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The current focus in Autonomous Experimentation (AE) is on developing robust workflows to conduct the AE effectively. This entails the need for well-defined approaches to guide the AE process, including strategies for hyperparameter tuning and high-level human interventions within the workflow loop. This paper presents a comprehensive analysis of the influence of initial experimental conditions and in-loop interventions on the learning dynamics of Deep Kernel Learning (DKL) within the realm of AE in scanning probe microscopy. We explore the concept of the "seed effect," where the initial experiment setup has a substantial impact on the subsequent learning trajectory. Additionally, we introduce an approach of the seed point interventions in AE allowing the operator to influence the exploration process. Using a dataset from Piezoresponse Force Microscopy on PbTiO3 thin films, we illustrate the impact of the "seed effect" and in-loop seed interventions on the effectiveness of DKL in predicting material properties. The study highlights the importance of initial choices and adaptive interventions in optimizing learning rates and enhancing the efficiency of automated material characterization. This work offers valuable insights into designing more robust and effective AE workflows in microscopy with potential applications across various characterization techniques. [ABSTRACT FROM AUTHOR]

An advanced scanning probe microscopy system enhanced with artificial intelligence (AI‐SPM) designed for self‐driving atomic‐scale measurements is presented. This system expertly identifies and manipulates atomic positions with high precision, autonomously performing tasks such as spectroscopic data acquisition and atomic adjustment. An outstanding feature of AI‐SPM is its ability to detect and adapt to surface defects, targeting or avoiding them as necessary. It is also designed to overcome typical challenges such as positional drift and tip apex atomic variations due to the thermal effects, ensuring accurate, site‐specific surface analysis. The tests under the demanding conditions of room temperature have demonstrated the robustness of the system, successfully navigating thermal drift and tip fluctuations. During these tests on the Si(111)‐(7 × 7) surface, AI‐SPM autonomously identified defect‐free regions and performed a large number of current–voltage spectroscopy measurements at different adatom sites, while autonomously compensating for thermal drift and monitoring probe health. These experiments produce extensive data sets that are critical for reliable materials characterization and demonstrate the potential of AI‐SPM to significantly improve data acquisition. The integration of AI into SPM technologies represents a step toward more effective, precise and reliable atomic‐level surface analysis, revolutionizing materials characterization methods. [ABSTRACT FROM AUTHOR]

Epoxyamine matrix-based composites containing 15 wt% of Fe nanoparticles and 1.5 or 2 wt% of carbon nanotubes, as well as composites containing only Fe particles, have been studied using microwave methods and various scanning probe microscopy techniques, such as scanning capacitance microscopy and scanning Kelvin probe force microscopy. The composites were prepared using technological methods that improve their homogeneity. Probe current dependences investigated by applying different voltages to the probe in the Kelvin probe force microscopy mode have shown that the falling regions of the dependences at both positive and negative values of the bias voltage are found only for the sample containing both the Fe particles and the CNT in the "soft epoxy" matrix. Microwave measurements of the transmission and reflection coefficients were performed in the frequency range from 26 to 38 GHz. The field dependences of the microwave power dissipation have been plotted. The ferromagnetic resonance in the composites has been investigated. Frequency dependences of the complex dielectric permittivity of the composites have been determined. Microwave properties of the CNT-containing and CNT-free composites have been compared. [ABSTRACT FROM AUTHOR]

The comparative analysis of the structural, morphological, and local electrical properties of CVD graphene films synthesized at atmospheric and low pressure CVD growth conditions was carried out. The use of electrical techniques of scanning probe microscopy, such as Kelvin probe force microscopy, scanning capacitance microscopy, electrostatic force microscopy, and conductive atomic-force microscopy for investigation of heterogeneous graphene coverage was discussed. A significant change in the surface potential values was observed indicating the formation of p-type multilayered graphene domains on single layer graphene at low pressure and n-type multilayered graphene films at atmospheric pressure CVD. The effect of Ar flow rate increasing during cooling stage in the temperature range of 700–200 °C causing graphite formation was described. The employment of surface potential spectroscopy allows to indicate the presence of nonlinear phenomena in heterogeneous graphene. [ABSTRACT FROM AUTHOR]

