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The charge state of noble metal atoms on a semiconductor surface is an important factor in surface catalysis. In this study, Au atoms were deposited on the rutile TiO2(110) surface to characterize its charge properties using atomic force microscopy with Kelvin probe force microscopy at 78 K. Au single atoms, dimers, and trimers at different sites on the surface were investigated. Positively charged Au atoms were verified at oxygen sites, while negatively charged Au atoms were found near oxygen vacancy sites. Furthermore, the charge states of small Au nanoclusters were clarified. Understanding the charge states of Au atoms is significant for identifying their efficient catalytic effects in surface catalysis.
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Near-field images of molecules provide information about their excited orbitals, giving rise to photonic and chemical functions. Such information is crucial to the elucidation of the full potential of molecules as components in functional materials and devices at the nanoscale. However, direct imaging inside single molecules with a complex structure in the near-field is still challenging because it requires in situ observation at a higher resolution than the molecular scale. Here, using a proven theoretical method that has demonstrated sub-nanoscale resolution based on photoinduced force microscopy (PiFM) experiment [Nat. Commun.12, 3865 (2021)10.1038/s41467-021-24136-2], we propose an approach to obtaining the near-field imaging with spatial patterns of electronic transitions of single molecules. We use an extended discrete dipole approximation method that incorporates microscopic nonlocal optical response of molecules and demonstrate that PiFM can visualize circular-dichroism signal patterns at sub-nanometer scale for both optically allowed and forbidden transitions. The result will open the possibility for the direct observation of complex spatial patterns of electronic transitions in a single molecule, providing insight into the optical function of single molecules and helping realize new functional materials and devices.
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Paraffin and octadecyltrichlorosilane (OTS) coatings can alleviate collisions between alkali-metal atoms and cell walls and then prolong the atomic spin-polarization lifetime. The surface structure and collision effects of these antirelaxation coatings, as well as the methods to avoid antirelaxation invalidity, have been the focus of researchers. This study investigated the thermolability of coating surface structure and the collision interactions between alkali metal atoms and coatings, considering the influence of various coating preparation factors, where this collision interaction is indirectly analyzed by measuring the collision energy dissipation between an atomic force microscopy (AFM) probe and the atoms on the coating surface. We found that appropriate evaporation time, carbochain length, and postannealing process can enhance the thermostability of the paraffin coating and eliminate its morphological defects. Furthermore, the OTS/water concentration, the soaking time, and the type of solvent have different levels of influence on the cluster formation and the thermostability of the OTS coatings. Moreover, the antirelaxation performance of coatings has been shown to be characterized by counting the energy dissipated when the AFM probe collides with the antirelaxation coating, replacing the conventional light-atom interaction- based method for measuring the relaxation characteristics, but requiring specific coating preparation factors to be maintained.
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BACKGROUND: To clarify the association between psychosocial problems and frailty in the areas affected by the Great East Japan Earthquake, and to develop strategies for preventive long-term care in the community, we launched the Kesennuma Study in 2019. This report describes the study design and the participants' profiles at baseline. METHODS: The prospective study comprised 9,754 people (4,548 men and 5,206 women) randomly selected from community-dwelling independent adults aged 65 to 84 who were living in Kesennuma City, Miyagi. The baseline survey was conducted in October 2019. It included information on general health, socio-economic status, frailty, lifestyle, psychological factors (eg, personality, depressive moods), and social factors (eg, social isolation, social capital). A follow-up questionnaire survey is planned. Mortality, incident disability, and long-term care insurance certifications will also be collected. RESULTS: A total of 8,150 questionnaires were returned (83.6% response rate), and 7,845 were included in the analysis (80.4%; mean age 73.6 [standard deviation, 5.5] years; 44.7% male). About 23.5% were considered frail. Regarding psychological and social functions, 42.7% had depressive moods, 29.1% were socially isolated, and only 37.0% participated in social activities at least once a month. However, 82.5% trusted their neighbors. CONCLUSION: While local ties were strong, low social activity and poor mental health were revealed as issues in the affected area. Focusing on the association between psychological and social factors and frailty, we aim to delay the need for long-term care for as long as possible, through exercise, nutrition, social participation, and improvement of mental health.
