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The study employs a multimicroscopy approach, combining Scanning Electrochemical Cell Microscopy (SECCM) and Field Emission Scanning Electron Microscopy (FESEM), to investigate electrochemical nucleation and growth (EN&G). Cu nanoparticles (NPs) are meticulously electrodeposited on glassy carbon (GC), to perform co‐located characterization, supported by analytical modeling and statistical analysis. The findings reveal clear correlations between electrochemical descriptors (i–t transients) and physical descriptors (NPs size and distribution), offering valuable insights into nucleation kinetics, influenced by varied overpotentials, surface state, and electrode's area. Analysis of the stochasticity of nucleation reveals intriguing temporal distributions, indicating an increased likelihood of nucleation with higher overpotential and larger electrode's area. Notably, the local surface state significantly influences nucleation site number and activity, leading to spatial differences in nucleation rates unaccounted for in macroscopic experiments. The updated analytical model for EN&G current transients, considering SECCM geometry, shows excellent agreement with FESEM measurements, facilitating the calculation of active sites within individual regions. These results deepen the understanding of EN&G phenomena from a new perspective, and lay the groundwork for further theoretical advancements, showcasing the great potential of current experimental methods in advancing precise electrochemical manufacturing of micro‐ and nanostructures. [ABSTRACT FROM AUTHOR]

Thermally‐induced dehydrogenative coupling of polyphenylenes on metal surfaces is an important technique to synthesize π ${\pi }$ ‐conjugated carbon nanostructures with atomic precision. However, this protocol has rarely been utilized to fabricate structurally defined carbon nanosheets composed of sp‐ and sp2‐hybridized carbon atoms. Here, we present the synthesis of butadiyne‐linked hexabenzocoronenes (HBCs) on Au(111) surfaces as core‐expanded graphdiynes. The reaction started from hexa(4‐ethylphenyl)benzene, which undergoes dehydrogenation toward hexa(4‐vinylphenyl)benzene, followed by planarization to hexabenzocoronene, coupling between the vinyl groups, and further dehydrogenation. In addition to butadiyne linkages, benzene groups were also found as another type of linker. The reaction sequences were monitored by scanning tunneling microscopy and bond‐resolved non‐contact atomic force microscopy, which disclose the structures of intermediates and final products. In combination with density functional theory simulations, the key steps from ethyl substituents to butadiyne and benzene linkers were elucidated. This is a new on‐surface synthesis of core‐expanded graphdiynes with unprecedented electronic properties. [ABSTRACT FROM AUTHOR]

2D materials are intriguing due to their remarkably thin and flat structure. This unique configuration allows the majority of their constituent atoms to be accessible on the surface, facilitating easier electron tunneling while generating weak surface forces. To decipher the subtle signals inherent in these materials, the application of techniques that offer atomic resolution (horizontal) and sub‐Angstrom (z‐height vertical) sensitivity is crucial. Scanning probe microscopy (SPM) emerges as the quintessential tool in this regard, owing to its atomic‐level spatial precision, ability to detect unitary charges, responsiveness to pico‐newton‐scale forces, and capability to discern pico‐ampere currents. Furthermore, the versatility of SPM to operate under varying environmental conditions, such as different temperatures and in the presence of various gases or liquids, opens up the possibility of studying the stability and reactivity of 2D materials in situ. The characteristic flatness, surface accessibility, ultra‐thinness, and weak signal strengths of 2D materials align perfectly with the capabilities of SPM technologies, enabling researchers to uncover the nuanced behaviors and properties of these advanced materials at the nanoscale and even the atomic scale. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Understanding the structure and function of bioelectric materials is challenging due to the complex nature of biomaterials and a lack of appropriate tools. The precisely defined structures and genetic tunability of viruses provide an excellent model system to investigate bioelectrical behavior in biomaterials. This study presents the molecular mechanisms of piezoelectricity in the M13 bacteriophage (phage) under various mechanical stresses for bio‐piezoelectric generation. A computational approach is used to calculate the piezoelectric tensors of the M13 phage and quantify its direction‐dependent dipole moments. By computationally designing negatively charged residues on the phage surface, the surface charge density is enhanced to 16.7 µC cm−2. Using genetic engineering, phages are experimentally designed with different charges and tail structures to create model phage nanostructures, including individual phages, vertically standing phage films, and horizontally aligned phage films. Their vertical, horizontal, and shear‐mode piezoelectric properties are then measured using scanning probe microscopy techniques. The resulting phage‐based piezoelectric energy generators exhibit an effective piezoelectric coefficient of 15.4 pm V−1 and a power density of 4.2 µW cm−2. This phage‐based bioengineering approach provides a versatile platform for investigating fundamental mechanisms of bioelectricity and designing bioelectric materials for applications in energy harvesting, biomemory, and biosensors. [ABSTRACT FROM AUTHOR]

Passive films are essential for the longevity of metals and alloys in corrosive environments. A great deal of research has been devoted to understanding and characterizing passive films, including their chemical composition, uniformity, thickness, porosity, and conductivity. Many characterization techniques are conducted under vacuum, which do not portray the true in‐service environments passive films will endure. Scanning electrochemical probe microscopy (SEPM) techniques have emerged as necessary tools to complement research on characterizing passive films to enable the in situ extraction of passive film parameters and monitoring of local breakdown events of compromised films. Herein, we review the current research efforts using scanning electrochemical microscopy, scanning electrochemical cell microscopy (or droplet cell measurements), and local electrochemical impedance spectroscopy techniques to advance the knowledge of local properties of passivated metals. The future use of SEPM for quantitative extraction of local film characteristics within in‐service environments (i.e., with varying pH, solution composition, and applied potential) is promising, which can be correlated to nanostructural and microstructural features of the passive film and underlying metal using complementary microscopy and spectroscopy methods. The outlook on this topic is highlighted, including exciting avenues and challenges of these methods in characterizing advanced alloy systems and protective surface films. [ABSTRACT FROM AUTHOR]