The dielectric gap between the scanning probe microscopy (SPM) tip and the surface of a ferroelectric using conductive atomic force microscopy and piezoresponse force microscopy (PFM) is investigated. While the gap functions as a dielectric layer, it also allows tunneling current to inject charges into the ferroelectric when a critical loading force between 10–20 µN is applied to a tip with a radius of 25 nm under a bias voltage of 0.5 V. It is observed that the permittivity of the dielectric gap determines the coercive voltage measured by the piezoresponse hysteresis loop. While such studies done in air often produce coercive voltages much larger than those studied for the same materials in capacitor‐based studies, the use of high permittivity media such as water (ɛr = 79) or silicone oil (ɛr = 2.1‐2.8) produces coercive fields that more closely match those measured in conventional capacitor‐based polarization hysteresis loop measurements. Furthermore, using water as a dielectric medium in PFM imaging enhances the accuracy in extracting the amplitude and phase data from periodically poled lithium niobate crystals. These findings provide insight into the nanoscale phenomena of polarization switching instigated by the SPM tip and provide a pathway to improved quantitative studies. [ABSTRACT FROM AUTHOR]

We introduce a new scanning probe microscopy (SPM) concept called reverse tip sample scanning probe microscopy (RTS SPM), where the tip and sample positions are reversed as compared to traditional SPM. The main benefit of RTS SPM over the standard SPM configuration is that it allows for simple and fast tip changes. This overcomes two major limitations of SPM which are slow data acquisition and a strong dependency of the data on the tip condition. A probe chip with thousands of sharp integrated tips is the basis of our concept. We have developed a nanofabrication protocol for Si based probe chips and their functionalization with metal and diamond coatings, evaluated our probe chips for various RTS SPM applications (multi-tip imaging, SPM tomography, and correlative SPM), and showed the high potential of the RTS SPM concept. [ABSTRACT FROM AUTHOR]

Atomic-scale imaging using scanning probe microscopy is a pivotal method for investigating the morphology and physico-chemical properties of nanostructured surfaces. Time resolution represents a significant limitation of this technique, as typical image acquisition times are on the order of several seconds or even a few minutes, while dynamic processes—such as surface restructuring or particle sintering, to be observed upon external stimuli such as changes in gas atmosphere or electrochemical potential—often occur within timescales shorter than a second. In this article, we present a fully redesigned field programmable gate array (FPGA)-based instrument that can be integrated into most commercially available standard scanning probe microscopes. This instrument not only significantly accelerates the acquisition of atomic-scale images by orders of magnitude but also enables the tracking of moving features such as adatoms, vacancies, or clusters across the surface (“atom tracking”) due to the parallel execution of sophisticated control and acquisition algorithms and the fast exchange of data with an external processor. Each of these measurement modes requires a complex series of operations within the FPGA that are explained in detail.

Abstract In the last decade, contact electrification has gained attention for its potential in energy harvesting, addressing fundamental physics. Scanning probe microscopy (SPM) has evolved as a powerful platform, enabling the in situ characterization/manipulation of a sample's tribological/electrical properties at nanoscale. However, although both the sliding and tapping modes are available in the energy harvesting, the lateral sliding using contact mode SPM has predominantly been employed in triboelectric study. In this work, contact electrification on polydimethylsiloxane is investigated, using peak force tapping atomic force microscopy (PF‐AFM). As PF‐AFM quasi‐discretely offers vertical tapping motions of the probe with a regulated force amplitude, resembling a vertical‐type triboelectric nanogenerator, while minimizing lateral forces. The subsequent surface potential measurements reveal that the generated tribocharge is influenced by both the effective work function difference and energy dissipation at the interface. Furthermore, the accumulation of transferred charges is explored by measuring tip‐sample current during the PF‐AFM operation, showing the comparable results with the surface potential measurement. The results can be attributed to the contact potential difference assisted by the energy dissipation at the interface. This study offers an advanced opportunity to understand and study charge generation behavior based on surface properties without damaging the sample.

