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Neutral radical bis(dithiolene) gold complexes [Au(dt)2]Ë are known to exhibit a strong absorption in the 1400-2000 nm NIR absorption range. Here, we demonstrate that the NIR signature of mixed-ligand bis(dithiolene) gold complexes [Au(dtA)(dtD)]Ë associating two different dithiolene, dtA and dtD, is found at higher energy, out of the range of the homoleptic analogs [Au(dtA)2]Ë and [Au(dtD)2]Ë, in the looked-after NIR-II 1000-1400 nm absorption range. An efficient synthetic approach towards precursor mixed-ligand monoanionic gold bis(dithiolene) complexes [Au(dtA)(dtD)]-1 is reported. Using this strategy, no symmetrical complexes are formed and, upon electrocrystallization, no scrambling was observed in solution, allowing for the isolation of radical gold bis(dithiolene) complex such as [Au(bdt)(Et-thiazdt)]Ë (bdt: benzene-1,2-dithiolate; Et-thiazdt: N-ethyl-thiazoline-2-thione-3,4-dithiolate), which behaves as a single-component conductor. It is shown from theoretical calculations that the spin polarization induced by electron repulsions leads to a strong localization of the spin-orbitals, and provides a sound basis to understand, (i) the different ligand-based oxidation potentials, (ii) the NIR optical absorption at notably higher energies and (iii) the larger potential difference of the two redox processes than in the parent symmetric complexes. The solid-state properties of the radical complex [Au(bdt)(Et-thiazdt)]Ë are the consequence of a strongly 1D electronic structure with weakly dimerized chains and electronic localization favoring a semiconducting behavior, stable under pressures up to 18.2 GPa. Altogether, the versatility of the preparation method of [Au(dtA)(dtD)]-1 salts opens the route for a wide library of different mixed-ligand radical complexes [Au(dtA)(dtD)]Ë with simultaneously an adaptable absorption in the NIR-II range and the rich structural chemistry of single-component conductors.
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Symmetry-protected band degeneracy, coupled with a magnetic order, is the key to realizing novel magnetoelectric phenomena in topological magnets. While the spin-polarized nodal states have been identified to introduce extremely-sensitive electronic responses to the magnetic states, their possible role in determining magnetic ground states has remained elusive. Here, taking external pressure as a control knob, we show that a metal-insulator transition, a spin-reorientation transition, and a structural modification occur concomitantly when the nodal-line state crosses the Fermi level in a ferrimagnetic semiconductor Mn3Si2Te6. These unique pressure-driven magnetic and electronic transitions, associated with the dome-shaped Tc variation up to nearly room temperature, originate from the interplay between the spin-orbit coupling of the nodal-line state and magnetic frustration of localized spins. Our findings highlight that the nodal-line states, isolated from other trivial states, can facilitate strongly tunable magnetic properties in topological magnets.
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Ultrafast optical manipulation of magnetic phenomena is an exciting achievement of mankind, expanding one's horizon of knowledge toward the functional nonequilibrium states. The dynamics acting on an extremely short timescale push the detection limits that reveal fascinating light-matter interactions for nonthermal creation of effective magnetic fields. While some cases are benchmarked by emergent transient behaviors, otherwise identifying the nonthermal effects remains challenging. Here, a femtosecond time-resolved resonant magnetic X-ray diffraction experiment is introduced, which uses an X-ray free-electron laser (XFEL) to distinguish between the effective field and the photoinduced thermal effect. It is observed that a multiferroic Y-type hexaferrite exhibits magnetic Bragg peak intensity oscillations manifesting entangled antiferromagnetic (AFM) and ferromagnetic (FM) Fourier components of a coherent AFM magnon. The magnon trajectory constructed in 3D space and time domains is decisive to evince ultrafast field formation preceding the lattice thermalization. A remarkable impact of photoexcitation across the electronic bandgap is directly unraveled, amplifying the photomagnetic coupling that is one of the highest among AFM dielectrics. Leveraging the above-bandgap photoexcitation, this energy-efficient optical process further suggests a novel photomagnetic control of ferroelectricity in multiferroics.