Microscopy has been pivotal in improving the understanding of structure‐function relationships at the nanoscale and is by now ubiquitous in most characterization labs. However, traditional microscopy operations are still limited largely by a human‐centric click‐and‐go paradigm utilizing vendor‐provided software, which limits the scope, utility, efficiency, effectiveness, and at times reproducibility of microscopy experiments. Here, a coupled software–hardware platform is developed that consists of a software package termed AEcroscopy (short for Automated Experiments in Microscopy), along with a field‐programmable‐gate‐array device with LabView‐built customized acquisition scripts, which overcome these limitations and provide the necessary abstractions toward full automation of microscopy platforms. The platform works across multiple vendor devices on scanning probe microscopes and electron microscopes. It enables customized scan trajectories, processing functions that can be triggered locally or remotely on processing servers, user‐defined excitation waveforms, standardization of data models, and completely seamless operation through simple Python commands to enable a plethora of microscopy experiments to be performed in a reproducible, automated manner. This platform can be readily coupled with existing machine‐learning libraries and simulations, to provide automated decision‐making and active theory‐experiment optimization to turn microscopes from characterization tools to instruments capable of autonomous model refinement and physics discovery. [ABSTRACT FROM AUTHOR]

Recently, in electric mobilities and stationary energy storage device applications, the development of long‐lasting, low‐cost, and high‐safety lithium‐ion batteries (LIBs) is widely studied. LiFePO4 (LFP) is a core cathode material for LIBs owing to its cost‐effectiveness and high safety. However, it exhibits low electronic conductivity and sluggish Li+ diffusion, hindering the application of LFP cathodes in high‐power battery industries. Herein, a triazole‐motivated electrolyte additive, 1‐(trimethylsilyl)−1H‐benzotriazole (TMSBTA) is presented, for mitigating iron dissolution via HF scavenging, reinforcing the robustness of the solid electrolyte interphase and constructing a cathode–electrolyte interface (CEI) to balance the ion and electron conduction of the CEI on the LFP cathode. Scanning probe microscopy performed in the conductive atomic force microscopy mode indicates that the electronically conductive CEI created by the oxidative decomposition of TMSBTA enables rapid and homogeneous lithiation and delithiation during cycling without morphological changes in the LFP particles. This study elucidates the design principles of the CEI on the LFP cathode and is expected to guide integrated electrolyte additive engineering for LFP‐containing LIBs. [ABSTRACT FROM AUTHOR]

In the pursuit of high‐spin building blocks for the formation of covalently bonded 1D or 2D materials with controlled magnetic interactions, π ${\pi }$ ‐electron magnetism offers an ideal framework to engineer ferromagnetic interactions between nanographenes. As a first step in this direction, we explore the spin properties of ferromagnetically coupled triangulenes—triangular nanographenes with spin S=1 ${S = 1}$ . By combining in‐solution synthesis of rationally designed molecular precursors with on‐surface synthesis, we successfully achieve covalently bonded S=2 ${S = 2}$ triangulene dimers and S=3 ${S = 3}$ trimers on Au(111). Starting with the triangulene dimer, we meticulously characterize its low‐energy magnetic excitations using inelastic electron tunneling spectroscopy (IETS). IETS reveals conductance steps corresponding to a quintet‐to‐triplet excitation, and a zero‐bias peak resulting from higher‐order spin‐spin scattering of the five‐fold degenerate ferromagnetic ground state. The Heisenberg model captures the key parameters of inter‐triangulene ferromagnetic exchange, and its successful extension to the larger S=3 ${S = 3}$ system validates the model's accuracy. We anticipate that incorporating ferromagnetically coupled building blocks into the repertoire of magnetic nanographenes will unlock new possibilities for designing carbon nanomaterials with complex magnetic ground states. [ABSTRACT FROM AUTHOR]

The emergence of π‐magnetism in low‐dimensional carbon‐based nanostructures, such as nanographenes (NGs), has captured significant attention due to their unique properties and potential applications in spintronics and quantum technologies. Recent advancements in on‐surface synthesis under ultra‐high vacuum conditions have enabled the atomically precise engineering of these nanostructures, effectively overcoming the challenges posed by their inherent strong chemical reactivity. This review highlights the essential concepts and synthesis methods used in studying NGs. It also outlines the remarkable progress made in understanding and controlling their magnetic properties. Advanced characterization techniques, such as scanning tunneling microscopy (STM) and non‐contact atomic force microscopy (nc‐AFM), have been instrumental in visualizing and manipulating these nanostructures, which highlighting their critical role in the field. The review underscores the versatility of carbon‐based π‐magnetic materials and their potential for integration into next‐generation electronic devices. It also outlines future research directions aimed at optimizing their synthesis and exploring applications in cutting‐edge technologies. [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]

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]

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]

In scanning electrochemical microscopy (SECM), the addition of a redox active species plays an essential role. Those deliberately added mediators may alter results in SECM studies. In investigations of lithium‐ion battery (LIB) materials, especially of the positive electrode, the oxidation potentials of commonly used mediator substances such as ferrocene are located within the operation potential of the electrode. Thus, they possibly interfere with the regular charge/discharge processes. In situ studies are therefore in need of approaches reducing or eliminating the use of mediators. Within this publication, a novel mediator dosing (MD) concept is introduced. A capillary was closely positioned at the tip of the scanning probe. By gravity flow, stable flow rates of mediator solution of up to 32.4±0.6 μL h−1 were achieved. These low amounts were found to be sufficient to form a ferrocene zone at the probe tip enabling feedback mode SECM measurements with comparable quality to measurements directly in ferrocene solution. Proof of concept experiments were conducted by investigation of a thin‐film electrode with a micro‐structured surface. Furthermore, the MD concept was applied in imaging experiments of a commercially available LIB graphite electrode. [ABSTRACT FROM AUTHOR]

