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Kelvin probe microscopy (KPFM) is a well-established scanning probe technique, used to measure surface potential accurately; it has found extensive use in the study of a range of materials phenomena. In its conventional form, KPFM frustratingly precludes imaging samples or scenarios where large surface potential exists or large surface potential gradients are created outside the typical +/-10V window. If the potential regime measurable via KPFM could be expanded, to enable precise and reliable metrology, through a high voltage KPFM (HV-KPFM) adaptation, it could open up pathways towards a range of novel experiments, where the detection limit of regular KPFM has so far prevented the use of the technique. In this work, HV-KPFM has been realised and shown to be capable of measuring large surface potential and potential gradients with accuracy and precision. The technique has been employed to study a range of materials (positive temperature coefficient of resistivity ceramics, charge storage fluoropolymers and pyroelectrics) where accurate spatially resolved mapping of surface potential within high voltage regime facilitates novel physical insight. The results demonstrate that HV-KPFM can be used as an effective tool to fill in existing gaps in surface potential measurements while also opening routes for novel studies in materials physics., Comment: Main Text: 16 pages, 5 figures Supplementary information:4 pages, 2 tables and 2 figures

Ferroelectric domain wall (DW) conductivity (DWC) can be attributed to two separate mechanisms: (a) the injection/ejection of charge carriers across the Schottky barrier formed at the (metal-) electrode-DW junction and (b) the transport of those charge carriers along the DW. Current-voltage (IU) characteristics, recorded at variable temperatures from LiNbO$_3$ (LNO) DWs, are clearly able to differentiate between these two contributions. Practically, they allow us here to directly quantify the physical parameters relevant for the two mechanisms (a) and (b) mentioned above. These are, e.g., the resistance of the DW, the saturation current, the ideality factor, and the Schottky barrier height of the electrode/DW junction. Furthermore, the activation energies needed to initiate the thermally-activated electronic transport along the DWs, can be extracted. In addition, we show that electronic transport along LiNbO$_3$ DWs can be elegantly viewed and interpreted in an adapted semiconductor picture based on a double-diode/double-resistor equivalent circuit model, the R2D2 model. Finally, our R2D2 model was checked for its universality by fitting the DWC data not only to z-cut LNO bulk DWs, but equally to z-cut thin-film LNO DWs, and DWC from x-cut DWs as reported in literature., Comment: 10 pages, 7 figures; with included supporting information (6 pages, 4 figures)

Fundamentally, lithium niobate is an extremely good electrical insulator. However, this can change dramatically when 180{\deg} domain walls are present, as they are often found to be strongly conducting. Absolute conductivities depend on the inclination angles of the walls with respect to the [001] polarisation axis and so, if these inclination angles can be altered, then electrical conductivities can be tuned, or even toggled on and off. In 500nm thick z-cut ion-sliced thin films, localised wall angle variations can be controlled by both the sense and magnitude of applied electrical bias. We show that this results in a diode-like charge transport response which is effective for half-wave rectification, albeit only at relatively low ac frequencies. Most importantly, however, we also demonstrate that such domain wall diodes can be used to construct "AND" and inclusive "OR" logic gates, where "0" and "1" output states are clearly distinguishable. Realistic device modelling allows an extrapolation of results for the operation of these domain wall diodes in more complex arrangements and, although non-ideal, output states can still be distinguished even in two-level cascade logic. Although conceptually simple, we believe that our experimental demonstration of operational domain wall-enabled logic gates represents a significant step towards the future broader realisation of "domain wall nanoelectronics".

Recently, electrically conducting heterointerfaces between dissimilar band-insulators (such as lanthanum aluminate and strontium titanate) have attracted considerable research interest. Charge transport has been thoroughly explored and fundamental aspects of conduction firmly established. Perhaps surprisingly, similar insights into conceptually much simpler conducting homointerfaces, such as the domain walls that separate regions of different orientations of electrical polarisation within the same ferroelectric band-insulator, are not nearly so well-developed. Addressing this disparity, we herein report magnetoresistance in approximately conical 180o charged domain walls, which occur in partially switched ferroelectric thin film single crystal lithium niobate. This system is ideal for such measurements: firstly, the conductivity difference between domains and domain walls is extremely and unusually large (a factor of at least 1013) and hence currents driven through the thin film, between planar top and bottom electrodes, are overwhelmingly channelled along the walls; secondly, when electrical contact is made to the top and bottom of the domain walls and a magnetic field is applied along their cone axes (perpendicular to the thin film surface), then the test geometry mirrors that of a Corbino disc, which is a textbook arrangement for geometric magnetoresistance measurement. Our data imply carriers at the domain walls with extremely high room temperature Hall mobilities of up to ~ 3,700cm2V-1s-1. This is an unparalleled value for oxide interfaces (and for bulk oxides too) and is most comparable to mobilities in other systems typically seen at cryogenic, rather than at room, temperature., Comment: 22 pages main text, 24 pages supplementary information. Published in advanced materials, DOI:https://doi.org/10.1002/adma.202204298

In 2014, Charge Gradient Microscopy (CGM) was first reported as a new scanning probe imaging mode, particularly well-suited for the characterisation of ferroelectrics. The implementation of the technique is straightforward; it involves monitoring currents that spontaneously develop between a passive conducting atomic force microscopy tip and Earth, as the tip is scanned across the specimen surface. However, details on the fundamental origin of contrast and what images mean, in terms of associated ferroelectric microstructures, are not yet fully understood. Here, by comparing information from CGM and Kelvin Probe Force Microscopy (KPFM), obtained from the same sets of ferroelectric domains (in both lithium niobate and barium titanate), we show that CGM reasonably reflects the spatial derivative of the measured surface potential. This is conceptually different from measuring local gradients in the surface bound-charge density or in any associated screening charges: after all, we see clear CGM signals, even when polarisation is entirely in-plane. We therefore suggest that CGM in ferroelectrics might be more accurately called Potential Gradient Microscopy (PGM). Intriguingly, in all cases examined, the measured surface potential (determined both through KPFM and by integrating the CGM signal) is of the opposite sign to that intuitively expected for a completely clean ferroelectric in vacuum. This is commonly observed and presumed due to a charge accumulation on the ferroelectric surface which is not easily removed.