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CsV3Sb5 exhibits superconductivity at Tc = 3.2 K after undergoing intriguing two high-temperature transitions: charge density wave order at ~98 K and electronic nematic order at Tnem ~ 35 K. Here, we investigate nematic susceptibility in single crystals of Cs(V1-xTix)3Sb5 (x = 0.00-0.06) where double-dome-shaped superconducting phase diagram is realized. The nematic susceptibility typically exhibits the CurieâWeiss behaviour above Tnem, which is monotonically decreased with x. Moreover, the CurieâWeiss temperature is systematically suppressed from ~30 K for x = 0 to ~4 K for x = 0.0075, resulting in a sign change at x = ~0.009. Furthermore, the Curie constant reaches a maximum at x = 0.01, suggesting drastically enhanced nematic susceptibility near a putative nematic quantum critical point (NQCP) at x = ~0.009. Strikingly, Tc is enhanced up to ~4.1 K with full Meissner shielding realized at x = ~0.0075-0.01, forming the first superconducting dome near the NQCP. Our findings directly point to a vital role of nematic fluctuations in enhancing the superconducting properties of Cs(V1-xTix)3Sb5.
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Supercondutividade , Titânio , Humanos , Eletrônica , Febre , RegistrosRESUMO
Ca1-xLaxFeAs2 (CLFA112) belongs to a new family of Fe-based superconductors (FeSCs) and has a unique crystal structure featuring an arsenic zigzag chain layer, which has been proposed to be a possible two-dimensional topological insulator. This suggests that CLFA112 is a potential topological superconductor-a platform to realize Majorana fermions. Up to now, even a clear superconducting (SC) gap in CLFA112 has never been observed, and the SC properties of CLFA112 remain largely elusive. In this letter, we report the results of an atomic-scale investigation of the electronic structure of CLFA112 crystals using low-temperature scanning tunneling microscopy (STM). We revealed four different types of surfaces exhibiting distinct electronic properties, with all surfaces displaying dominating 2 × 1 surface reconstructions. On a Ca/La layer on top of an FeAs layer, a clear SC gap of ~12 mV was observed only at the crevices (vacancies) where the FeAs layer can be directly accessed. Remarkably, the FeAs termination layer displayed a dispersing nematic modulation both in real and q space. We also present peculiar zero-bias conductance peaks for the very As chain layer that is believed to exhibit a topological edge state as well as the influence of La dopants on the As chain layer.
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The structure of dielectric perovskite BaZrO3, long known to be cubic at room temperature without any structural phase transition with variation in temperature, has been recently disputed to have different ground state structures with lower symmetries involving octahedra rotation. Pressure-dependent Raman scattering measurements can identify the hierarchy of energetically-adjacent polymorphs, helping in turn to understand its ground state structure at atmospheric pressure. Here, the Raman scattering spectra of high-quality BaZrO3 single crystals grown by the optical floating zone method are investigated in a pressure range from 1 atm to 42 GPa. First, based on the analyses of the infrared and Raman spectra measured at atmospheric pressure, it was found that all the observed vibrational modes could be assigned according to the cubic Pm3¯m structure. In addition, by applying pressure, two structural phase transitions were found at 8.4 and 19.2 GPa, one from the cubic to the rhombohedral R3¯c phase and the other from the rhombohedral to the tetragonal I4/mcm phase. Based on the two pressure-induced structural phase transitions, the true ground state structure of BaZrO3 at room temperature and ambient pressure was corroborated to be cubic while the rhombohedral phase was the closest second.
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In spite of great application potential as transparent n-type oxides with high electrical mobility at room temperature, threading dislocations (TDs) often found in the (Ba,La)SnO3 (BLSO) films can limit their intrinsic properties so that their role in the physical properties of BLSO films need to be properly understood. The electrical properties and electronic structure of BLSO films grown on SrTiO3 (001) (STO) and BaSnO3 (001) (BSO) substrates are comparatively studied to investigate the effect of the TDs. In the BLSO/STO films with TD density of ~1.32 × 1011 cm-2, n-type carrier density ne and electron mobility are significantly reduced, as compared with the BLSO/BSO films with nearly no TDs. This indicates that TDs play the role of scattering-centers as well as acceptor-centers to reduce n-type carriers. Moreover, in the BLSO/STO films, both binding energies of an Sn 3d core level and a valence band maximum are reduced, being qualitatively consistent with the Fermi level shift with the reduced n-type carriers. However, the reduced binding energies of the Sn 3d core level and the valence band maximum are clearly different as 0.39 and 0.19 eV, respectively, suggesting that the band gap renormalization preexisting in proportion to ne is further suppressed to restore the band gap in the BLSO/STO films with the TDs.
