure and magnetic properties over the entire processing chain.