Externally-triggerable optical pump-probe scanning tunneling microscopy with a time resoloution of tens-picosecond.

Photoinduced carrier dynamics of nanostructures play a crucial role in developing novel functionalities in advanced materials. Optical pump-probe scanning tunneling microscopy (OPP-STM) represents distinctive capabilities of real-space imaging of such carrier dynamics with nanoscale spatial resolution. However, combining the advanced technology of ultrafast pulsed lasers with STM for stable time-resolved measurements has remained challenging.

Hydrogen Bonding Propagated Phase Separation in Quasi-Epitaxial Single Crystals: A Pd-Br Molecular Insulator.

In condensed matter, phase separation is strongly related to ferroelasticity, ferroelectricity, ferromagnetism, electron correlation, and crystallography. These ferroics are important for nano-electronic devices such as non-volatile memory. However, the quantitative information regarding the lattice (atomic) structure at the border of phase separation is unclear in many cases.

Versatile Post-Doping toward Two-Dimensional Semiconductors.

We have developed a simple and straightforward way to realize controlled postdoping toward 2D transition metal dichalcogenides (TMDs). The key idea is to use low-kinetic-energy dopant beams and a high-flux chalcogen beam simultaneously, leading to substitutional doping with controlled dopant densities. Atomic-resolution transmission electron microscopy has revealed that dopant atoms injected toward TMDs are incorporated substitutionally into the hexagonal framework of TMDs.

Subcycle mid-infrared coherent transients at 4 MHz repetition rate applicable to light-wave-driven scanning tunneling microscopy.

We produce subcycle mid-infrared (MIR) pulses at a 4 MHz repetition rate via the optical rectification (OR) of sub-10 fs near-infrared pulses delivered by an optical parametric chirped pulse amplifier. The coherent MIR pulses generated in a GaSe crystal under an ultrabroadband phase-matching condition contain only 0.58-0.

Continuous Heteroepitaxy of Two-Dimensional Heterostructures Based on Layered Chalcogenides.

The in-plane connection and layer-by-layer stacking of atomically thin layered materials are expected to allow the fabrication of two-dimensional (2D) heterostructures with exotic physical properties and future engineering applications. However, it is currently necessary to develop a continuous growth process that allows the assembly of a wide variety of atomic layers without interface degradation, contamination, and/or alloying. Herein, we report the continuous heteroepitaxial growth of 2D multiheterostructures and nanoribbons based on layered transition metal dichalcogenide (TMDC) monolayers, employing metal organic liquid precursors with high supply controllability.

Evolution of local conductance pathways in a single-molecule junction studied using the three-dimensional dynamic probe method.

Understanding of the dynamics of the bonding states of molecules with electrodes while the molecular conformation is changed is particularly important for elucidating the details of electrochemical devices as well as molecular devices in which the reaction dynamics of the electrodes and molecules plays an important role, such as in fuel cells, catalysis and bioelectrochemical devices. However, it has been difficult to make measurements when the distance between counter electrodes is short, namely, the molecule is raised from a lying form, almost parallel and close to the electrodes, toward a standing form and vice versa. We previously have developed a method called the three-dimensional (3D) dynamic probe method, which enables conductance measurement while the conformation of a single-molecule junction is precisely controlled by scanning tunneling microscopy (STM) techniques.

Surface-mediated spin dynamics probed by optical-pump-probe scanning tunneling microscopy.

In current materials science and technologies, surface effects on carrier and spin dynamics in functional materials and devices are of great importance. In this paper, we present the surface-sensitive probing of electron spin dynamics, performed by optical-pump-probe scanning tunneling microscopy (OPP-STM). Time-resolved spin lifetime information on a manganese (Mn)-deposited GaAs(110) surface was successfully obtained for the first time.

The effect of nitrogen lone-pair interaction on the conduction in a single-molecule junction with amine-Au bonding.

We have applied our previously developed three-dimensional dynamic probe method to analyze the conductance in a Au-/1,4-benzenediamine (BDA)/Au single molecule junction. This structure is a typically used example to demonstrate the high performance of the break junction (BJ) method for measuring conductance with small variations, however, details of the interaction of the nitrogen (N) lone-pair in the amine group with a Au electrode, which is considered to have a fundamental role in determining the conductance of the single molecule junction with the amine, have not yet been clarified and still remain an important issue to be resolved. In this study, we have succeeded, for the first time, in observing the site-dependent change in conductance of this system while the molecular conformation was accurately controlled, and the results were well reproduced by a simulation taking account of the effect of the N lone-pair in an amine bonding with a Au electrode.