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A complex interplay of different energy scales involving Coulomb repulsion, spin-orbit coupling, and Hund's coupling energy in 2D van der Waals (vdW) material produces a novel emerging physical state. For instance, ferromagnetism in vdW charge transfer insulator CrGeTe_{3} provides a promising platform to simultaneously manipulate the magnetic and electrical properties for potential device implementation using few nanometers thick materials. Here, we show a continuous tuning of magnetic and electrical properties of a CrGeTe_{3} single crystal using pressure. With application of pressure, CrGeTe_{3} transforms from a ferromagnetic insulator with Curie temperature T_{C}â¼66 K at ambient condition to a correlated 2D Fermi metal with T_{C} exceeding â¼250 K. Notably, absence of an accompanying structural distortion across the insulator-metal transition (IMT) suggests that the pressure induced modification of electronic ground states is driven by electronic correlation furnishing a rare example of bandwidth-controlled IMT in a vdW material.
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BACKGROUND: The effects of shoes and foot type on balance are unclear. We aimed to investigate the differences between static and dynamic balance among three foot types and the changes in postural balance while wearing typical athletic shoes. METHODS: Based on the Foot Posture Index, the feet of 39 participants were classified as pronated, neutral, or supinated by a physiatrist. Static and dynamic balance function were assessed by center of gravity (COG) sway velocity with eyes open and eyes closed and a modified Star Excursion Balance Test in a random order with participants either barefoot or wearing shoes. RESULTS: The COG sway velocity was significantly higher in the supinated foot group than in the neutral foot group (barefoot: eyes open, P = .004, eyes closed, P = .001). Normalized composite reach distance (NCRD) was significantly lower in the pronated and supinated foot groups (barefoot: P = .039, P = .008; shoes: P = .018, P = .018). In all three foot type groups, COG sway velocity was significantly decreased (P < .05) and NCRD was significantly increased (P < .05) while wearing typical athletic shoes. CONCLUSIONS: The medial longitudinal arch of the foot affects postural balance. Typical athletic shoes improve postural balance regardless of foot type. However, the pronated and supinated foot groups still had lower dynamic postural balance compared with the neutral foot group, even when wearing athletic shoes. People with pronated and supinated feet may need additional interventions, such as foot orthoses or balance training.
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Órtoses do Pé , Esportes , Pé , Humanos , Equilíbrio Postural , SapatosRESUMO
Realizing a state of matter in two dimensions has repeatedly proven a novel route of discovering new physical phenomena. Van der Waals (vdW) materials have been at the center of these now extensive research activities. They offer a natural way of producing a monolayer of matter simply by mechanical exfoliation. This work demonstrates that the possible multiferroic state with coexisting antiferromagnetic and ferroelectric orders persists down to the bilayer flake of NiI2. By exploiting the optical second-harmonic generation technique, both magnitude and direction of the ferroelectric order, arising from the cycloidal spin order, are successfully traced. The possible multiferroic state's transition temperature decreases from 58 K for the bulk to about 20 K for the bilayer. Our observation will spur extensive efforts to demonstrate multifunctionality in vdW materials, which have been tried mostly by using heterostructures of singly ferroic ones until now.
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Transparent p-CuI/n-SiZnSnO (SZTO) heterojunction diodes are successfully fabricated by thermal evaporation of a (111) oriented p-CuI polycrystalline film on top of an amorphous n-SZTO film grown by the RF magnetron sputtering method. A nitrogen annealing process reduces ionized impurity scattering dominantly incurred by Cu vacancy and structural defects at the grain boundaries in the CuI film to result in improved diode performance; the current rectification ratio estimated at ±2 V is enhanced from ≈106 to ≈107. Various diode parameters, including ideality factor, reverse saturation current, offset current, series resistance, and parallel resistance, are estimated based on the Shockley diode equation. An energy band diagram exhibiting the type-II band alignment is proposed to explain the diode characteristics. The present p-CuI/n-SZTO diode can be a promising building block for constructing useful optoelectronic components such as a light-emitting diode and a UV photodetector.