We describe an approach to determine the in-plane crystallographic surface directions in scanning probe microscopy (SPM) images. This method is based on a one-time characterization of the SPM instrument with an appropriate test sample and is exemplified by the analysis of non-contact atomic force microscopy (NC-AFM) images on surfaces whose natural cleavage occurs along {111} planes. We introduce a two-dimensional rotation matrix relating the crystallographic surface directions known from an analysis of the macroscopic crystal to the directions in the NC-AFM images. The procedure takes into account rotations and mirror axes resulting from sample mounting, the SPM scanner rotation, the choice of scan direction, as well as data processing, storage, and display. We demonstrate the practicability of the approach by determining the [ 11 2 ̄ ] direction in topographic images of a CeO2(111) film grown on a Si(111) wafer and atomic resolution images of CaF2(111) with an instrument based on the beetle-type scanner. [ABSTRACT FROM AUTHOR]

Carbon black (CB) has wide range of industrial applications, including in the manufacturing of automobile tires, rubber products, inks, and plastics. To improve the properties of the target products and establish recycling systems, it must be fully characterized. However, characterization of CB is challenging owing to its structural complexity and the limitation of conventionally used experimental techniques, especially for surface structures at the nanoscale. In this study, we characterized the surface structures of two commercial CB via atomic force and scanning tunneling microscopy. Analysis of well-dispersed aggregates on atomically flat solid surfaces revealed primary particles of diverse sizes. The particle surfaces lacked edges, grooves, and steps that should be observed between stacked graphene sheets, which contradicts the widely accepted crystallite model. Observed images suggest that the graphene sheets exhibit a size distribution, inferring that multiple non-uniformly sized small graphene sheets are stacked turbostratically, with each sheet displaying a localized curvature rather than the ideal planar form. Varying size of sheets and curvature indicate the presence of a decent number of edges terminated with hydrogen and oxygen-containing functional groups. This interpretation was corroborated by conventional spectroscopic techniques: Raman spectroscopy, X-ray photoelectron spectroscopy, temperature-programmed desorption, and infrared absorption spectroscopy.

Shear-force acoustic near-field microscopy (SANM) is employed to monitor stochastic formation and post dynamic response of a water meniscus that bridges a tapered gold probe (undergoing lateral oscillations of a few nanometers amplitude at constant frequency) and a flat (gold or silicon oxide) substrate. As the probe further approaches the substrate, its amplitude decreases. Shear forces (of yet unknown precise origin) are typically invoked to explain the apparently pure damping effects affecting the probe's motion. Herein, SANM measurements underscore instead the role of near-field acoustic emission from the water meniscus as an elastic energy dissipation channel involved in shear interactions. A simplified thermodynamic argument is provided to justify the formation of a water meniscus between the probe and the sample once they are at sufficient separation distance. The reported measurements focus on the role played by the tip's geometry (by using probes of slender and chubby apex termination). The results shed some light on the potential origin of the so-called shear forces, invoked in many scanning probe microscopy applications, but not yet well understood. [ABSTRACT FROM AUTHOR]

The effect of carbon coating on a surface structure of a high-dose implanted/annealed silicon carbide (SiC) during annealing was examined using scanning probe microscopy (SPM), deep-ultraviolet (DUV) Raman spectroscopy, and transmission electron microscopy (TEM). In SPM, the surfaces of 500- and 30 °C-implanted/annealed SiC samples without coating exhibited a periodic-step structure and granular structure, respectively. The difference between these surfaces is attributed to the absence or presence of residual implantation damage. In contrast, surface flatness was maintained in the 500 °C-implanted/annealed SiC sample with carbon coating. However, the surface of the coated 30 °C-implanted/annealed SiC sample exhibited a geometric structure with a lattice pattern parallel to the ⟨ 11 2 ¯ 0 ⟩ axes. The DUV Raman spectra and TEM images indicated that the implanted layer of this sample metamorphosed into a mixture of 3C-SiC twin domains and amorphous-SiC regions. During the cooling process after annealing, the 3C-SiC region was more raised than the amorphous-SiC region owing to the difference in the thermal expansion coefficients, thus resulting in the generation of a geometric surface structure. In the metamorphosed implanted layer, the carbon coating does not completely prevent surface roughening. [ABSTRACT FROM AUTHOR]