Revealing the Conformational Dynamics in a Single-Molecule Junction by Site- and Angle-Resolved Dynamic Probe Method.

Single-molecule junctions have been extensively studied because of their high potential for future nanoscale device applications as well as their importance in basic studies for molecular science and technology. However, since the bonding sites at an electrode and the molecular tilt angles, for example, cannot be determined experimentally, analyses have been performed assuming the structures of such interactive key factors, with uncertainties and inconsistencies remaining in the proposed mechanisms. We have developed a methodology that enables the probing of conformational dynamics in single-molecule junctions simultaneously with the direct characterization of molecular bonding sites and tilt angles.

Modulation of electrical potential and conductivity in an atomic-layer semiconductor heterojunction.

Semiconductor heterojunction interfaces have been an important topic, both in modern solid state physics and in electronics and optoelectronics applications. Recently, the heterojunctions of atomically-thin transition metal dichalcogenides (TMDCs) are expected to realize one-dimensional (1D) electronic systems at their heterointerfaces due to their tunable electronic properties. Herein, we report unique conductivity enhancement and electrical potential modulation of heterojunction interfaces based on TMDC bilayers consisted of MoS2 and WS2.

Attractive interaction between Mn atoms on the GaAs(110) surface observed by scanning tunneling microscopy.

Scanning tunneling microscopy/spectroscopy (STM/STS) was carried out to investigate the structures of Mn atoms deposited on a GaAs(110) surface at room temperature to directly observe the characteristics of interactions between Mn atoms in GaAs. Mn atoms were paired with a probability higher than the random distribution, indicating an attractive interaction between them. In fact, re-pairing of unpaired Mn atoms was observed during STS measurement.

Microscopic basis for the band engineering of Mo1-xWxS2-based heterojunction.

Transition-metal dichalcogenide layered materials, consisting of a transition-metal atomic layer sandwiched by two chalcogen atomic layers, have been attracting considerable attention because of their desirable physical properties for semiconductor devices, and a wide variety of pn junctions, which are essential building blocks for electronic and optoelectronic devices, have been realized using these atomically thin structures. Engineering the electronic/optical properties of semiconductors by using such heterojunctions has been a central concept in semiconductor science and technology. Here, we report the first scanning tunneling microscopy/spectroscopy (STM/STS) study on the electronic structures of a monolayer WS2/Mo1-xWxS2 heterojunction that provides a tunable band alignment.

Mechanically activated switching of Si-based single-molecule junction as imaged with three-dimensional dynamic probe.

Understanding and extracting the full functions of single-molecule characteristics are key factors in the development of future device technologies, as well as in basic research on molecular electronics. Here we report a new methodology for realizing a three-dimensional (3D) dynamic probe of single-molecule conductance, which enables the elaborate 3D analysis of the conformational effect on molecular electronics, by the formation of a Si/single molecule/Si structure using scanning tunnelling microscopy (STM). The formation of robust covalent bonds between a molecule and Si electrodes, together with STM-related techniques, enables the stable and repeated control of the conformational modulation of the molecule.

Dynamic probe of ZnTe(110) surface by scanning tunneling microscopy.

The reconstructed surface structure of the II-VI semiconductor ZnTe (110), which is a promising material in the research field of semiconductor spintronics, was studied by scanning tunneling microscopy/spectroscopy (STM/STS). First, the surface states formed by reconstruction by the charge transfer of dangling bond electrons from cationic Zn to anionic Te atoms, which are similar to those of IV and III-V semiconductors, were confirmed in real space. Secondly, oscillation in tunneling current between binary states, which is considered to reflect a conformational change in the topmost Zn-Te structure between the reconstructed and bulk-like ideal structures, was directly observed by STM.

Real space probe of short-range interaction between Cr in a ferromagnetic semiconductor ZnCrTe.

The short-range interaction between Cr atoms was directly examined by scanning tunneling microscopy measurements on a Zn(0.95)Cr(0.05)Te film.

Probing ultrafast spin dynamics with optical pump-probe scanning tunnelling microscopy.