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In order to understand the superconducting gap nature of a [Formula: see text] single crystal with [Formula: see text], in-plane thermal conductivity [Formula: see text], in-plane London penetration depth [Formula: see text], and the upper critical fields [Formula: see text] have been investigated. At zero magnetic field, it is found that no residual linear term [Formula: see text] exists and [Formula: see text] follows a power-law [Formula: see text] (T: temperature) with n = 2.66 at [Formula: see text], supporting nodeless superconductivity. Moreover, the magnetic-field dependence of [Formula: see text]/T clearly shows a shoulder-like feature at a low field region. The temperature dependent [Formula: see text] curves for both in-plane and out-of-plane field directions exhibit clear upward curvatures near [Formula: see text], consistent with the shape predicted by the two-band theory and the anisotropy ratio between the [Formula: see text](T) curves exhibits strong temperature-dependence. All these results coherently suggest that [Formula: see text] is a nodeless, multiband superconductor.
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OBJECTIVE: To compare postural balance ability in patients with low back pain between groups with and without lumbosacral radiculopathy. METHODS: Patients who were referred for electromyography because of low back pain during the period from April 2017 through June 2018 were chosen as subjects. They were divided into groups with and without lumbosacral radiculopathy based on the results of electromyography. We used Tetrax (Sunlight Medical Ltd., Ramat Gan, Israel) to objectively evaluate postural balance ability, and to measure the fall risk, stability index, weight distribution index, and Fourier index. RESULTS: Patients in the lumbosacral radiculopathy group showed significantly higher fall risk (73.25 vs. 38.00; p<0.05), weight distribution index (8.57 vs. 5.00; p<0.05), and stability index (21.19 vs. 13.16; p<0.05) than those in the group without lumbosacral radiculopathy. The Fourier index at high-medium frequency was significantly increased in the lumbosacral radiculopathy group (8.27 vs. 5.56; p<0.05), whereas weight-bearing on the side of radiculopathy was significantly decreased. CONCLUSION: Patients with lumbosacral radiculopathy have decreased postural balance compared with patients without this condition. Somatosensory disturbances in lumbosacral radiculopathy might cause postural balance impairment. Assessment and treatment plan not only for pain reduction but also for postural balance improvement should be considered in the management of patients with lumbosacral radiculopathy.
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The zero field 53Cr nuclear magnetic resonance was measured at low temperatures to investigate the interactions in the bond-frustrated S = 3/2 Heisenberg helimagnet ZnCr2Se4. A quadratic decrease of the sublattice magnetization was determined from the temperature dependence of the isotropic hyperfine field. We calculated the magnetization using linear spin wave theory for the incommensurate spiral spin order and compared this outcome with experimental results to estimate the coupling constants. The hyperfine fields at Cr and Se ions provide evidences that the spin polarization of Cr ions is transferred to neighboring Se ions due to the covalent bonding between them, resulting in reduced magnetic moment in the Cr ion. This observation indicates that the Jahn-Teller effect, which leads to distortion inducing spin-lattice coupling, is not completely missing in ZnCr2Se4.
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Robot-assisted therapy is an effective treatment for stroke patients and has recently gained popularity. Clinicians and researchers are trying to identify predictors to stratify patients for ensuring better stroke rehabilitation outcomes. However, previous studies have reported controversial results regarding the predictors of upper limb recovery after robot-assisted therapy. Our objective was to determine whether the demographic and clinical characteristics of stroke patients influence the motor and functional outcomes after robot-assisted therapy. We conducted a retrospective analysis of 48 hemiplegic patients who performed upper limb goal-directed tasks using RAPAEL Smart Glove (Neofect, Gyeonggi-do, Republic of Korea). Robot-assisted therapy was administered for 5 days a week over 4 weeks, and each session was for 30 minutes. The parameters of the primary outcomes after robot-assisted therapy were measured with the manual function test and functional independence measure. Correlation analysis showed that age, initial cognitive function, and the initial manual function test and the Modified Ashworth Scale for upper extremity scores were significant factors for independently predicting functional outcomes after robot-assisted therapy. Linear regression analysis revealed that the initial Mini-Mental State Examination (P < 0.001) and initial manual function test (P < 0.001) scores were significant predictors of the primary outcomes. In conclusion, our study suggests that stroke patients presenting with less spasticity, better initial cognitive function, and better initial motor function have a significant correlation with the functional outcomes after robot-assisted therapy.