Material-by-design has been a long-standing aspiration that has recently become a reality. Such designer materials have been repeatedly demonstrated using the top-down approach of mechanical exfoliation and stacking, leading to a variety of artificial 2D heterostructures with new properties that are otherwise unattainable. Consequently, tremendous research frontiers in physics, chemistry, engineering, and life science have been created. While thousands of layered crystals exist in nature, only a few dozen of them with manageable chemical-stability have been made into heterostructures using this method. Moreover, experimental investigations of materials that have received limited exploration in the 2D realm, such as cuprates, halides, and perovskites, along with their heterostructures, have been fundamentally hindered by their rapid chemical degradation. Another critical challenge imposed by exfoliating and stacking 2D layers in ambient environment is the absorption of itinerant gas molecules that further contaminate sensitive 2D interfaces in the heterostructures. Such contamination and compromised material properties significantly hinder surface-sensitive local probes—scanning probe microscopy (SPM)—that often require nanometer to atomic scale surface cleanliness. In this article, we aim to provide a technical review of recent development toward 2D materials and heterostructure fabrication in more controlled environments that are suitable for SPM characterizations. These include the development of more efficient mechanical exfoliation and dry-transfer techniques, as well as the incorporation of 2D material exfoliation and transfer in inert gas, low vacuum, and, eventually, ultra-high vacuum environments. Finally, we provide an outlook on the remaining challenges and opportunities in ultra-clean 2D material fabrication techniques.

Focused ion beam (FIB) has become a powerful tool for transmission electron microscopy sample preparation in the nanoelectronics industry and has in recent years also shown its benefits for specific preparation steps in electrical scanning probe microscopy (SPM). Most recently, a novel SPM approach – so-called reverse tip sample (RTS) SPM – has been proposed in which the position of sample and tip are switched compared to standard SPM; in RTS SPM the sample is attached to the end of a cantilever beam. To achieve this configuration, the region of interest must first be extracted from a substrate and then needs to be reliably fixed to the cantilever by FIB. Therefore, we have explored and developed dedicated FIB preparation methods for RTS SPM in this work. Our established procedures ensure a strong mechanical and good electrical connection of the sample to the cantilever for both cross-section and top view sample preparation. Furthermore, we introduce an approach for mounting samples from a full wafer size workflow. This paper presents the developed FIB procedures and discusses the quality and stability of all mounted samples and their electrical evaluation in RTS SPM.

Atomic-scale imaging using scanning probe microscopy is a pivotal method for investigating the morphology and physico-chemical properties of nanostructured surfaces. Time resolution represents a significant limitation of this technique, as typical image acquisition times are on the order of several seconds or even a few minutes, while dynamic processes-such as surface restructuring or particle sintering, to be observed upon external stimuli such as changes in gas atmosphere or electrochemical potential-often occur within timescales shorter than a second. In this article, we present a fully redesigned field programmable gate array (FPGA)-based instrument that can be integrated into most commercially available standard scanning probe microscopes. This instrument not only significantly accelerates the acquisition of atomic-scale images by orders of magnitude but also enables the tracking of moving features such as adatoms, vacancies, or clusters across the surface ("atom tracking") due to the parallel execution of sophisticated control and acquisition algorithms and the fast exchange of data with an external processor. Each of these measurement modes requires a complex series of operations within the FPGA that are explained in detail.

Scanning probe microscopy (SPM) has enabled significant new insights into the nanoscale and microscale properties of solar cell materials and underlying working principles of photovoltaic and optoelectronic technology. Various SPM modes, including atomic force microscopy, Kelvin probe force microscopy, conductive atomic force microscopy, piezoresponse force microscopy, and scanning near-field optical microscopy, can be used for the investigation of electrical, optical and chemical properties of associated functional materials. A large body of work has improved the understanding of solar cell device processing and synthesis in close synergy with SPM investigations in recent years. This review provides an overview of SPM measurement capabilities and attainable insight with a focus on recently widely investigated halide perovskite materials., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Abstract Controlling nanoscale tip‐induced material removal is crucial for achieving atomic‐level precision in tomographic sensing with atomic force microscopy (AFM). While advances have enabled volumetric probing of conductive features with nanometer accuracy in solid‐state devices, materials, and photovoltaics, limitations in spatial resolution and volumetric sensitivity persist. This work identifies and addresses in‐plane and vertical tip‐sample junction leakage as sources of parasitic contrast in tomographic AFM, hindering real‐space 3D reconstructions. Novel strategies are proposed to overcome these limitations. First, the contrast mechanisms analyzing nanosized conductive features are explored when confining current collection purely to in‐plane transport, thus allowing reconstruction with a reduction in the overestimation of the lateral dimensions. Furthermore, an adaptive tip‐sample biasing scheme is demonstrated for the mitigation of a class of artefacts induced by the high electric field inside the thin oxide when volumetrically reduced. This significantly enhances vertical sensitivity by approaching the intrinsic limits set by quantum tunneling processes, allowing detailed depth analysis in thin dielectrics. The effectiveness of these methods is showcased in tomographic reconstructions of conductive filaments in valence change memory, highlighting the potential for application in nanoelectronics devices and bulk materials and unlocking new limits for tomographic AFM.