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Terremotos , Fragilidad , Humanos , Masculino , Femenino , Anciano , Fragilidad/prevención & control , Estudios Prospectivos , Japón/epidemiología , Vida Independiente , Anciano FrágilRESUMEN
Titanium dioxide (TiO2) is of considerable interest as a photocatalyst and a catalyst support. Surface hydroxyl groups (OH) are the most common adsorbates on the TiO2 surface and are believed to play crucial roles in their applications. Although the characteristics of bridging hydroxyl (OHbr) have been well understood, the adsorption structure and charged states of terminal hydroxyl (OHt) have not yet been experimentally elucidated at an atomic scale. In this study, we have investigated an isolated OHt on the rutile TiO2(110) surface by atomic force microscopy (AFM) and Kelvin probe force microscopy (KPFM). We found that OHt is in a negatively charged state. The unique characteristic of OHt is different from that of OHbr and involves the amphoterism and diversity of catalytic reactions of TiO2.
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The strain has been employed for controlled modification of electronical and mechanical properties of two-dimensional (2D) materials. However, the thermal strain-engineered behaviors of the CVD-grown MoS2have not been systematically explored. Here, we investigated the strain-induced structure and properties of CVD-grown triangular MoS2flakes by several advanced atomic force microscopy. Two different kinds of flakes with sharp-corner or vein-like nanostructures are experimentally discovered due to the size-dependent strain behaviors. The critical size of these two kinds of flakes can be roughly estimated at â¼17µm. Within the small flakes, the sharp-corner regions show specific strain-modified properties due to the suffering of large tensile strain. While in the large MoS2flakes, the complicated vein-like nanoripple structures were formed due to the interface slipping process under the larger tensile strain. Our work not only demonstrates the size-specific strain behaviors of MoS2flakes but also sheds light on the artificial design and preparation of strain-engineered nanostructures for the devices based on the 2D materials.
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We present a theoretical study on the measurement of photoinduced force microscopy (PiFM) for composite molecular systems. Using discrete dipole approximation, we calculate the self-consistent response electric field of the entire system, including the PiFM tip, substrate, and composite molecules. We demonstrate a higher sensitivity for PiFM measurement on resonant molecules than the previously obtained tip-sample distance dependency, z-4, owing to multifold enhancement of the localized electric field induced at the tip-substrate nanogap and molecular polarization. The enhanced localized electric field in PiFM allows high-resolution observation of forbidden optical electronic transitions in dimer molecules. We investigate the wavelength dependence of PiFM for dimer molecules, obtaining images at incident light wavelengths corresponding to the allowed and forbidden transitions. We reveal that these PiFM images drastically change with the frequency-dependent spatial structures of the localized electric field vectors and resolve different types of nanoparticles beyond the resolution for the optically allowed transitions. This study demonstrates that PiFM yields multifaceted information based on microscopic interactions between nanomaterials and light.
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Understanding oxygen adsorption and dissociation on the five-fold coordinated titanium (Ti5c) site of the rutile TiO2 surface is important in clarifying chemical reaction processes. Accordingly, three different configurations of molecularly adsorbed O2, including parallel side-on, inclined side-on and end-on configurations, and their dissociation were directly observed with atomic resolution at 78 K by atomic force microscopy. Our results experimentally demonstrated that the three adsorbed O2 configurations could be changed by electric field stimulation. The initial configurations of the adsorbed O2 and transition of O2 configurations were related to their coverage. On the other hand, the tunneling current stimulation could dissociate these O2 species, indicating that they are precursors for the O adatom (Oad). It is proposed that the effect of electric field stimulation contributes to the transition of these three adsorbed O2 configurations, and the effect of the tunneling current is the main factor for the dissociation of the adsorbed O2. In addition, based on the atomic contrast and height histograms of Oad, different charge states of Oad were observed, which could coexist on the surface region. The present study demonstrates an intuitional observation of O2 adsorption and dissociation on the Ti5c site, and thus is expected to be useful to understand the surface reactions on the oxide surface.
