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Expanding the performance of field effect devices is a key challenge of the ever-growing chip industry at the core of current technologies. A highly desired nonvolatile response in tiny multiferroic transistors is expected by electric field control of atomic movements rather than the typical electronic redistribution. Recently, such field effect control of structural transitions was established in commensurate stacking configurations of honeycomb van der Waals (vdW) polytypes by sliding narrow boundary dislocations between oppositely polarized domains. The interfacial ferroelectric response, however, relied on preexisting boundary strips between relatively large micron-scale domains, severely limiting practical implementations. Here, we report the robust switching of single-domain polytypes in nm-scale islands embedded in super lubricant vdW arrays. We etch cavities into a thin layered spacer and then encapsulate it with parallel functional flakes. The incommensurate flakes above and under the spacer sag and touch at each cavity to form uniform crystalline islands free from interlayer deformations. By imaging the polytypes' ferroelectric response, we observe reversible nucleation and annihilation of boundary strips and geometry-adaptable hysteresis loops. Using mechanical stress, we accurately position the boundary strip, modify the interlayer twist angle, and nucleate intermediate polar domain patterns. By precisely designing the size, shape, symmetry, and distribution of the islands in these Super Lubricant Arrays of Polytype (SLAP), we envision numerous device functionalities and SlideTronics applications. These range from ultra-sensitive detectors of atomic-scale shifts to nonvolatile multi-ferroic tunneling transistors with tunable coercive switching fields, and even elastically-coupled memory cells for neuromorphic architectures.

Compared to electronic phase transitions, structural phase transitions of crystals are challenging to control due to the energy cost of breaking dense solid bonds. Recently, however, electric field switching of stacking configuration between honeycomb layers, held together by relatively weak van der Waals (vdW) attractions, was demonstrated. In response to the external fields, the layers slide between commensurate meta-stable configurations with discrete symmetries and distinct lattice orientations. These 2D vdW polytypes host diverse electronic orders such as ferroelectricity and magnetism, providing multiferroic switching via lubricant sliding of incommensurate boundary strips. Ahead, we address recent observations in honeycomb polytypes and identify remaining challenges for extending this conceptual "SlideTronics" mechanism into rapid, local, and practical multiferroic devices. The stacking energies, symmetries, and orbital overlaps that underlie the band structures and internal charge distributions are discussed, along with poly-properties like interfacial-ferroelectricity, ladder-like cumulative polarization, superconductivity, and orbital magnetic orders. Distinct from conventional 3D multiferroic crystals, the 2D vdW assembly and the sliding switching mechanism open poly-opportunities for novel device concepts.

Van der Waals (vdW) polytypes of broken inversion and mirror symmetries were recently shown to exhibit switchable electric polarization even at the ultimate two-layer thin limit. Their out-of-plane polarization was found to accumulate in a ladder-like fashion with each successive layer, offering 2D building blocks for the bottom-up construction of 3D ferroelectrics. Here, we demonstrate experimentally that beyond a critical stack thickness, the accumulated polarization in rhombohedral polytypes of molybdenum disulfide (r-MoS2) saturates. The underlying saturation mechanism, deciphered via DFT and self-consistent Poisson-Schr\"odinger calculations, point to a purely electronic redistribution involving: (1) polarization-induced bandgap closure that allows for cross-stack charge transfer and the emergence of free surface charge; (2) reduction of the polarization saturation value, as well as the critical thickness at which it is obtained, by the presence of free carriers. The resilience of polar layered structures to atomic surface reconstruction, which is essentially unavoidable in polar 3D crystals, potentially allows for the design of new devices with mobile surface charges. Our findings, which are of general nature, should be accounted for when designing switching and/or conductive devices based on ferroelectric layered materials.

Excitonic resonances in two-dimensional semiconductors play a crucial role in enhancing nonlinear light-matter interactions. However, the influence of resonant dynamics on the time-dependent behavior of these nonlinear effects has received little attention, as optical wave-mixing is commonly assumed to be instantaneous. In this study, we investigate the impact of excited state dynamics on the generation of second and third-order nonlinearities from Monolayer $\text{WSe}_\text{2}$ in ambient conditions. By shaping a sub-10fs driving pulse to complement the exciton resonant dynamics, we demonstrate a significant enhancement of four-wave-mixing beyond what is achieved using a transform-limited pulse. Conversely, a time-reversed pulse shape leads to destructive quantum interference effects, suppressing nonlinear generation. We apply this technique simultaneously to two successive exciton states, showcasing the selective choice in the resonant state that produces nonlinearity. The ability to control nonlinear carrier dynamics in two-dimensional semiconductors holds promise for remote noninvasive optical manipulation in optoelectronic devices.

A crystalline solid is a periodic sequence of identical cells, each containing one or more atoms. If the constituting unit cell is not centrosymmetric, charge may distribute unevenly between the atoms, resulting in internal electric polarization. This effect serves as the basis for numerous ferroelectric, piezoelectric, and pyroelectric phenomena. In nearly all polar materials, including multilayered van der Waals stacks that were recently found to exhibit interfacial polarization, inversion symmetry is broken by having two or more atomic species within the unit cell. Here, we show that even elemental crystals, consisting of one type of atom, and composed of non-polar centrosymmetric layers, exhibit electric polarization if arranged in an appropriate three-dimensional architecture. This concept is demonstrated here for inversion and mirror asymmetric mixed-stacking tetra-layer polytypes of non-polar graphene sheets. Furthermore, we find that the room temperature out-of-plane electric polarization increases with external electrostatic doping, rather than decreases owing to screening. Using first-principles calculations, as well as tight-binding modeling, we unveil the origin of polytype-induced polarization and its dependence on doping. Extension of this idea to graphene multilayers suggests that solely by lateral shifts of constituent monolayers one can obtain multiple meta-stable interlayer stacking sequences that may allow for even larger electrical polarization.

Ferroelectricity in atomically thin bilayer structures has been recently predicted1 and measured[2-4] in two-dimensional (2D) materials with hexagonal non-centrosymmetric unit-cells. Interestingly, the crystal symmetry translates lateral shifts between parallel 2D layers to a change of sign in their out-of-plane electric polarization, a mechanism referred to as "Slide-Tronics"[4]. These observations, however, have been restricted to switching between only two polarization states under low charge carrier densities[5-12], strongly limiting the practical application of the revealed phenomena[13]. To overcome these issues, one needs to explore the nature of the polarization that arises in multi-layered van der Waals (vdW) stacks, how it is governed by intra- and inter-layer charge redistribution, and to which extent it survives the introduction of mobile charge carriers, all of which are presently unknown14. To explore these questions, we conduct surface potential measurements of parallel WSe2 and MoS2 multi-layers with aligned and anti-aligned configurations of the polar interfaces. We find evenly spaced, nearly decoupled potential steps, indicating highly confined interfacial electric fields, which provide means to design multi-state "ladder ferroelectrics". Furthermore, we find that the internal polarization remains significant upon electrostatic doping of a mobile charge carrier density as high as 1013 cm-2, with substantial in-plane conductivity. Using first-principles calculations based on density functional theory (DFT), we trace the extra charge redistribution in real and momentum space and identify an eventual doping-induced depolarization mechanism.