The impact of Artificial Intelligence (AI) is rapidly expanding, revolutionizing both science and society. It is applied to practically all areas of life, science, and technology, including materials science, which continuously requires novel tools for effective materials characterization. One of the widely used techniques is scanning probe microscopy (SPM). SPM has fundamentally changed materials engineering, biology, and chemistry by providing tools for atomic-precision surface mapping. Despite its many advantages, it also has some drawbacks, such as long scanning times or the possibility of damaging soft-surface materials. In this paper, we focus on the potential for supporting SPM-based measurements, with an emphasis on the application of AI-based algorithms, especially Machine Learning-based algorithms, as well as quantum computing (QC). It has been found that AI can be helpful in automating experimental processes in routine operations, algorithmically searching for optimal sample regions, and elucidating structure-property relationships. Thus, it contributes to increasing the efficiency and accuracy of optical nanoscopy scanning probes. Moreover, the combination of AI-based algorithms and QC may have enormous potential to enhance the practical application of SPM. The limitations of the AI-QC-based approach were also discussed. Finally, we outline a research path for improving AI-QC-powered SPM. RESEARCH HIGHLIGHTS: Artificial intelligence and quantum computing as support for scanning probe microscopy. The analysis indicates a research gap in the field of scanning probe microscopy. The research aims to shed light into ai-qc-powered scanning probe microscopy., (© 2024 Wiley Periodicals LLC.)

The functionalities of materials are governed by the atom type and arrangement, and perturbations caused by defects and adsorbate interactions often significantly alter the behavior of materials. Scanning probe microscopy (SPM) can capture complex interactions caused by the structures on surfaces. It is, however, difficult to analyze such interactions appearing there. In this paper, an image-processing technique that employs template matching to recognize local structures in SPM images and calculate positional correlations is reported. This approach opens new avenues for investigating intricate perturbations in the sciences and provides detailed insights into materials science.

Understanding how carbon dioxide (CO 2 ) behaves and interacts with surfaces is paramount for the development of sensors and materials to attempt CO 2 mitigation and catalysis. Here, we combine simultaneous atomic force microscopy (AFM) and scanning tunneling microscopy (STM) using CO-functionalized probes with density functional theory (DFT)-based simulations to gain fundamental insight into the behavior of physisorbed CO 2 molecules on a gold(111) surface that also contains one-dimensional metal-organic chains formed by 1,4-phenylene diisocyanide (PDI) bridged by gold (Au) adatoms. We resolve the structure of self-assembled CO 2 islands, both confined between the PDI-Au chains as well as free-standing on the surface and reveal a chiral arrangement of CO 2 molecules in a windmill-like structure that encloses a standing-up CO 2 molecule and other foreign species existing at the surface. We identify these species by the comparison of height-dependent AFM and STM imaging with DFT-calculated images and clarify the origin of the kagome tiling exhibited by this surface system. Our results show the complementarity of AFM and STM using functionalized probes and their potential, when combined with DFT, to explore greenhouse gas molecules at surface-supported model systems.

Scanning probe microscopy (SPM) and advanced atomic force microscopy (AFM ++ ) have become pivotal for nanoscale elucidation of the structural, optoelectronic and photovoltaic properties of halide perovskite single crystals and polycrystalline films, both under ex situ and in situ conditions. These techniques reveal detailed information about film topography, compositional mapping, charge distribution, near-field electrical behaviors, cation-lattice interactions, ion dynamics, piezoelectric characteristics, mechanical durability, thermal conductivity, and magnetic properties of doped perovskite lattices. This article outlines the advancements in SPM techniques that deepen our understanding of the optoelectronic and photovoltaic performances of halide perovskites.