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Interfacial engineering, such as molecule intercalation, can modify properties and optimize performance of van der Waals heterostructures and their devices. Here, we investigated the pristine and water molecule intercalated heterointerface of niobium disulphide (NbS2) on hexagonal boron nitride (h-BN) (NbS2/BN) using advanced atomic force microscopy (AFM), and observed the metal-insulator transition (MIT) of first layer (1L-) of NbS2 induced by water molecule intercalation. In pristine sample, interfacial charge transfers were confirmed by the direct detection of trapped static charges at the post-exposed h-BN surface, produced by mechanically peeling off the 1L-NbS2 from the substrate. The interfacial charge transfers facilitate the intercalation of water molecules at the heterointerface. The intercalated water layers make a MIT of 1L-NbS2, while the pristine metallic state of the following NbS2 layers remains preserved. This work is of great significance to help understand the interfacial properties of 2D metal/insulator heterostructures and can pave the way for further preparation of an ultrathin transistor.
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For the first time, the charge states of adsorbed oxygen adatoms on the rutile TiO2(110)-1×1 surface are successfully measured and deliberately manipulated by a combination of noncontact atomic force microscopy and Kelvin probe force microscopy at 78 K under ultrahigh vacuum and interpreted by extensive density functional theory modeling. Several kinds of single and double oxygen adatom species are clearly distinguished and assigned to three different charge states: Oad-/2Oad-, Oad2-/2Oad2-, and Oad--Oad2-, i.e., formal charges of either one or two electrons per atom. Because of the strong atomic-scale image contrast, these states are clearly resolved. The observations are supported by measurements of the short-range force and local contact potential difference as a function of the tip-sample distance as well as simulations. Comparison with the simulations suggests subatomic resolution by allowing us to resolve the rotated oxygen p orbitals. In addition, we manage to reversibly switch the charge states of the oxygen adatoms between the Oad- and Oad2- states, both individually and next to another oxygen, by modulating the frequency shift at constant positive voltage during both charging and discharging processes, i.e., by the tip-induced electric field of one orientation. This work provides a novel route for the investigation of the charge state of the adsorbates and opens up novel prospects for studying transition-metal-oxide-based catalytic reactions.
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We have carried out high-speed imaging of the topography and local contact potential difference (LCPD) on rutile TiO2(110) in O2 gas by atomic force microscopy (AFM) and Kelvin probe force microscopy (KPFM). We succeeded in KPFM/AFM imaging with atomic resolution at 1 frame min-1 and observed the adsorbate on a hydroxylated TiO2(110) surface. The observed adsorbate is considered to be oxygen adatoms (Oa), hydroperoxyls (HO2), or terminal hydroxyls (OHt). After adsorption, changes in the topography and the LCPD of the adsorbate were observed. This phenomenon is thought to be caused by the charge transfer of the adsorbate. This technique has the potential to observe catalytic behavior with atomic resolution.
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Clarifying the atomic configuration of step edges on a rutile TiO2 surface is crucial for understanding its fundamental reactivity, and the direct observation of atomic step edges is still a challenge. AFM is a powerful tool for investigating surface structures with true atomic resolution, and it provides the opportunity to resolve the real structure of step edges with improved techniques. In this work, we successfully imaged the atomic configuration of 001 and 1-11 step edges on the surface of rutile TiO2(110)-(1 × 1), and we present the direct observation of oxygen vacancies along the 1-11 step edges, indicating that one 1-11 step edge site corresponds to one oxygen vacancy using AFM. We also made use of the simultaneous AFM/STM measurements to explore the electronic structure of step edges, which enhanced the evidence of oxygen vacancies existing along the 1-11 step edges and further demonstrated that the 001 step edge was terminated by an O row. The effect of the reduced 1-11 step edges was explored by probing the O2 adsorption and the nucleation behavior of gold clusters. It was found that oxygen vacancies along the 1-11 step edges could contribute to O2 dissociative adsorption and there was no obvious difference compared with the oxygen vacancies on the flat terrace. The reduced step edge and terrace likewise acted as nucleation and growth sites for gold atoms/nanoparticles, in line with previous reports. The present study provides a complete characterization of the atomic configuration of the step edges on the TiO2(110) surface and plays an important role in investigating the surface chemistry of metal oxides.