Spin‐crossover compounds can be switched between two stable states with different magnetic moments, conformations, electronic, and optical properties, which opens appealing perspectives for technological applications including miniaturization down to the scale of single molecules. Although control of the spin states is crucial their direct identification is challenging in single‐molecule experiments. Here we investigate the spin‐crossover complex [Fe(HB(1,2,4‐triazol‐1‐yl)3)2] on a Cu(111) surface with scanning tunneling microscopy and density functional theory calculations. Spin crossover of single molecules in dense islands is achieved via electron injection. Spin‐flip excitations are resolved in scanning tunneling spectra in a magnetic field enabling the direct identification of the molecular spin state, and revealing the existence of magnetic anisotropy in the HS molecules. [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]

Organic–inorganic 2D heterostructures combine the high optical absorption of organic molecules with exciton‐dominated optical properties in layered transition metal dichalcogenides (TMDs) such as MoS2. Critical to the interaction and the optical response in such hybrid systems is the electronic band alignment at the interface between the two species. Here, the coupling of monolayers of perylene derivatives is investigated with bilayer MoS2. In particular, variation in the perylene orientation on the MoS2 surface is identified using Raman spectroscopy and scanning probe microscopy. Low‐temperature optical spectroscopy reveals orientation‐dependent interlayer exciton formation. Furthermore, power‐dependent photoluminescence measurements provide insight into the modified interlayer charge transfer in these heterostructures. A saturation of interlayer states is found under high excitation power when the perylene molecules are in a perpendicular orientation to the surface that leads to electron accumulation in the MoS2, whereas parallel alignment of the perylene molecules leads to enhanced populations of organic–inorganic interlayer excitons. This work provides insights into the optimization of organic–inorganic heterostructures, with particular relevance to applications for optoelectronic and excitonic devices. [ABSTRACT FROM AUTHOR]

An unusual self‐assembly pattern is observed for highly ordered 1500‐nm‐thick films of monodisperse 13‐nm‐sized colloidal PbSe quantum dots, originating from their faceted truncated cube‐like shape. Specifically, self‐assembled PbSe dots exhibited attachment to the substrate by <001> planes followed by an interconnection through the {001} facets in plan‐view and {110}/{111} facets in cross‐sectional‐view, thus forming a cubic superlattice. The thermoelectric properties of the PbSe superlattice thin films are investigated by means of frequency domain thermoreflectance, scanning thermal probe microscopy, and four‐probe measurements, and augmented by computational efforts. Thermal conductivity of the superlattice films is measured as low as 0.7 W m−1 K−1 at room temperature due to the developed nanostructure. The low values of electrical conductivity are attributed to the presence of insulating oleate capping ligands at the dots’ surface and the small contact area between the PbSe dots within the superlattice. Experimental efforts aiming at the removal of the oleate ligands are conducted by annealing or molten‐salt treatment, and in the latter case, yielded a promising improvement by two orders of magnitude in thermoelectric performance. The result indicates that the straightforward molten‐salt treatment is an interesting approach to derive thermoelectric dot superlattice thin films over a centimeter‐sized area. [ABSTRACT FROM AUTHOR]

Single crystals of (001)‐oriented 0.7Pb(Mg1/3Nb2/3)−0.3PbTiO3 (PMN‐30PT) with a composition near the morphotropic phase boundary have attracted considerable attention due to their superior dielectric and electromechanical performance. Recently, a new alternating current (electric field) poling approach used for the enhancement of dielectric and piezoelectric properties. However, the microscopic domain variants that govern the performance, especially under high‐frequency alternating current (AC) voltages, remain largely unexplored. In this work, the domain microstructure under AC poling reveals the presence of four monoclinic (MA) domain variants using a suite of scanning probe microscopy methods, and X‐ray diffraction (XRD) reciprocal space mapping is tuned. It is reported on the emergence of hierarchical fine domains – needle‐shaped, and 109° domain walls under applied high‐frequency AC poling. Time‐resolved Kelvin probe force microscopy (KPFM) reveals the charge dynamics and relaxation behavior of these needle domains and walls. The findings provide new insight and guidance to the domain engineering by high‐frequency AC poling for the development of advanced transducer technology. [ABSTRACT FROM AUTHOR]

We report on‐surface synthesis of heterochiral 1D heptahelicene oligomers after deposition of a racemic heptahelicene monomer on an Au(111) surface followed by Ullmann coupling under ultrahigh vacuum conditions. Structure, chirality and mode of adsorption of the resulting dimers to octamers are inferred from the scanning probe microscopy and theoretical calculations. [ABSTRACT FROM AUTHOR]

Surface chemistry significantly influences the physicochemical and functional properties of nanoparticles, thus necessitating the investigation of surfaces, especially when subjected to chemisorption. Seeking a method that delivers both high‐resolution imaging and precise chemical information, tip‐enhanced Raman spectroscopy (TERS) emerges as a critical technique. By the combination of scanning probe microscopy with Raman spectroscopy, TERS effectively addresses the limitations of traditional optical microscopes in the study of nanoparticles. The results provide detailed nanoscale structural insights, shed light on surface chemistry, and enable the detection of Raman‐forbidden modes caused by the substantial electric field at the tip apex (≈3 × 108 V m−1). This electric field plays a crucial role in altering selection rules, thereby broadening the scope of TERS beyond merely detecting Raman modes. By combining topographical with TERS mapping, the presence of a carbonate monolayer on the barium titanate (BaTiO3) nanoparticle surface is unveiled – an observation elusive to common characterization techniques. [ABSTRACT FROM AUTHOR]

