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Despite ongoing efforts aimed at increasing energy density in all-solid-state-batteries, the optimal composite cathode morphology, which requires minimal volume change, small void development, and good interfacial contact, remains a significant concern within the community. In this work, we focus on the theoretical investigation of the above-mentioned mechanical defects in the composite cathode during electrochemical cycling. It is demonstrated that these mechanical defects are highly dependent on the SE material properties, the external stack pressure and the cathode active material (CAM) loading. The following conclusions are highlighted in this study: (1) Higher CAM loading (>50 vol. %) causes an increase in mechanical defects, including large cathode volume change (>5%), contact loss (50%) and porosity (>1%). (2) High external stack pressure up to 7MPa reduces mechanical defects while preventing internal fracture in the cathode. (3) Soft SE materials with small Youngs modulus (<10GPa) and low hardness (<2GPa) can significantly minimize these mechanical defects during cycling. (4) A design strategy is proposed for high CAM loading with minimal mechanical defects when different SE materials are utilized in the composite cathode, including oxide-type SE, sulfide-type SE, and halide-type SE. The research provides specific guidelines to optimize the composite cathode in terms of mechanical properties. These guidelines broaden the design approach towards improving the performance of SSB, by highlighting the importance of considering the mechanical properties of battery materials., Comment: 20 pages, 8 figures

Using first-principles calculations and group-theory based models, we study the stabilization of ferrielectricity (FiE) in CuInP$_2$Se$_6$. We find that the FiE ground state is stabilized by a large anharmonic coupling between the polar mode and a fully symmetric Raman-active mode. Our results open possibilities for controlling the single-step switching barrier for polarization by tuning the Raman-active mode. We discuss the implications of our findings in the context of designing next-generation optoelectronic devices that can overcome the voltage-time dilemma.

Transition-metal dichalcogenides containing tellurium anions show remarkable charge-lattice modulated structures and prominent interlayer character. Using cryogenic scanning transmission electron microscopy (STEM), we map the atomic-scale structures of the high temperature (HT) and low temperature (LT) modulated phases in 1T'-TaTe$_{2}$. At HT, we directly show in-plane metal distortions which form trimerized clusters and staggered, three-layer stacking. In the LT phase at 93 K, we visualize an additional trimerization of Ta sites and subtle distortions of Te sites by extracting structural information from contrast modulations in plan-view STEM data. Coupled with density functional theory calculations and image simulations, this approach opens the door for atomic-scale visualizations of low temperature phase transitions and complex displacements in a variety of layered systems.

Stacking order can significantly influence the physical properties of two-dimensional (2D) van der Waals materials. The recent isolation of atomically thin magnetic materials opens the door for control and design of magnetism via stacking order. Here we apply hydrostatic pressure up to 2 GPa to modify the stacking order in a prototype van der Waals magnetic insulator CrI3. We observe an irreversible interlayer antiferromagnetic (AF) to ferromagnetic (FM) transition in atomically thin CrI3 by magnetic circular dichroism and electron tunneling measurements. The effect is accompanied by a monoclinic to a rhombohedral stacking order change characterized by polarized Raman spectroscopy. Before the structural change, the interlayer AF coupling energy can be tuned up by nearly 100% by pressure. Our experiment reveals interlayer FM coupling, which is the established ground state in bulk CrI3, but never observed in native exfoliated thin films. The observed correlation between the magnetic ground state and the stacking order is in good agreement with first principles calculations and suggests a route towards nanoscale magnetic textures by moir\'e engineering.

We report measurements of current-induced torques in heterostructures of Permalloy (Py) with TaTe$_2$, a transition-metal dichalcogenide (TMD) material possessing low crystal symmetry, and observe a torque component with Dresselhaus symmetry. We suggest that the dominant mechanism for this Dresselhaus component is not a spin-orbit torque, but rather the Oersted field arising from a component of current that flows perpendicular to the applied voltage due to resistance anisotropy within the TaTe$_2$. This type of transverse current is not present in wires made from a single uniform layer of a material with resistance anisotropy, but will result whenever a material with resistance anisotropy is integrated into a heterostructure with materials having different resistivities, thereby producing a spatially non-uniform pattern of current flow. This effect will therefore influence measurements in a wide variety of heterostructures incorporating 2D TMD materials and other materials with low crystal symmetries.