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CONTEXT: The roles of adult daycare services during disaster evacuations in the relationships with community resilience are unknown. The initial 72 hours after a disaster are crucial because people in the disaster area depend on their own efforts or the resources available at the moment until the arrival of external support. OBJECTIVE: To clarify the evacuation-related decision making of the administrators of adult daycare services within 72 hours after the Great East Japan Earthquake and to describe the roles of adult daycare services during the month following the earthquake. DESIGN: Qualitative study using semistructured interviews. The transcribed interviews were analyzed anonymously through an inductive qualitative content analysis using ATLAS.ti. SETTING: Kesennuma City, Miyagi Prefecture. PARTICIPANTS: Eleven key informants (3 primary care providers and 8 administrators) from 8 institutions. RESULTS: Immediately after the disaster, 6 institutions implemented shelter-in-place. The evacuation behaviors of the adult daycare institutions were diverse, but each institution was transformed repeatedly within 72 hours. With respect to evacuation decision making, the primary issues involved whether to go to mandatory evacuation sites. However, after 3 days, the institutions relocated from these sites to other places. During a period of approximately 1 month, 7 institutions managed the evacuation of service users and care providers. The expanded institutional roles were as follows: "confirming the safety of the users' families," "substituting residential facilities," and "imposing leadership during the evacuation." CONCLUSIONS: If institutions choose to shelter-in-place, it should be sustained for as long as possible. Sufficiently planned stores of food and water to accommodate daytime users are needed. Institutions that employ shelter-in-place as an evacuation plan should maintain close contact with local governments. Furthermore, local governments should predetermine how to manage these institutions in the event of a disaster. To build community resilience for disasters, developing linkage with private organizations' resilience is beneficial.
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Centros de Día para Mayores/métodos , Toma de Decisiones , Terremotos , Centros de Día para Mayores/organización & administración , Anciano , Anciano de 80 o más Años , Planificación en Desastres/métodos , Refugio de Emergencia/métodos , Refugio de Emergencia/estadística & datos numéricos , Humanos , Entrevistas como Asunto/métodos , Japón , Investigación CualitativaRESUMEN
The present work proposes magnetic resonance force microscopy (MRFM) based on ferromagnetic resonance (FMR) modulation of a magnetic tip using microwave transmission via a coaxial resonator instead of using conventional microwave irradiation by an external antenna. In this MRFM, the coaxial resonator is electrically connected to the magnetic cantilever tip, which enables simple implementation of FMR excitation of a magnetic tip in conventional magnetic force microscopy. The FMR frequency of the tip can be easily extracted from the reflection spectrum of a transmission line connected to the magnetic tip. The excitation of tip FMR is confirmed from the microwave frequency dependence of the mechanical response of the tip oscillation. This MRFM is effective for extracting the magnetic interaction force near a sample surface without perturbation of its magnetic state. Nanometer-scale imaging of magnetic domain structures on a demagnetized thin-film permanent magnet is successfully demonstrated.
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We propose a new multi-image method for obtaining the frequency shift, tunneling current and local contact potential difference (LCPD) on a TiO2(110) surface with atomic resolution. The tunneling current image reveals rarely observed surface oxygen atoms contrary to the conventional results. We analyze how the surface and subsurface defects affect the distribution of the LCPD. In addition, the subsurface defects are observed clearly in the tunneling current image, in contrast to a topographic image. To clarify the origin of the atomic contrast, we perform site-dependent spectroscopy as a function of the tip-sample distance. The multi-image method is expected to be widely used to investigate the charge transfer phenomena between the nanoparticles and surface sites, and it is useful for elucidating the mechanisms of catalytic reactions.
