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The device concept of ferroelectric-based negative capacitance (NC) transistors offers a promising route for achieving energy-efficient logic applications that can outperform the conventional semiconductor technology, while viable operation mechanisms remain a central topic of debate. In this work, we report steep slope switching in MoS₂transistors back-gated by single-layer polycrystalline PbZr_0.35Ti_0.65O₃. The devices exhibit current switching ratios up to 8 × 10⁶within an ultra-low gate voltage window of$$V_{{{\mathrm{g}}}} = \pm \! 0.5$$$V_g=\pm 0.5$V and subthreshold swing (SS) as low as 9.7 mV decade⁻¹at room temperature, transcending the 60 mV decade⁻¹Boltzmann limit without involving additional dielectric layers. Theoretical modeling reveals the dominant role of the metastable polar states within domain walls in enabling the NC mode, which is corroborated by the relation between SS and domain wall density. Our findings shed light on a hysteresis-free mechanism for NC operation, providing a simple yet effective material strategy for developing low-power 2D nanoelectronics.

While grain boundaries (GBs) in conventional inorganic semiconductors are frequently considered as detrimental for photogenerated carrier transport, their exact role remains obscure for the emerging hybrid perovskite semiconductors. A primary challenge for GB-property investigations is that experimentally they need to be performed at the top surface, which is not only insensitive to depth-dependent inhomogeneities but also could be susceptible to topographic artifacts. Accordingly, we have developed a unique approach based on tomographic atomic force microscopy, achieving a fully-3D, photogenerated carrier transport map at the nanoscale in hybrid perovskites. This reveals GBs serving as highly interconnected conducting channels for carrier transport. We have further discovered the coexistence of two GB types in hybrid perovskites, one exhibiting enhanced carrier mobilities, while the other is insipid. Our approach reveals otherwise inaccessible buried features and previously unresolved conduction pathways, crucial for optimizing hybrid perovskites for various optoelectronic applications including solar cells and photodetectors.

The dynamics of ferroelectric domain switching are directly mapped in a PbZr_0.2Ti_0.8O₃thin film using piezoresponse force microscopy. Employing the rastering tip as a poling electrode to locally apply a fixed bias near the coercive field, while simultaneously monitoring the evolving domain pattern during continuous imaging, the effectively independent switching dynamics for numerous domains are directly investigated. While areal poling follows the anticipated S‐curve, this is shown to be the collective outcome of linear terminal radial growth for an ensemble of independently nucleating domains. By repeating such spatially resolved measurements in the same region, but with progressively greater fields, nucleation sites and growth patterns are shown to clearly repeat. This reveals apparent defects which comparatively promote switching, and nucleation times and growth rates that accelerate exponentially. After analyzing and mapping the ratio of activation energies for nucleation to growth, a high density of nucleation sites can possibly be activated with higher poling fields—even if only at the start of a poling process—enabling faster and more efficient switching to be engineered as directly demonstrated.

Complex oxide heterointerfaces and van der Waals heterostructures present two versatile but intrinsically different platforms for exploring emergent quantum phenomena and designing new functionalities. The rich opportunity offered by the synergy between these two classes of materials, however, is yet to be charted. Here, we report an unconventional nonlinear optical filtering effect resulting from the interfacial polar alignment between monolayer MoS₂and a neighboring ferroelectric oxide thin film. The second harmonic generation response at the heterointerface is either substantially enhanced or almost entirely quenched by an underlying ferroelectric domain wall depending on its chirality, and can be further tailored by the polar domains. Unlike the extensively studied coupling mechanisms driven by charge, spin, and lattice, the interfacial tailoring effect is solely mediated by the polar symmetry, as well explained via our density functional theory calculations, pointing to a new material strategy for the functional design of nanoscale reconfigurable optical applications.