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Superconductivity from Domain Wall Fluctuations in Sliding Ferroelectrics

Bilayers of two-dimensional van der Waals materials that lack an inversion center can show a novel form of ferroelectricity, where certain stacking arrangements of the two layers lead to an interlayer polarization. Under an external out-of-plane electric field, a relative sliding between the two layers can occur, accompanied by an interlayer charge transfer and a ferroelectric switching. We show that the domain walls that mediate ferroelectric switching are a locus of strong attractive interactions between electrons. The attraction is mediated by the ferroelectric domain wall fluctuations, effectively driven by the soft interlayer shear phonon. We comment on the possible relevance of this attraction mechanism to the recent observation of an interplay between sliding ferroelectricity and superconductivity in bilayer T 𝑑 −MoTe 2 . We also discuss the possible role of this mechanism in the superconductivity of moiré bilayers.

Chaudhary, Gaurav [Univ. of Cambridge (United King

Creating and Probing Large Gap 2D Topological Insulators for Quantum Computing (Final Report)

Research under this award focused on experimental and theoretical efforts in developing and characterizing 2D topological insulators (TIs). Key areas of investigation included materials synthesis, device fabrication and characterization, and theoretical advancements. The team synthesized ZrTe 5 , a material with potential for TI phases. Additionally, the team pursued the synthesis of elemental thin films like Indene and Bismuthene, known for their large TI gaps. Indene was successfully stabilized on SiC. Another approach involved stacking and twisting transition metal dichalcogenides (TMDs) to engineer desired TI band structures. On the theoretical front, advancements made under this award predicted remarkable topological properties in twisted WSe2 bilayers, motivating experimental efforts to realize these states. Regarding device fabrication and characterization, significant progress was made in reducing contact resistance, crucial for reliable transport measurements. Contactless Pulsed Tunneling Spectroscopy (CPTS) was employed to study the electronic properties of WTe 2 and WSe 2 . However, challenges in device fabrication and electrode material selection hampered efforts to obtain desired spectra. Ancillary work, utilizing pulsed electrical methods, on the study of sliding ferroelectrics yielded impactful results demonstrating high speed operation and lack of degradation of devices after many billions of cycles.

77 NANOSCIENCE AND NANOTECHNOLOGY

Revealing atomic-scale switching pathways in van der Waals ferroelectrics

Two-dimensional (2D) van der Waals (vdW) materials hold the potential for ultrascaled ferroelectric (FE) devices due to their silicon compatibility and robust polarization down to atomic scale. However, the inherently weak vdW interactions enable facile sliding between layers, introducing complexities beyond those encountered in conventional ferroelectric materials and presenting substantial challenges in uncovering intricate switching pathways. Here, we combine atomic-resolution imaging under in situ electrical biasing conditions with first-principles calculations to unravel the atomic-scale switching mechanisms in SnSe, a vdW group IV monochalcogenide. Our results uncover the coexistence of a consecutive 90° switching pathway and a direct 180° switching pathway from antiferroelectric (AFE) to FE order in this vdW system. Atomic-scale investigations and strain analysis reveal that the switching processes simultaneously induce interlayer sliding and compressive strain, while the lattice remains coherent despite the presence of multidomain structures. These findings elucidate vdW ferroelectric switching dynamics at atomic scale and lay the foundation for the rational design of 2D ferroelectric nanodevices.

Li, Xinyan [Rice University, Houston, TX (United S

Room-temperature multiferroicity in sliding van der Waals semiconductors with sub-0.3 V switching

The search for van der Waals (vdW) multiferroic materials has been challenging but also holds great potential for the next-generation multifunctional nanoelectronics. The group-IV monochalcogenide, with an anisotropic puckered structure and an intrinsic in-plane polarization at room temperature, manifests itself as a promising candidate with coupled ferroelectric and ferroelastic order as the basis for multiferroic behavior. Unlike the intrinsic centrosymmetric AB stacking, we demonstrate a multiferroic phase of tin selenide (SnSe), where the inversion symmetry breaking is maintained in AA-stacked multilayers over a wide range of thicknesses. We observe that an interlayer-sliding-induced out-of-plane (OOP) ferroelectric polarization couples with the in-plane (IP) one, making it possible to control out-of-plane polarization via in-plane electric field and vice versa. Notably, thickness scaling yields a sub-0.3 V ferroelectric switching, which promises future low-power-consumption applications. Furthermore, coexisting armchair- and zigzag-like structural domains are imaged under electron microscopy, providing experimental evidence for the degenerate ferroelastic ground states theoretically predicted. Non-centrosymmetric SnSe, as the first layered multiferroic at room temperature, provides a novel platform not only to explore the interactions between elementary excitations with controlled symmetries, but also to efficiently tune the device performance via external electric and mechanical stress.

Chen, Rui [University of California, Berkeley, CA

Identifying Strain Stacking Boundaries between Multiphase Domains in Atomically Thin Two-Dimensional Magnets

Stacking engineering of van der Waals materials is an important strategy to control the materials’ properties, such as electronic correlations, ferroelectricity, and layer-dependent two-dimensional magnetism. A timely testbed for the study of the latter is atomically thin chromium trihalides (CrX 3 , X = Cl, Br, I). Notably, by understanding the sliding mechanism between different stacking sequences, control of the stacking arrangement, and thus magnetic properties in CrX 3 , can be achieved. Such insight, however, is currently lacking. Here, in this study, advanced electron microscopy methods are used to identify multiple stacking sequences corresponding to different bulk phases in atomically thin CrX 3 (X = Cl and Br) down to bilayer thickness and with lateral domain sizes as small as tens of nanometers. Indications of nanometer scale transitions and interactions at the stacking boundaries are found, including a universally preferred sliding direction that is consistent with density functional theory calculations and the strain fields at lateral heterostructure boundaries. This study demonstrates the necessity to consider local stacking structures when interpreting averaged magnetic properties measured with macroscale probes. Additionally, the preferred sliding direction insight from this study provides a strategy to control stacking sequence in atomically thin CrX 3 samples during the exfoliation and sample fabrication process.

DFT calculations

Mapping causal patterns in crystalline solids

The evolution of the atomic structures of the combinatorial library of Sm-substituted thin film BiFeO 3 along the phase transition boundary from the ferroelectric rhombohedral phase to the non-ferroelectric orthorhombic phase is explored using scanning transmission electron microscopy. Localized properties, including polarization, lattice parameter, and chemical composition, are parameterized from atomic-scale imaging, and their causal relationships are reconstructed using a linear non-Gaussian acyclic model. This approach is further extended to explore the spatial variability of the causal coupling using the sliding window transform method, which revealed that new causal relationships emerged at both the expected locations, such as domain walls and interfaces, and at additional regions forming clusters in the vicinity of the walls or spatially distributed features. While the exact physical origins of these relationships are unclear, they likely represent nanophase-separated regions in the morphotropic phase boundaries. Overall, we posit that an in-depth understanding of complex disordered materials away from thermodynamic equilibrium necessitates understanding not only the generative processes that can lead to observed microscopic states but also the causal links between multiple interacting subsystems.

Causal inference