Photoconductive atomic force microscopy can probe monolayers of PbS/perovskite quantum dots (QDs) with a contact area of 1-3 QDs in stable and reproducible acquisition conditions for I / V curves and photocurrent maps. From the measurements, quantitative values for the barrier height, built-in voltage, diffusion constant and ideality factor are deduced with high precision. The data analysis is based on modelling a superposition of the drift current of the photo-excited charges and a diffusion current across the interface barriers, providing physical insight into the underlying processes. Besides looking into PbS/perovskite on an indium tin oxide substrate, it is shown how the photocurrent is modified by changing either the QD ligand (to thiocyanate) or the substrate (to micro- and nanostructured gold). The dependence of the photocurrent on the light irradiance is found to follow a power law with an exponent of 0.64. Generally, quantitative measurements with high spatial resolution (on the single QD level) can provide significant insight into the processes in nanostructured hybrid optoelectronic components.

Scanning probe microscopy (SPM), in particular at low temperature (LT) under ultra-high vacuum (UHV) conditions, offers the possibility of real-space imaging with resolution reaching the atomic level. However, its potential for the analysis of complex biological molecules has been hampered by requirements imposed by sample preparation. Transferring molecules onto surfaces in UHV is typically accomplished by thermal sublimation in vacuum. This approach however is limited by the thermal stability of the molecules, i. e. not possible for biological molecules with low vapour pressure. Bypassing this limitation, electrospray ionisation offers an alternative method to transfer molecules from solution to the gas-phase as intact molecular ions. In soft-landing electrospray ion beam deposition (ESIBD), these molecular ions are subsequently mass-selected and gently landed on surfaces which permits large and thermally fragile molecules to be analyzed by LT-UHV SPM. In this concept, we discuss how ESIBD+SPM prepares samples of complex biological molecules at a surface, offering controls of the molecular structural integrity, three-dimensional shape, and purity. These achievements unlock the analytical potential of SPM which is showcased by imaging proteins, peptides, DNA, glycans, and conjugates of these molecules, revealing details of their connectivity, conformation, and interaction that could not be accessed by any other technique., (© 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH.)

Material-by-design has been a long-standing aspiration that has recently become a reality. Such designer materials have been repeatedly demonstrated using the top-down approach of mechanical exfoliation and stacking, leading to a variety of artificial 2D heterostructures with new properties that are otherwise unattainable. Consequently, tremendous research frontiers in physics, chemistry, engineering, and life science have been created. While thousands of layered crystals exist in nature, only a few dozen of them with manageable chemical-stability have been made into heterostructures using this method. Moreover, experimental investigations of materials that have received limited exploration in the 2D realm, such as cuprates, halides, and perovskites, along with their heterostructures, have been fundamentally hindered by their rapid chemical degradation. Another critical challenge imposed by exfoliating and stacking 2D layers in ambient environment is the absorption of itinerant gas molecules that further contaminate sensitive 2D interfaces in the heterostructures. Such contamination and compromised material properties significantly hinder surface-sensitive local probes—scanning probe microscopy (SPM)—that often require nanometer to atomic scale surface cleanliness. In this article, we aim to provide a technical review of recent development toward 2D materials and heterostructure fabrication in more controlled environments that are suitable for SPM characterizations. These include the development of more efficient mechanical exfoliation and dry-transfer techniques, as well as the incorporation of 2D material exfoliation and transfer in inert gas, low vacuum, and, eventually, ultra-high vacuum environments. Finally, we provide an outlook on the remaining challenges and opportunities in ultra-clean 2D material fabrication techniques. [ABSTRACT FROM AUTHOR]