Studies of spin dynamics in low-dimensional systems are important from both fundamental and practical points of view. Spin-polarized scanning tunnelling microscopy allows localized spin dynamics to be characterized and plays important roles in nanoscale science and technology. However, nanoscale analysis of the ultrafast dynamics of itinerant magnetism, as well as its localized characteristics, should be pursued to advance further the investigation of quantum dynamics in functional structures of small systems.

Bases for time-resolved probing of transient carrier dynamics by optical pump-probe scanning tunneling microscopy.

The tangled mechanism that produces optical pump-probe scanning tunneling microscopy spectra from semiconductors was analyzed by comparing model simulation data with experimental data. The nonlinearities reflected in the spectra, namely, the excitations generated by paired laser pulses with a delay time, the logarithmic relationship between carrier density and surface photovoltage (SPV), and the effect of the change in tunneling barrier height depending on SPV, were examined along with the delay-time-dependent integration process used in measurement. The optimum conditions required to realize reliable measurement, as well as the validity of the microscopy technique, were demonstrated for the first time.

Nanoscale probing of transient carrier dynamics modulated in a GaAs-PIN junction by laser-combined scanning tunneling microscopy.

The modulation of carrier dynamics in a GaAs-PIN junction after photoexcitation by an ultrashort-pulse laser was probed by shaken-pulse-pair-excited scanning tunneling microscopy (SPPX-STM), which enables nanoscale mapping of time-resolved STM images. The effect of the built-in potential on the carrier dynamics, diffusion and drift, which cannot be probed by the optical pump-probe technique, was successfully visualized in real space.

Scanning tunneling microscopy/spectroscopy on self-assembly of a glycine/Cu(111) nanocavity array.

The step-by-step analysis of a hierarchical self-assembly revealed the incorporation of nanocavity blocks in a metastable orientation to stabilize the organized array. The confinement of 2D electrons by a quantum corral was verified. Furthermore, manipulation of an isolated C(60) molecule was realized using nanocavities of ∼1.

Physical performance and knee osteoarthritis among community-dwelling women in Japan: the Hizen-Oshima Study, cross-sectional study.

Osteoarthritis (OA) is the most common chronic joint disorder. Relationships between knee OA and physical performance have been examined, but mainly in patients with knee OA. Clarifying the relationship between knee OA and physical performance among community-dwelling individuals is thus important.

Laser-combined scanning tunnelling microscopy for probing ultrafast transient dynamics.

The development of time-resolved scanning tunnelling microscopy (STM), in particular, attempts to combine STM with ultrafast laser technology, is reviewed with emphasis on observed physical quantities and spatiotemporal resolution. Ultrashort optical pulse technology has allowed us to observe transient phenomena in the femtosecond range, which, however, has the drawback of a relatively low spatial resolution due to the electromagnetic wavelength used. In contrast, STM and its related techniques, although the time resolution is limited by the circuit bandwidth (∼100 kHz), enable us to observe structures at the atomic level in real space.

Cross-sectional and longitudinal studies of three-dimensional stereotactic surface projection SPECT analysis in Parkinson's disease.

Although dementia is increasingly recognized as a common feature in Parkinson's disease (PD), its pathological substrate remains unknown. We conducted cross-sectional and longitudinal brain perfusion SPECT analyses to explore changes during the course of developing dementia in PD. Fifty-five patients originally diagnosed with PD were imaged in the cross-sectional study.

Optical doping: active control of metal-insulator transition in nanowire.

The reversible control of metal-insulator transition (MIT) in In/Si(111) nanowires is demonstrated by tuning the band filling of the one-dimensional surface state by optical doping. The control of MIT is carried out by regulating the Fermi level in the surface state around the half-filled position, depending on the carrier density introduced at the interface. We successfully achieved the reversible and active control of MIT via the charge doping by regulating the intensity of photoexcitation.

Microscopic basis for the mechanism of carrier dynamics in an operating p-n junction examined by using light-modulated scanning tunneling spectroscopy.

The doping characteristics and carrier transport in a GaAs p-n junction were visualized with a approximately 10 nm spatial resolution, using light-modulated scanning tunneling spectroscopy. The dynamics of minority carriers under operating conditions, such as recombination, diffusion, and electric field induced drift, which had previously been analyzed on the basis of empirical electric properties, were successfully examined on the nanoscale. These results provide a solid basis for elucidating the mechanism of the carrier transport properties predicted by using the macroscopic analysis.