Myasthenia gravis (MG) is an immune-related adverse event (irAE), and as an irAE, MG (irAE-MG) generally has a monophasic course, with only a few case reports of irAE-MG flare-ups during the course ...of the disease. We herein report a case of pembrolizumab-induced MG with relapsing symptoms. irAE-MG is a rare disease that has not yet been fully characterized, and our case shows that MG symptoms may relapse. Therefore, regular follow-up is necessary, even after the symptoms improve with immunosuppressive therapy.
Walking speed is strongly influenced by the severity of motor paralysis in post-stroke patients. Nevertheless, some patients with mild motor paralysis still walk slowly. Factors associated with this ...difference in walking speed have not been elucidated. To confirm walking characteristics of patients with mild motor paralysis and slow walking speed, this study identified patient subgroups based on the association between the severity of motor paralysis and walking speed. Fugl-Meyer assessment synergy score (FMS) and the walking speed were measured (n = 42), and cluster analysis was performed based on the association between FMS and walking speed to identify the subgroups. FMS and walking speed were associated (ρ = 0.50); however, some patients walked slowly despite only mild motor paralysis. Cluster analysis using FMS and walking speed as the main variables classified patients into subgroups. Patients with mild motor paralysis (FMS: 18.4 ± 2.09 points) and slow walking speed (0.28 ± 0.14 m/s) exhibited poorer trunk stability, increased co-contraction of the shank muscle, and increased intramuscular coherence in walking compared to other clusters. This group was identified by their inability to fully utilize the residual potential of motor function. In walking training, intervention in instability and excessive cortical control may be effective.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Aromaticity is a fundamental concept in chemistry. It is described by Hückel's rule that states that a cyclic planar π-system is aromatic when it shares 4n+2 π-electrons and antiaromatic when it ...possesses 4n π-electrons. Antiaromatic compounds are predicted to exhibit remarkable charge transport properties and high redox activities. However, it has so far only been possible to measure compounds with reduced aromaticity but not antiaromatic species due to their energetic instability. Here, we address these issues by investigating the single-molecule charge transport properties of a genuinely antiaromatic compound, showing that antiaromaticity results in an order of magnitude increase in conductance compared with the aromatic counterpart. Single-molecule current-voltage measurements and ab initio transport calculations reveal that this results from a reduced energy gap and a frontier molecular resonance closer to the Fermi level in the antiaromatic species. The conductance of the antiaromatic complex is further modulated electrochemically, demonstrating its potential as a high-conductance transistor.
Abstract
The electrical properties of DNA have been extensively investigated within the field of molecular electronics. Previous studies on this topic primarily focused on the transport phenomena in ...the static structure at thermodynamic equilibria. Consequently, the properties of higher-order structures of DNA and their structural changes associated with the design of single-molecule electronic devices have not been fully studied so far. This stems from the limitation that only extremely short DNA is available for electrical measurements, since the single-molecule conductance decreases sharply with the increase in the molecular length. Here, we report a DNA zipper configuration to form a single-molecule junction. The duplex is accommodated in a nanogap between metal electrodes in a configuration where the duplex is perpendicular to the nanogap axis. Electrical measurements reveal that the single-molecule junction of the 90-mer DNA zipper exhibits high conductance due to the delocalized π system. Moreover, we find an attractive self-restoring capability that the single-molecule junction can be repeatedly formed without full structural breakdown even after electrical failure. The DNA zipping strategy presented here provides a basis for novel designs of single-molecule junctions.
We hypothesized that postural instability observed in individuals with Parkinson's disease (PD) can be classified as distinct subtypes based on comprehensive analyses of various evaluated parameters ...obtained from time-series of center of pressure (CoP) data during quiet standing. The aim of this study was to characterize the postural control patterns in PD patients by performing an exploratory factor analysis and subsequent cluster analysis using CoP time-series data during quiet standing.
127 PD patients, 47 aged 65 years or older healthy older adults, and 71 healthy young adults participated in this study. Subjects maintain quiet standing for 30 s on a force platform and 23 variables were calculated from the measured CoP time-series data. Exploratory factor analysis and cluster analysis with a Gaussian mixture model using factors were performed on each variable to classify subgroups based on differences in characteristics of postural instability in PD.
The factor analysis identified five factors (magnitude of sway, medio-lateral frequency, anterio-posterior frequency, component of high frequency, and closed-loop control). Based on the five extracted factors, six distinct subtypes were identified, which can be considered as subtypes of distinct manifestations of postural disorders in PD patients. Factor loading scores for the clinical classifications (younger, older, and PD severity) overlapped, but the cluster classification scores were clearly separated.
The cluster categorization clearly identifies symptom-dependent differences in the characteristics of the CoP, suggesting that the detected clusters can be regarded as subtypes of distinct manifestations of postural disorders in patients with PD.