Highly hydrophilic and antifouling poly(vinylidene fluoride) (PVDF) ultrafiltration membranes are developed with excellent permeation using a zirconium‐based metal–organic framework (MOF‐801). MOF‐801 is synthesized by a solvothermal method using zirconium(IV) oxychloride octahydrate (ZrOCl2⋅8H2O) and fumaric acid. The chemical functionality of MOF‐801 is studied by Fourier transform infrared (FTIR) spectroscopy and X‐ray diffraction (XRD) whereas surface morphology and elemental composition are probed by scanning electron microscopy (SEM)/energy‐dispersive X‐ray analysis (EDX). The PVDF/MOF‐801 membranes are characterized in terms of FTIR, XRD, FESEM/EDX and atomic force microscopy. The performance of the hybrid PVDF/MOF‐801 membranes in terms of pure water flux and antifouling ability is found to be improved compared with bare PVDF membranes. The wettability of the membranes is measured by water contact angle and found to be 76.7° for bare PVDF membrane, which decreases upon the addition of MOF‐801 to 55.1° due to the increase in surface hydrophilicity. A notable increase in roughness of 226.29 nm and a porosity of 67.91% is observed for the addition of 2 wt% MOF‐801 in PVDF membrane matrix. The flux recovery ratio of the hybrid membrane is increased from 66.4% to 89.6% and from 68.3% to 85.2% for bovine serum albumin (BSA) and humic acid (HA) separation, respectively. In addition, the reversible and irreversible fouling performance during the rejection of BSA (93%) and HA (88%) indicates the enhanced antifouling property of the PVDF/MOF‐801 membranes. A zone of inhibition test evidences the outstanding antibiofouling activity of the PVDF/MOF‐801 membranes against E. coli and S. aureus. Overall results demonstrated the suitability of hybrid PVDF/MOF‐801 membranes for water and wastewater treatment. © 2023 Society of Industrial Chemistry. [ABSTRACT FROM AUTHOR]

BiFeO3 is a rare single‐phase multiferroic which shows coupled ferroelectricity, ferroelasticity and antiferromagnetism at room temperature. Many fantastic properties of BiFeO3 are regulated by its domain structure. While (001) rhombohedral BiFeO3 thin films can possibly develop up‐to eight degenerate states of two‐variant 71° ferroelastic domain stripes, complete selective control of all possible switching paths between these states has not yet been achieved. Here, combining phase field simulations and scanning probe microscopy experiments, we demonstrated such a complete selective control. The tip bias and the built‐in field were shown to affect the volume fraction of the 71°, 109° and 180° switched domains in rhombohedral BiFeO3 thin films under single‐point loading. Meanwhile, tip scanning further broke the symmetry of the nucleated domains, leading to different switched domain patterns. We then grew BiFeO3 thin films with a specific two‐variant 71° ferroelastic domain state and showed that such a state could be deterministically switched into the other seven two‐variant domain states by collaborative controlling tip scanning and tip bias in scanning probe microscopy experiments. These results should deepen our current understanding on the domain switching kinetics in BiFeO3 thin films and indicate they are promising platforms for developing configurable electronic and spintronic devices. [ABSTRACT FROM AUTHOR]

A method for patterning single‐layer graphene (SLG) and single‐layer oxidized graphene (SOG) within a continuous atomic layer to form lateral heterojunctions is presented. Raman spectroscopy is employed to investigate the evolution of defect‐related Raman peaks during excimer‐UV irradiation, facilitating the identification of structural changes and defect formation processes. Electrical transport measurements reveal that SOG‐patterned field‐effect transistors (FETs) exhibit varying characteristics depending on the degree of oxidation, thus offering the potential to tailor the electrical properties of graphene devices for specific requirements. Scanning Kelvin probe microscopy measurements reveal the surface potential and work function of the SOG regions compared with those of SLG. The effective functionality of the SOG pattern to operate as a resistor, allowing control of the electrical conductivity in the SOG‐patterned SLG channels, is demonstrated. This capability restricts the current flow while preserving the pristine electrical properties of the graphene channel. Moreover, the SOG pattern can serve as a potential barrier to constructing SLG‐SOG‐patterned integrated circuits, providing exciting opportunities for engineering advanced electronic components. This breakthrough in graphene devices simplifies the fabrication process of graphene‐based FETs and provides the foundation for developing atomically thin integrated circuits for a wide range of applications. [ABSTRACT FROM AUTHOR]

Surface/interface engineering of methylammonium lead bromide (MAPbBr3) single crystals (SCs) is crucial for carrier generation/recombination, separation, and transportation, thereby enabling superior optoelectronics. Herein, a surface‐engineered crystallization technique is presented in which a thin polycrystalline MAPbBr3 layer is in situ grown on the surface of bulk mm‐sized MAPbBr3 SCs. The growth direction and the atomic distribution of both the polycrystalline surface layer and the single crystalline core have been analyzed by damage‐free atomic‐resolution transmission electron microscopy (TEM). The polycrystalline nature of the crystals gives rise to bright green emission under UV light. Scanning probe microscopy results show that the current at the emissive MAPbBr3 film/MAPbBr3 SC surface is five times higher than that at a non‐emissive surface when illuminated. Lateral photodetectors based on MAPbBr3 film/MAPbBr3 SCs can achieve excellent detectivities (≈1013 Jones) and high photoresponsivities (≈20 A W−1). Furthermore, a semiconductor‐based fluorescence quick response (FQR) code is patterned on the same bright green‐emitting surface of the MAPbBr3 film/MAPbBr3 SC using a picosecond laser pulse, with a scalability of 3 × 3 mm2. An FQR code integrated with a photodetector may serve as a potential double security tag in bank cards, passports, door security, etc. [ABSTRACT FROM AUTHOR]

Strained macrocycles display interesting properties, such as conformational rigidity, often resulting in enhanced π‐conjugation or enhanced affinity for non‐covalent guest binding, yet they can be difficult to synthesize. Here we use computational modeling to design a template to direct the formation of an 18‐porphyrin nanoring with direct meso‐meso bonds between the porphyrin units. Coupling of a linear 18‐porphyrin oligomer in the presence of this template gives the target nanoring, together with an unexpected 36‐porphyrin ring by‐product. Scanning tunneling microscopy (STM) revealed the elliptical conformations and flexibility of these nanorings on a Au(111) surface. [ABSTRACT FROM AUTHOR]