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Hemiplegia/reabilitação , Robótica , Reabilitação do Acidente Vascular Cerebral/métodos , Extremidade Superior/fisiopatologia , Avaliação da Deficiência , Feminino , Hemiplegia/fisiopatologia , Humanos , Masculino , Testes de Estado Mental e Demência , Pessoa de Meia-Idade , Estudos Retrospectivos , Acidente Vascular Cerebral/fisiopatologiaRESUMO
Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and 75As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na1-xLi x FeAs; For x ≤ 0.02, the nematic transition promotes SFs. In contrast, for x ≥ 0.03, the system undergoes a non-magnetic phase transition at a temperature T0 into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.
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OBJECTIVE: To investigate the relationship between functional level and muscle thickness (MT) of the rectus femoris (RF) and the gastrocnemius (GCM) in young children with cerebral palsy (CP). METHODS: The study participants were comprised of 26 children (50 legs) with spastic CP, aged 3-6 years, and 25 age-matched children with typical development (TD, 50 legs). The MT of the RF, medial GCM, and lateral GCM was measured with ultrasound imaging. The functional level was evaluated using the Gross Motor Function Measurement-88 (GMFM-88), Gross Motor Function Classification System (GMFCS), and based on the mobility area of the Korean version of the Modified Barthel Index (K-MBI). The measurement of spasticity was evaluated with the Modified Ashworth Scale (MAS). RESULTS: We note that the height, weight, body mass index, and MT of the RF, and the medial and lateral GCM were significantly higher in the TD group (p<0.05). There was a direct relationship between MT of the RF and medial GCM and the GMFM-88, GMFCS, and mobility scores of the K-MBI in individuals with early CP. In addition, we have noted that there was a direct relationship between MT of the lateral GCM and the GMFM-88 and GMFCS. Although there was a tendency toward lower MT with increasing MAS ratings in the knee and ankle, the correlation was not statistically significant. CONCLUSION: In young children with CP, MT of the RF and GCM was lower than in age-matched children with TD. Furthermore, it is noted with confidence that a significant positive correlation existed between MT and functional level as evaluated using the GMFM-88, GMFCS, and mobility area of K-MBI.
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An electromagnon in the magnetoelectric (ME) hexaferrite Ba_{0.5}Sr_{2.5}Co_{2}Fe_{24}O_{41} (Co_{2}Z-type) single crystal is identified by time-domain terahertz (THz) spectroscopy. The associated THz resonance is active on the electric field (E^{ω}) of the THz light parallel to the c axis (⥠[001]), whose spectral weight develops at a markedly high temperature, coinciding with a transverse conical magnetic order below 410 K. The resonance frequency of 1.03 THz at 20 K changes -8.7% and +5.8% under external magnetic field (H) of 2 kOe along [001] and [120], respectively. A model Hamiltonian describing the conical magnetic order elucidates that the dynamical ME effect arises from antiphase motion of spins which are coupled with modulating electric dipoles through the exchange striction mechanism. Moreover, the calculated frequency shift points to the key role of the Dzyaloshinskii-Moriya interaction that is altered by static electric polarization change under different H.
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We investigate the pressure and thermal annealing effects on BaFe2-x Co x As2 (Co-Ba122) single crystals with x = 0.1 and 0.17 via electrical transport measurements. The thermal annealing treatment not only enhances the superconducting transition temperature (T c) from 9.6 to 12.7 K for x = 0.1 and from 18.1 to 21.0 K for x = 0.17, but also increases the antiferromagnetic transition temperature (T N). Simultaneous enhancement of T c and T N by the thermal annealing treatment indicates that thermal annealing could substantially improve the quality of the Co-doped Ba122 samples. Interestingly, T c of the Co-Ba122 compounds shows a scaling behavior with a linear dependence on the resistivity value at 290 K, irrespective of tuning parameters such as chemical doping, pressure, and thermal annealing. These results not only provide an effective way to access the intrinsic properties of the BaFe2As2 system, but may also shed a light on designing new materials with higher superconducting transition temperature.