Single molecules, the smallest independently stable units in the material world, serve as the fundamental building blocks of matter. Among different branches of single-molecule sciences, single-molecule chemical reactions, by revealing the behavior and properties of individual molecules at the molecular scale, are particularly attractive because they can advance the understanding of chemical reaction mechanisms and help to address key scientific problems in broad fields such as physics, chemistry, biology and materials science. This review provides a timely, comprehensive overview of single-molecule chemical reactions based on various technical platforms such as scanning probe microscopy, single-molecule junction, single-molecule nanostructure, single-molecule fluorescence detection and crossed molecular beam. We present multidimensional analyses of single-molecule chemical reactions, offering new perspectives for research in different areas, such as photocatalysis/electrocatalysis, organic reactions, surface reactions and biological reactions. Finally, we discuss the opportunities and challenges in this thriving field of single-molecule chemical reactions. [ABSTRACT FROM AUTHOR]

Controlling nanoscale tip‐induced material removal is crucial for achieving atomic‐level precision in tomographic sensing with atomic force microscopy (AFM). While advances have enabled volumetric probing of conductive features with nanometer accuracy in solid‐state devices, materials, and photovoltaics, limitations in spatial resolution and volumetric sensitivity persist. This work identifies and addresses in‐plane and vertical tip‐sample junction leakage as sources of parasitic contrast in tomographic AFM, hindering real‐space 3D reconstructions. Novel strategies are proposed to overcome these limitations. First, the contrast mechanisms analyzing nanosized conductive features are explored when confining current collection purely to in‐plane transport, thus allowing reconstruction with a reduction in the overestimation of the lateral dimensions. Furthermore, an adaptive tip‐sample biasing scheme is demonstrated for the mitigation of a class of artefacts induced by the high electric field inside the thin oxide when volumetrically reduced. This significantly enhances vertical sensitivity by approaching the intrinsic limits set by quantum tunneling processes, allowing detailed depth analysis in thin dielectrics. The effectiveness of these methods is showcased in tomographic reconstructions of conductive filaments in valence change memory, highlighting the potential for application in nanoelectronics devices and bulk materials and unlocking new limits for tomographic AFM. [ABSTRACT FROM AUTHOR]

Enantiospecific effects play an uprising role in chemistry and technical applications. Chiral molecular networks formed by self‐assembly processes at surfaces can be imaged by scanning probe microscopy (SPM). Low contrast and high noise in the topography map often interfere with the automatic image analysis using classical methods. The long SPM image acquisition times restrain Artificial Intelligence‐based methods requiring large training sets, leaving only tedious manual work, inducing human‐dependent errors and biased labeling. By generating realistic looking synthetic images, the acquisition of real datasets is avoided. Two state‐of‐the‐art object detection architectures are trained to localize and classify chiral unit‐cells in a regular molecular chiral network formed by self‐assembly of linear molecular bricks. The comparison of different architectures and datasets demonstrates that the training on purely synthetic data outperforms models trained using augmented datasets. A Faster R‐CNN model trained solely on synthetic data achieved an excellent mean average precision of 99% on real data. Hence this approach and the transfer to real data show high success, also highlighting the high robustness against experimental noise and different zoom levels across the full experimentally reasonable parameter range. The generalizability of this idea is demonstrated by achieving equally high performance on a different structure, too. [ABSTRACT FROM AUTHOR]

This study compares different types of scanning probe microscopy (SPM) probes according to the function of the surface layer at the tip apex. Three main types of SPM probes were analyzed: scanning tunneling microscopy (STM) tungsten probes, conductive atomic force microscopy (AFM) probes, and non-conductive AFM probes. The tungsten STM probes were coated with a graphite layer to simulate the effects of carbonization. The tested AFM probes were specifically NenoProbe conductive AFM probes (platinum-coated tip) and Akiyama non-conductive AFM probes coated with gold. The gold coating is intended to improve surface conductivity and help achieve a homogeneous, oxidation-resistant surface. The three samples were measured in a field emission microscope to study their current-voltage characteristics. The obtained current-voltage characteristics were tested and analyzed by the Forbes field emission orthodoxy test, providing the field emission parameters that correlate with the state of the scanning probe tip. In this study, the most important parameter is the formal emission area parameter, which indicates the formal tunneling current density through the probe tip-sample nanogap. For an STM tip, this reflects the size and shape of the region from which electrons tunnel to the sample surface. If this area is larger than expected or desired, it may indicate problems with tip function or tip wear. This information is critical for evaluating the performance and accuracy of the STM tip and can help diagnose problems and optimize its function. [ABSTRACT FROM AUTHOR]