Photoresponsive supramolecular polymers have a major potential for applications in responsive materials that are externally triggered by light with spatio‐temporal control of their polymerisation state. While changes in macroscopic properties revealed the adaptive nature of these materials, it remains challenging to capture the dynamic depolymerisation process at the molecular level, which requires fast observation techniques combined with in situ irradiation. By implementing in situ UV illumination into a High‐Speed Atomic Force Microscope (HS‐AFM) setup, we have been able to capture the disassembly of a light‐driven molecular motor‐based supramolecular polymer. The real‐time visualisation of the light‐triggered disassembly process not only reveals cooperative depolymerisation, it also shows that this process continues after illumination is halted. Combining the data with cryo‐electron microscopy and spectroscopy approaches, we obtain a molecular‐level description of the motor‐based polymer dynamics reminiscent of actin chain‐end depolymerisation. Our detailed understanding of supramolecular depolymerisation will drive the development of future responsive polymer systems. [ABSTRACT FROM AUTHOR]

Deeper understanding of processes involved in operation of lithium‐ion batteries (LIBs) is necessary to further optimize them for future applications. Extensive research was conducted on the formation of a solid electrolyte interphase (SEI) on negative battery electrodes, still leaving several questions unanswered. Scanning probe microscopies (SPMs) enable in situ and operando investigations and have the potential to explain some phenomena. Scanning electrochemical microscopy (SECM) and scanning ion conductance microscopy (SICM) could be employed in LIB studies. A novel SICM method based on the redox couple ferrocene/ferrocenium is introduced for applications in carbonate solvents widely used in LIBs. Proof of concept measurements were conducted with a micro milled copper circuit board as model substrate. Furthermore, the proposed SICM approach was hyphenated with feedback mode SECM resulting in the simultaneous mapping of morphology and electrochemical activity. A flexible dual‐probe arrangement was developed enabling usage of both SPM techniques at the same time, and furthermore, an easy replacement of both individual probes if needed. The setup was applied in the characterisation of commercial graphite electrodes for LIBs before and after conducting a pre‐charging protocol. Changes in electrochemical activity and topography of the graphite electrode were resolved in simultaneously generated SECM/SICM recordings. [ABSTRACT FROM AUTHOR]

Mixed‐dimensional heterostructures provide additional freedom to construct diverse functional electronic and optoelectronic devices, gaining significant interest. Herein, highly‐aligned pseudo‐1D tellurium is epitaxially grown on 2D monolayer transition metal dichalcogenides (TMDs), including MoSe2, MoS2, and WS2. A one‐pot chemical vapor deposition (CVD) technique eliminates the normally required transfer steps, thereby producing mixed‐dimensional heterostructures with an ultraclean interface. The controllable epitaxial growth of Te/TMD heterostructures are verified by Raman, scanning probe microscopy (SPM), and transmission electron microscopy (TEM) observation. The photoluminescence results indicate that the emission from TMDs is quenched in the heterostructure, confirming the efficient transfer of photogenerated carriers from TMDs to Te. Additionally, the mixed‐dimensional p‐n Te/MoSe2 heterojunction photodetector presents self‐driven behavior with high responsivity (328 mA W−1), external quantum efficiency (79%), and specific detectivity (8.2 × 109 Jones). The modified facile synthesis strategy and proposed growth mechanism in this study shed light on synthesizing mixed‐dimensional heterojunctions. This opens avenues for fabricating functional devices with reduced sizes and high densities, further enabling miniaturization and integration opportunities. [ABSTRACT FROM AUTHOR]

Electrocatalysis plays a pivotal role in renewable energy conversion and associated chemical production, enabling a variety of emerging sustainability technologies with societal impacts. Achieving marked improvement in electrocatalytic performance relies on a deep understanding of catalyst microstructures and catalytic mechanisms, with a particular emphasis on the detailed, spatiotemporally resolved characterizations of the underlying fundamental electrocatalytic processes. This fundamental need drives the development of operando imaging techniques, which improve the ability to detect dynamic structural changes in electrocatalysts and establish clear structure‐performance relationships for morphologically complex, hierarchically structured catalytic materials. This review aims to highlight significant advancements in the application of operando imaging techniques to develop a deeper understanding of important heterogeneous electrocatalytic reactions critical for emerging sustainability technologies. We summarize the up‐to‐date key mechanistic insights regarding these reactions achieved through a range of operando imaging techniques, including electron microscopies, X‐ray imaging techniques, scanning probe microscopies, and optical microscopies. We conclude by pointing out emerging directions and future prospects within the field of operando imaging in electrocatalysis. [ABSTRACT FROM AUTHOR]

The character of the electronic structure of acenes has been the subject of longstanding discussion. However, convincing experimental evidence of their open‐shell character has so far been missing. Here, we present the on‐surface synthesis of tridecacene molecules by thermal annealing of octahydrotridecacene on a Au(111) surface. We characterized the electronic structure of the tridecacene by scanning probe microscopy, which reveals the presence of an inelastic signal at 126 meV. We attribute the inelastic signal to spin excitation from the singlet diradical ground state to the triplet excited state. To rationalize the experimental findings, we carried out many‐body ab initio calculations as well as model Hamiltonians to take into account the effect of the metallic substrate. Moreover, we provide a detailed analysis of how the dynamic electron correlation and virtual charge fluctuation between the molecule and metallic surface reduces the singlet‐triplet band gap. Thus, this work provides the first experimental confirmation of the magnetic character of tridecacene. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Limited charge separation/transport efficiency remains the primary obstacle of achieving satisfying photoelectrochemical (PEC) water splitting performance. Therefore, it is essential to develop diverse interfacial engineering strategies to mitigate charge recombination. Despite obvious progress having been made, most works only considered a single‐side modulation in either the electrons of conduction band or the holes of valence band in a semiconductor photoanode, leading to a limited PEC performance enhancement. Beyond this conventional thinking, we developed a novel coupling modification strategy to achieve a composite electrode with bidirectional carrier transport for a better charge separation, in which Ti2C3Tx MXene quantum dots (MQDs) and α‐Fe2O3 nanodots (FO) are anchored on the surface of ZnIn2S4 (ZIS) nanoplates, resulting in markedly improved PEC water splitting of pure ZIS photoanode. Systematic studies indicated that the bidirectional charge transfer pathways were stimulated due to MQDs as "electron extractor" and S−O bonds as carriers transport channels, which synergistically favors significantly enhanced charge separation. The enhanced kinetic behavior at the FO/MQDs/ZIS interfaces was systematically and quantitatively evaluated by a series of methods, especially scanning photoelectrochemical microscopy. This work may deepen our understanding of interfacial charge separation, and provide valuable guidance for the rational design and fabrication of high‐performance composite electrodes. [ABSTRACT FROM AUTHOR]