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Thermal transport properties of patterned binary self-assembled monolayers (SAMs) on Au(111) were examined using scanning thermal microscopy (SThM) with both contact and noncontact methods. We ...fabricated two-dimensional (2D) patterns with two separate domains of n-hexadecanethiol/benzenethiol, benzenethiol/n-butanethiol, or n-hexadecanethiol/n-butanethiol. In the experimental setup, the efficiency of thermal transport from a SThM tip to the SAM surface can be evaluated in terms of the temperature change at the SThM tip. In the contact regime, where a SThM tip physically contacts the SAM surface, direct thermal transport through the SAM and radiation-based thermal transport through the space where SAMs exist may contribute to a drop in temperature at the tip. In the noncontact regime, thermal transport relies on radiation-based heat dissipation from the heated tip to the SAMs. 2D mapping of the spatial temperature distribution on SAMs reflects the difference in thermal transport properties of the two SAM domains. We found that the contact method is effective for visualizing the temperature contrast, which reflects the thermal transport properties of the constituent molecules when the domains of the SAMs have a similar height, while the noncontact method allows visualization of the temperature distribution, which is related to the height of each domain of the SAMs, rather than the chemical structures of the constituent molecules. Combination of contact and noncontact SThM enables 2D imaging of thermal transport properties and topographic imaging simultaneously and represents a new technique for investigating the thermal properties of materials surfaces, which is essential for nanoscale thermal management.
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IJS, KILJ, NUK, PNG, UL, UM
Structural and electronic detail at the metal–molecule interface has a significant impact on the charge transport across the molecular junctions, but its precise understanding and control still ...remain elusive. On the single-molecule scale, the metal–molecule interface structures and relevant charge transport properties are subject to fluctuation, which contain the fundamental science of single-molecule transport and implication for manipulability of the transport properties in electronic devices. Here, we present a comprehensive approach to investigate the fluctuation in the metal–molecule interface in single-molecule junctions, based on current–voltage (I–V) measurements in combination with first-principles simulation. Contrary to conventional molecular conductance studies, this I–V approach provides a correlated statistical description of both the degree of electronic coupling across the metal–molecule interface and the molecular orbital energy level. This statistical approach was employed to study fluctuation in single-molecule junctions of 1,4-butanediamine (DAB), pyrazine (PY), 4,4′-bipyridine (BPY), and fullerene (C60). We demonstrate that molecular-dependent fluctuation of σ-, π-, and π-plane-type interfaces can be captured by analyzing the molecular orbital (MO) energy level under mechanical perturbation. While the MO level of DAB with the σ-type interface shows weak distance dependence and fluctuation, the MO level of PY, BPY, and C60 features unique distance dependence and molecular-dependent fluctuation against the mechanical perturbation. The MO level of PY and BPY with the σ+π-type interface increases with the increase in the stretch distance. In contrast, the MO level of C60 with the π-plane-type interface decreases with the increase in the stretching perturbation. This study provides an approach to resolve the structural and electronic fluctuation in the single-molecule junctions and insight into the molecular-dependent fluctuation in the junctions.
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Here, we report multinuclear organometallic molecular wires having (2,5-diethynylthiophene)diyl-Ru(dppe)
2
repeating units. Despite the molecular dimensions of 2-4 nm the multinuclear wires show high ...conductance (up to 10
−2
to 10
−3
G
0
) at the single-molecule level with small attenuation factors (
β
) as revealed by STM-break junction measurements. The high performance can be attributed to the efficient energy alignment between the Fermi level of the metal electrodes and the HOMO levels of the multinuclear molecular wires as revealed by DFT-NEGF calculations. Electrochemical and DFT studies reveal that the strong Ru-Ru interaction through the bridging ligands raises the HOMO levels to access the Fermi level, leading to high conductance and small
β
values.
Multinuclear organometallic molecular wires having (diethynylthiophene)diyl-Ru(dppe)
2
repeating units show high conductance with small attenuation factors. The strong Ru-Ru interaction is the key for the long-range carrier transport.
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The microscopic mechanism of time-dependent crack growth (TDCG) in single crystal (SC) Ni-based superalloys under a relatively high-temperature condition (900 °C) is critically investigated. Two ...alloy types are compared: alloy A containing 3% rhenium (Re) and alloy B containing no Re. With an initial stress intensity (K) value of 40 MPam1/2, both alloys show similar two step TDCG, i.e. a steady stage followed by an acceleration stage. The total life to failure (tf) of alloy B is, however, an order of magnitude shorter than alloy A. In addition to the conventional fractography, cross-sectional analyses (EBSD and EDS) are also conducted for an interrupted crack tip. Two distinct fracture modes are then identified in both alloys: {111} twin-induced shear fracture and non-crystallographic fracture along dendrite boundaries. The twin systems observed are the secondary ones having a relatively smaller Schmid factor compared to the primary ones that remain inactive under the tension. In the case of alloy A, the twin induces local phase transformation involving TCP precipitation, decomposition of γ (Ni)/γ’ (Ni3Al) structure and recrystallization, which eventually enhances local ductility and dominates the crack growth rate. In the case of alloy B, the macroscopic appearances of these fracture modes are much the same, but they are significantly facilitated by micro-voids formed exclusively in γ channel whose stability is much lower than that in alloy A. The apparently brittle TDCG nature of alloy B compared to alloy A can be interpreted as an enhanced localization of plasticity at the crack tip.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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