As electrical control of N\'eel order opens the door to reliable antiferromagnetic spintronic devices, understanding the microscopic mechanisms of antiferromagnetic switching is crucial. Spatially-resolved studies are necessary to distinguish multiple nonuniform switching mechanisms; however, progress has been hindered by the lack of tabletop techniques to image the N\'eel order. We demonstrate spin Seebeck microscopy as a sensitive, table-top method for imaging antiferromagnetic order in thin films, and apply this technique to study spin-torque switching in NiO/Pt and Pt/NiO/Pt heterostructures. We establish the interfacial antiferromagnetic spin Seebeck effect in NiO as a probe of surface N\'eel order, resolving antiferromagnetic spin domains within crystalline twin domains. By imaging before and after applying current-induced spin torque, we resolve spin domain rotation and domain wall motion, acting simultaneously. We correlate the changes in spin Seebeck images with electrical measurements of the average N\'eel orientation through the spin Hall magnetoresistance, confirming that we image antiferromagnetic order., Comment: 26 pages including supporting information

We report the connection between the stacking order and magnetic properties of bilayer CrI$_3$ using first-principles calculations. We show that the stacking order defines the magnetic ground state. By changing the interlayer stacking order one can tune the interlayer exchange interaction between antiferromagnetic and ferromagnetic. To measure the predicted stacking-dependent magnetism, we propose using linear magnetoelectric effect. Our results not only gives a possible explanation for the observed antiferromagnetism in bilayer CrI$_3$ but also have direct implications in heterostructures made of two-dimensional magnets.

Systems that simultaneously exhibit superconductivity and spin-orbit coupling are predicted to provide a route toward topological superconductivity and unconventional electron pairing, driving significant contemporary interest in these materials. Monolayer transition-metal dichalcogenide (TMD) superconductors in particular lack inversion symmetry, enforcing a spin-triplet component of the superconducting wavefunction that increases with the strength of spin-orbit coupling. In this work, we present an experimental and theoretical study of two intrinsic TMD superconductors with large spin-orbit coupling in the atomic layer limit, metallic 2H-TaS$_2$ and 2H-NbSe$_2$. For the first time in TaS$_2$, we investigate the superconducting properties as the material is reduced to a monolayer and show that high-field measurements point to the largest upper critical field thus reported for an intrinsic TMD superconductor. In few-layer samples, we find that the enhancement of the upper critical field is sustained by the dominance of spin-orbit coupling over weak interlayer coupling, providing additional platforms for unconventional superconducting states in two dimensions., Comment: 8 pages, 4 figures, plus supplemental material

The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. Here we create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 photoluminescence intensity strongly depends on the relative alignment between photo-excited spins in WSe2 and the CrI3 magnetization, due to ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure., Comment: Supplementary Materials included. To appear in Science Advances

Using symmetry arguments and a tight-binding model, we show that for layered collinear anti- ferromagnets, magneto-optic effects can be generated and manipulated by controlling crystal symmetries through a gate voltage. This provides a promising route for electric field manipulation of the magneto-optic effects without modifying the underlying magnetic structure. We further demonstrate the gate control of magneto-optic Kerr effect (MOKE) in bilayer MnPSe3 using first-principles calculations. The field-induced inversion symmetry breaking effect leads to gate-controllable MOKE whose direction of rotation can be switched by the reversal of the gate voltage.

Layered transition metal trichalcogenides with the chemical formula $ABX_3$ have attracted recent interest as potential candidates for two-dimensional magnets. Using first-principles calculations within density functional theory, we investigate the magnetic ground states of monolayers of Mn- and Cr-based semiconducting trichalcogenides. We show that the second and third nearest-neighbor exchange interactions ($J_2$ and $J_3$) between magnetic ions, which have been largely overlooked in previous theoretical studies, are crucial in determining the magnetic ground state. Specifically, we find that monolayer $\text{CrSiTe}_3$ is an antiferromagnet with a zigzag spin texture due to significant contribution from $J_3$, whereas $\text{CrGeTe}_3$ is a ferromagnet with a Curie temperature of 106 K. Monolayers of Mn-compounds ($\text{MnPS}_3$ and $\text{MnPSe}_3$) always show antiferromagnetic Neel order. We identify the physical origin of various exchange interactions, and demonstrate that strain can be an effective knob for tuning the magnetic properties. Possible magnetic ordering in the bulk is also discussed. Our study suggests that $\text{ABX}_3$ can be a promising platform to explore 2D magnetic phenomena., Comment: 7 pages, 5 figures, 1 table

The electronic structure of SrTiO3(001) surfaces was studied using scanning tunneling spectroscopy and density-functional theory. With high dynamic range measurements, an in-gap transition level was observed on SrO-terminated surfaces, at 2.7 eV above the valence band maximum. The density of centers responsible for this level was found to increase with surface segregation of oxygen vacancies and decrease with exposure to molecular oxygen. Based on these finding, the level is attributed to surface O vacancies. A level at a similar energy is predicted theoretically on SrO-terminated surfaces. For TiO2-terminated surfaces, no discrete in-gap state was observed, although one is predicted theoretically. This lack of signal is believed to be due to the nature of defect wavefunction involved, as well as the possible influence of transport limitations in the tunneling spectroscopy measurements., Comment: 17 pages, 8 figures