On‐surface synthesis serves as a powerful approach to construct π‐conjugated carbon nanostructures that are not accessible by conventional wet chemistry. Nevertheless, this method has been limited by the types and numbers of available on‐surface transformations. While the majority of successful cases exploit thermally triggered dehalogenative carbon–carbon coupling and cyclodehydrogenation, rearrangement of appropriate functional moieties has received limited research attention. Here, the unprecedented interchain coupling and thermally induced skeleton rearrangement are described of (dihydro)indeno[2,1‐b]fluorene (IF) polymers on an Au(111) surface under ultrahigh vacuum conditions, leading to different ladder polymers as well as fully fused graphene nanoribbon segments containing pentagonal and heptagonal rings. Au‐coordinated nanoribbons are also observed. All structures are unambiguously characterized by high‐resolution scanning probe microscopy. The current results provide an avenue to fabricating a wider variety of π‐conjugated polymers and carbon nanostructures comprising nonhexagonal rings as well as rarely explored organometallic nanoribbons. [ABSTRACT FROM AUTHOR]

We outline an approach to fabricate nanoscale artificial quasiperiodic tilings with thermal‐scanning probe lithography. Quasiperiodic tilings such as the Ammann‐Beenker, Square Fibonacci tiling, and Penrose are fabricated and imaged with thermal‐conductance feedback microscopy, followed by electron microscopy. The design implementation, chemical, and physical challenges involved in fabricating such artificial systems using nanolithography are discussed. Additionally, the potential applications of fabricated quasiperiodic tilings are explored. [ABSTRACT FROM AUTHOR]

Major advancements in fields as diverse as biology and quantum computing have relied on a multitude of microscopy techniques. Despite the considerable proliferation of these instruments, significant bottlenecks remain in terms of processing, analysis, storage, and retrieval of the acquired datasets. Aside from lack of file standards, individual domain‐specific analysis packages are often disjoint from the underlying datasets, and thus keeping track of analysis and processing steps remains tedious for the end‐user, hampering reproducibility. Here, the pycroscopy ecosystem of packages is introduced, an open‐source python‐based ecosystem underpinned by a common data model. The data model, termed the N‐dimensional spectral imaging data format, is realized in pycroscopy's sidpy package. This package is built on top of dask arrays, thus leveraging dask array attributes, but expanding them to accelerate microscopy relevant analysis and visualization. Several examples of the use of the pycroscopy ecosystem to create workflows for data ingestion and analysis of scanning transmission electron microscopy (STEM) and scanning probe microscopy data are shown. Adoption of such standardized routines will be critical to usher in the next generation of autonomous instruments where processing, computation, and meta‐data storage will be critical to overall experimental operations. [ABSTRACT FROM AUTHOR]

The solid‐electrolyte interphase (SEI) is key to stable, high voltage lithium‐ion batteries (LIBs) as a protective barrier that prevents electrolyte decomposition. The SEI is thought to play a similar role in highly concentrated water‐in‐salt electrolytes (WISEs) for emerging aqueous batteries, but its properties remain unknown. In this work, we utilized advanced scanning electrochemical microscopy (SECM) and operando electrochemical mass spectrometry (OEMS) techniques to gain deeper insight into the SEI that occurs within highly concentrated WISEs. As a model, we focus on a 55 mol/kg K(FSA)0.6(OTf)0.4 electrolyte and a 3,4,9,10‐perylenetetracarboxylic diimide negative electrode. For the first time, our work showed distinctly passivating structures with slow apparent electron transfer rates alike to the SEI found in LIBs. In situ analyses indicated stable passivating structures when PTCDI was stepped to low potentials (≈−1.3 V vs. Ag/AgCl). However, the observed SEI was discontinuous at the surface and H2 evolution occurred as the electrode reached more extreme potentials. OEMS measurements further confirmed a shift in the evolution of detectable H2 from −0.9 V to <−1.4 V vs. Ag/AgCl when changing from dilute to concentrated electrolytes. In all, our work shows a combined approach of traditional battery measurements with in situ analyses for improving characterization of other unknown SEI structures. [ABSTRACT FROM AUTHOR]

Carbohydrates are the most abundant organic material on Earth and the structural "material of choice" in many living systems. Nevertheless, design and engineering of synthetic carbohydrate materials presently lag behind that for protein and nucleic acids. Bottom‐up engineering of carbohydrate materials demands an atomic‐level understanding of their molecular structures and interactions in condensed phases. Here, high‐resolution scanning tunneling microscopy (STM) is used to visualize at submolecular resolution the three‐dimensional structure of cellulose oligomers assembled on Au(1111) and the interactions that drive their assembly. The STM imaging, supported by ab initio calculations, reveals the orientation of all glycosidic bonds and pyranose rings in the oligomers, as well as details of intermolecular interactions between the oligomers. By comparing the assembly of D‐ and L‐oligomers, these interactions are shown to be enantioselective, capable of driving spontaneous enantioseparation of cellulose chains from its unnatural enantiomer and promoting the formation of engineered carbohydrate assemblies in the condensed phases. [ABSTRACT FROM AUTHOR]