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We investigate the surface potential distribution on a TiO2 (110)-1 × 1 surface by Kelvin probe force microscopy (KPFM) and atom-dependent bias-distance spectroscopic mapping. The experimental results demonstrate that the local contact potential difference increases on twofold-coordinated oxygen sites, and decreases on OH defects and fivefold-coordinated Ti sites. We propose a qualitative model to explain the origin of the surface potential of TiO2 (110). We qualitatively calculate the surface potential induced by chemical potential and permanent surface dipole. The calculated results agree with our experimental ones. Therefore, we suggest that the surface potential of TiO2 (110) is dominated not only by the permanent surface dipole between the tip apex atom and surface, but also by the dipoles induced by the chemical interaction between the tip and sample. The KPFM technique demonstrate the possibility of investigation of the charge transfer phenomenon on TiO2 surface under gas conditions. It is useful for the elucidation of the mechanism of the catalytic reactions.
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We present an experimental study of coexisting p(2 × 1) and c(6 × 2) phases on an oxygen-terminated Cu(110) surface by noncontact atomic force microscopy (NC-AFM) at 78 K. Ball models of the growth processes of coexisting p(2 × 1)/c(6 × 2) phases on a terrace and near a step are proposed. We found that the p(2 × 1) and c(6 × 2) phases are grown from the super Cu atoms on both sides of O-Cu-O rows of an atomic spacing. In this paper, we summarize our investigations of an oxygen-terminated Cu(110) surface by NC-AFM employing O- and Cu-terminated tips. Also, we state several problems and issues for future investigation.
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We investigated the capability of obtaining atomic resolution surface potential images by frequency-modulation Kelvin probe force microscopy (FM-KPFM) without bias voltage feedback. We theoretically derived equations representing the relationship between the contact potential difference and the frequency shift (Δf) of an oscillating cantilever. For the first time, we obtained atomic resolution images and site-dependent spectroscopic curves for Δf and VLCPD on a Si (111)-7 × 7 surface. FM-KPFM without bias voltage feedback does not involve the influence of the FM-KPFM controller because it has no deviation from a parabolic dependence of Δf on the dc-bias voltage. It is particularly suitable for investigation on molecular electronics and organic photovoltaics, because electron or ion movement induced by dc bias is avoided and the electrochemical reactions are inhibited.
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In magnetic force microscopy (MFM), the tip-sample distance should be reduced to analyze the microscopic magnetic domain structure with high spatial resolution. However, achieving a small tip-sample distance has been difficult because of superimposition of interaction forces such as van der Waals and electrostatic forces induced by the sample surface. In this study, we propose a new method of MFM using ferromagnetic resonance (FMR) to extract only the magnetic field near the sample surface. In this method, the magnetization of a magnetic cantilever is modulated by FMR to separate the magnetic field and topographic structure. We demonstrate the modulation of the magnetization of the cantilever and the identification of the polarities of a perpendicular magnetic medium.
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Visualizing the optical response of individual molecules is a long-standing goal in catalysis, molecular nanotechnology, and biotechnology. The molecular response is dominated not only by the electronic states in their isolated environment but also by neighboring molecules and the substrate. Information about the transfer of energy and charge in real environments is essential for the design of the desired molecular functions. However, visualizing these factors with spatial resolution beyond the molecular scale has been challenging. Here, by combining photoinduced force microscopy and Kelvin probe force microscopy, we have mapped the photoinduced force in a pentacene bilayer with a spatial resolution of 0.6 nm and observed its "multipole excitation". We identified the excitation as the result of energy and charge transfer between the molecules and to the Ag substrate. These findings can be achieved only by combining microscopy techniques to simultaneously visualize the optical response of the molecules and the charge transfer between the neighboring environments. Our approach and findings provide insights into designing molecular functions by considering the optical response at each step of layering molecules.