Highly sensitive and uniform three‐dimensional (3D) hybrid heterogeneous structures for use in surface‐enhanced Raman scattering (SERS) experiments were fabricated by sequentially decorating high‐quality, ultra‐clean, graphene quantum dots (GQDs) and Ag nanoparticles (Ag‐NPs) onto 3D‐graphene. Finite‐difference time‐domain calculations and scanning Kelvin probe microscopy were used to verify that the Ag‐NPs/GQDs/3D‐graphene system facilitates substantial electromagnetic enhancement (due to the occurrence of two kinds of "gaps" between the Ag‐NPs that form 3D "hot spots") and additional chemical enhancement (in detecting some π‐conjugated molecules). The SERS mechanism was explored in further detail via experimental analysis and confirmed by performing theoretical calculations. The large surface area of the 3D substrate (due to the large specific surface areas of the GQDs and 3D‐graphene) results in a better enrichment effect which helps produce lower detection limits. In particular, the detection limits obtained using the Ag‐NPs/GQDs/3D‐graphene platform can reach 10−11 M for rhodamine 6G, 10−10 M for methylene blue and dopamine, and 10−7 M for tetramethylthiuram disulfide and methyl parathion in apple juice (these are superior to most of the results reported using graphene‐based SERS substrates). In summary, the 3D‐platform Ag‐NPs/GQDs/3D‐graphene/Si shows outstanding SERS performance. It therefore has excellent application prospects in biochemical molecular detection and food safety monitoring. [ABSTRACT FROM AUTHOR]

The solid‐electrolyte interphase (SEI) is key to stable, high voltage lithium‐ion batteries (LIBs) as a protective barrier that prevents electrolyte decomposition. The SEI is thought to play a similar role in highly concentrated water‐in‐salt electrolytes (WISEs) for emerging aqueous batteries, but its properties remain unknown. In this work, we utilized advanced scanning electrochemical microscopy (SECM) and operando electrochemical mass spectrometry (OEMS) techniques to gain deeper insight into the SEI that occurs within highly concentrated WISEs. As a model, we focus on a 55 mol/kg K(FSA)0.6(OTf)0.4 electrolyte and a 3,4,9,10‐perylenetetracarboxylic diimide negative electrode. For the first time, our work showed distinctly passivating structures with slow apparent electron transfer rates alike to the SEI found in LIBs. In situ analyses indicated stable passivating structures when PTCDI was stepped to low potentials (≈−1.3 V vs. Ag/AgCl). However, the observed SEI was discontinuous at the surface and H2 evolution occurred as the electrode reached more extreme potentials. OEMS measurements further confirmed a shift in the evolution of detectable H2 from −0.9 V to <−1.4 V vs. Ag/AgCl when changing from dilute to concentrated electrolytes. In all, our work shows a combined approach of traditional battery measurements with in situ analyses for improving characterization of other unknown SEI structures. [ABSTRACT FROM AUTHOR]

Mechanically driven polarization switching via scanning probe microscopy provides a valuable voltage‐free strategy for designing ferroelectric nanodomain structures. However, it is still challenging to realize reversible polarization switching with mechanical forces. Here, the mechanically driven reversible polarization switching observed in imprinted ferroelectric BiFeO3 thin films is reported, i.e., up‐to‐down switching by a sharp scanning tip and down‐to‐up switching by a blunt tip. Free energy calculations, phase‐field simulations, and piezoresponse force microscopy reveal that reversible mechanical switching arises from the interplay among the flexoelectric effect, the piezoelectric effect, and the internal upward built‐in field in BiFeO3 films. This study gains a deeper insight into the mechanism and control of mechanically driven polarization switching, and provides guidance for exploring potential ferroelectric‐based electro‐mechanical microelectronics. [ABSTRACT FROM AUTHOR]

Diamond‐like carbon (DLC) has attracted much attention due to its unique properties such as excellent physicochemical and biological properties. Herein, DLC coatings are deposited on four different silicon substrates using a radio frequency plasma‐assisted chemical vapor deposition (RF‐PECVD) technique. The structure and mechanical properties of DLC coatings deposited on different types of silicon substrates under different powers are compared. The surface morphology of the samples is characterized by scanning electron microscopy. The surface roughness of DLC films deposited on different silicon substrates is measured by scanning probe microscopy (SPM). The structural changes of the coatings are investigated by visible Raman spectroscopy. The analysis of DLC films deposited on different silicon substrates reveals that the structure of DLC films deposited on silicon is affected by different crystal directions of silicon substrates (different atomic densities in different crystal directions) and different conduction modes (electronic conduction and hole conduction). Regarding the DLC films deposited on the same substrate, the overall performance of P‐type silicon is better at 150 W, and the overall performance of N‐type silicon is better when the deposition power is 100 W. [ABSTRACT FROM AUTHOR]

Bicyclo[1.1.1]pentane (BCP) motifs are of growing importance to the pharmaceutical industry as sp3‐rich bioisosteres of benzene rings and as molecular building blocks in materials science. Herein we explore the behavior of 1,3‐disubstituted BCP moieties on metal surfaces by combining low‐temperature scanning tunneling microscopy / non‐contact atomic force microscopy studies with density functional theory modeling. We examine the configuration of individual BCP‐containing precursors on Au(111), their supramolecular assembly and thermally activated dehalogenative coupling reactions, affording polymeric chains with incorporated electronically isolating units. Our studies not only provide the first sub‐molecular insights of the BCP scaffold behavior on surfaces, but also extend the potential application of BCP derivatives towards integration in custom‐designed surface architectures. [ABSTRACT FROM AUTHOR]

Thermoelectric conversion may take a significant share in future energy technologies. Oxide‐based thermoelectric composite ceramics attract attention for promising routes for control of electrical and thermal conductivity for enhanced thermoelectric performance. However, the variability of the composite properties responsible for the thermoelectric performance, despite nominally identical preparation routes, is significant, and this cannot be explained without detailed studies of thermal transport at the local scale. Scanning thermal microscopy (SThM) is a scanning probe microscopy method providing access to local thermal properties of materials down to length scales below 100 nm. To date, realistic quantitative SThM is shown mostly for topographically very smooth materials. Here, methods for SThM imaging of bulk ceramic samples with relatively rough surfaces are demonstrated. "Jumping mode" SThM (JM‐SThM), which serves to preserve the probe integrity while imaging rough surfaces, is developed and applied. Experiments with real thermoelectric ceramics show that the JM‐SThM can be used for meaningful quantitative imaging. Quantitative imaging is performed with the help of calibrated finite‐elements model of the SThM probe. The modeling reveals non‐negligible effects associated with the distributed nature of the resistive SThM probes used; corrections need to be made depending on probe‐sample contact thermal resistance and probe current frequency. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium batteries (ASSLBs) are promising due to their high‐energy output and low‐risk profile, but their development has only just begun. Atomic force microscopy (AFM) and related techniques have had an impact on ASSLBs research by elucidating the interfacial, morphological, mechanical, electrical, and electrochemical properties of a wide range of electrodes and electrolytes. However, because a cross‐section cut is necessary to define the solid–solid interface, true in situ analysis is not practical. The first part of this review will assess recent advancements in the study of ASSLBs utilizing AFM and other scanning probe microscopy techniques. The interior solid–solid interfaces can be illuminated in situ using X‐ray computed tomography (X‐CT) and other nondestructive characterization techniques, whereas, in contrast, to deepen the subject, it is further examined how X‐CT vary from the use of other instruments for solid‐state battery characterization, compare the information that various methods may give, and assess how well they can accurately reflect real batteries. This review may serve as a reference and point researchers in the direction of future study on the solid–solid interface of ASSLBs. [ABSTRACT FROM AUTHOR]

Functionality of domain walls and other topological defects in ferroelectrics is being widely investigated for applications in electronic devices. While the intrinsic electronic properties of a wall have been considered, its inherent mechanical properties remain explored very little, despite the fact that coupling between strain and polarization is prevalent in many of these materials. Herein, an in‐depth study of variations in nanomechanical properties at 90o domain walls and their adjacent domains in single‐crystalline lead titanate (PbTiO3) is presented as a prototypical ferroelectric material using a combination of various atomic force microscopy (AFM)‐based methods. Considerable variations of elastic moduli are found at 90o domain walls extending up to ~100 nm into the domain areas. AFM nanoindentation also allows to extract local domain wall hardness and plastic and elastic deformation energies. These findings have implications for the design of ferroelectric domain wall functionality that incorporates the intrinsic elastic compliance of a domain wall. [ABSTRACT FROM AUTHOR]

Functionality of domain walls and other topological defects in ferroelectrics is being widely investigated for applications in electronic devices. While the intrinsic electronic properties of a wall have been considered, its inherent mechanical properties remain explored very little, despite the fact that coupling between strain and polarization is prevalent in many of these materials. Herein, an in‐depth study of variations in nanomechanical properties at 90o domain walls and their adjacent domains in single‐crystalline lead titanate (PbTiO3) is presented as a prototypical ferroelectric material using a combination of various atomic force microscopy (AFM)‐based methods. Considerable variations of elastic moduli are found at 90o domain walls extending up to ~100 nm into the domain areas. AFM nanoindentation also allows to extract local domain wall hardness and plastic and elastic deformation energies. These findings have implications for the design of ferroelectric domain wall functionality that incorporates the intrinsic elastic compliance of a domain wall. [ABSTRACT FROM AUTHOR]

Atomically thin, 2D semiconductors, such as transition metal dichalcogenides, complement silicon in ultra‐scaled nano‐electronic devices. However, the semiconductor and its interfaces become increasingly more difficult to characterize chemically and electrically. Conventional methodologies, including scanning probe microscopies, fail to capture insight into the chemical and electronic nature of the semiconductor, albeit vital to understand its impact on the semiconductor performance. Therefore, this work presents a unique and universal in situ approach combining time‐of‐flight secondary ion mass spectrometry and atomic force microscopy to map chemical differences between regions of different electrical conductivity in epitaxially deposited tungsten disulfide (WS2) on sapphire substrates. Surprisingly, WS2 regions of lower electrical conductivity possess a larger amount of sulfur compared to regions with higher conductivity, for which oxygen is also detected. Such difference in chemical composition likely roots from the non‐homogeneously terminated sapphire starting surface, altering the WS2 nucleation behavior and associated defect formation between neighboring sapphire terraces. These resulting sapphire terrace‐dependent doping effects in the WS2 hamper its electrical conductivity. Thus, accurate chemical assignment at a sub‐micrometer lateral resolution of atomically thin 2D semiconductors is vital to achieve a more detailed understanding on how the growth behavior affects the electrical properties. [ABSTRACT FROM AUTHOR]

Fermi's golden rule, a remarkable concept for the transition probability involving continuous states, is applicable to the interfacial electron‐transporting efficiency via correlation with the surface density of states (SDOS). Yet, this concept has not been reported to tailor single‐molecule junctions where gold is an overwhelmingly popular electrode material due to its superior amenability in regenerating molecular junctions. At the Fermi level, however, the SDOS of gold is small due to its fully filled d‐shell. To increase the electron‐transport efficiency, herein, gold electrodes are modified by a monolayer of platinum or palladium that bears partially filled d‐shells and exhibits significant SDOS at the Fermi energy. An increase by 2–30 fold is found for single‐molecule conductance of α,ω‐hexanes bridged via common headgroups. The improved junction conductance is attributed to the electrode self‐energy which involves a stronger coupling with the molecule and a larger SDOS participated by d‐electrons at the electrode‐molecule interfaces. [ABSTRACT FROM AUTHOR]

Ferroelectric domain walls have emerged as one of the most fascinating objects in condensed matter physics due to the broad variability of functional behaviors they exhibit. However, the vast majority of domain walls studies have been focused on bias‐induced dynamics and transport behaviors. Here, the scanning probe microscopy approach based on piezoresponse force microscopy (PFM) with a dynamically heated probe, combining local heating and local biasing of the material is introduced. This approach is used to explore the thermal polarization dynamics in soft Sn2P2S6 ferroelectrics, and allows for the exploration of phase transitions at individual domain walls. The strong and weak modulation regimes for the thermal PFM are introduced. The future potential applications of heated probe approach for functional SPM measurements including piezoelectric, elastic, microwave, and transport measurements are discussed. [ABSTRACT FROM AUTHOR]