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[This corrects the article DOI: 10.1039/C4CE02347A.].
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Orthodontic tooth movement (OTM) is generated by a mechanical force that induces an aseptic inflammatory response in the periodontal tissues and a subsequent coordinated process of bone resorption and apposition. In this review, we critically summarize the current knowledge on the immune processes involved in OTM inflammation and provide a novel insight into the relationship between classical inflammation and clinical OTM phases. We found that most studies focused on the acute inflammatory process, which ignites the initial alveolar bone resorption. However, the exact mechanisms and the immune reactions involved in the following OTM phases remain obscure. Recent studies highlight the existence of a typical innate response of resident and extravasated immune cells, including granulocytes and natural killer (NK), dendritic, and γδT cells. Based on few available studies, we shed light on an active, albeit incomplete, process of resolution in the lag phase, supported by continuously elevated ratios of M1/M2 macrophage and receptor activator of nuclear factor κB ligand/osteoprotegerin ratio. This partial resolution enables tissue formation and creates the appropriate environment for a transition between the innate and adaptive arms of the immune system, essential for the tissue's return to homeostasis. Nevertheless, as the mechanical trigger persists, the resolution turns into a low-grade chronic inflammation, which underlies the next, acceleration/linear OTM phase. In this stage, the acute inflammation dampens, and a simultaneous process of bone resorption and formation occurs, driven by B and T cells of the adaptive immune arm. Excessive orthodontic forces or tooth movement in periodontally affected inflamed tissues may hamper resolution, leading to "maladaptive homeostasis" and tissue loss due to uncoupled bone resorption and formation. The review ends with a brief description of the translational studies on OTM immunomodulation. Future studies are necessary for further uncovering cellular and molecular immune targets and developing novel strategies for controlling OTM by local and sustained tuning of the inflammatory process.
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Pérdida de Hueso Alveolar , Técnicas de Movimiento Dental , Remodelación Ósea , Humanos , Inflamación , Macrófagos , Osteoclastos , PeriodoncioRESUMEN
We demonstrate experimentally the ability to use a single-pixel detector for two-dimensional high-resolution x-ray imaging of fast dynamics. We image the rotation of a spinning chopper at 100 kHz and at spatial resolution of about 40 microns by using the computational ghost imaging approach. The technique we develop can be used for the imaging of fast dynamics of periodic and periodically stimulated effects with a large field of view and at low dose.
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The current study aimed at investigating the long-term biological mechanisms governing bone regeneration in osseous defects filled with bovine bone (BB). Tooth extraction sockets were filled with BB or left unfilled for natural healing in a C57BL/6 mouse alveolar regeneration bone model (n = 12). Seven weeks later, the alveolar bone samples were analyzed histologically with hematoxylin/eosin and tartrate-resistant acid phosphatase staining. A separate group (n = 10) was used for RNA sequencing. Osteoclast inhibition was induced by zoledronic acid (ZA) administration at 2 wk postextraction in a third group (n = 28) for examination of osseous changes and cellular functions with micro-computed tomography and quantitative reverse transcription polymerase chain reaction, respectively. Histological and radiological osseous healing was observed in both BB-filled and normal-healing sockets. However, BB regenerated bone showed significant robust expression of genes associated with bone homeostasis and osteoclasts' function. Osteoclasts' inhibition in BB-filled sockets led to decreased bone resorption markers and reduced bone formation to a greater extent than that observed in osteoclasts' inhibition with natural healing. BB displays long-term biologically active properties, despite a naive osseous histological appearance. These include activation of osteoclasts, which in turn promotes osseous remodeling and maturation of ossified bone.
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Osteoclastos , Animales , Huesos , Bovinos , Ratones , Ratones Endogámicos C57BL , Fosfatasa Ácida Tartratorresistente , Alveolo Dental/diagnóstico por imagen , Microtomografía por Rayos XRESUMEN
Five coordination polymers formed from combinations of copper(II) acetate and 4'-(4-alkyloxyphenyl)-3,2':6',3''-terpyridines with methoxy (1), n-butoxy (2), n-pentyloxy (3) and n-heptyloxy (4) substituents are reported. Reaction of 1 with Cu(OAc)2âH2O leads to the 1D-polymer [Cu2(µ-OAc)4(1)]n in which {Cu2(ï-OAc)4} paddle-wheel units are connected by ligands 1, or [{Cu4(µ3-OH)2(µ-OAc)2(µ3-OAc)2(AcO-κO)2(1)2}.2MeOH]n in which centrosymmetric tetranuclear clusters link pairs of ligands 1 to give a double-stranded 1D-polymer. Layering solutions of Cu(OAc)2âH2O (in MeOH) over 2, 3 or 4 (in CHCl3) leads to the assembly of the 1D-polymers [2{Cu2(µ-OAc)4(2)}.1.25MeOH]n, [Cu2(µ-OAc)4(3)]n and [{Cu2(µ-OAc)4(4)}.0.2CHCl3]n. In all compounds, the 3,2':6',3''-tpy unit coordinates only through the outer pyridine rings, but the conformation of the 3,2':6',3''-tpy responds to changes in the length of the alkyloxy tails leading to changes in the conformation of the polymer backbone and in the packing of the chains in the crystal lattice in the chains featuring {Cu2(ï-OAc)4} paddle-wheel linkers.
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We wish to make the following corrections to our published paper [...].
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The synthesis and characterization of 4'-(4-methoxyphenyl)-3,2':6',3â³-terpyridine (2) (IUPAC PIN 24-(4-methoxyphenyl)-12,22:26,32-terpyridine) are described, and its coordination behaviour with cobalt(II) thiocyanate has been investigated. In a series of experiments, crystals were grown at room temperature by layering a MeOH solution of Co(NCS)2 over a CHCl3 solution of 2 using 1:1, 1:2 or 2:1 molar ratios of metal salt-to-ligand. Crystals harvested within 2-3 weeks proved to be the 1D-coordination polymer [Co(2)(NCS)2(MeOH)2]n and powder X-ray diffraction (PXRD) confirmed that the crystals selected for single-crystal X-ray diffraction were representative of the bulk samples. Longer crystallization times with a Co(NCS)2 to 2 molar ratio of 1:1 yielded crystals of [Co(2)(NCS)2(MeOH)2]n (1D-chain) and the pseudopolymorphs [{Co(2)2(NCS)2}·3MeOH]n and [{Co(2)2(NCS)2}·2.2CHCl3]n ((4,4)-nets), each type of crystal originating from a different zone in the crystallization tube. PXRD for this last experiment confirmed that the dominant product in the bulk sample was the 1D-coordination polymer.
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By means of a specific heat (C) and electrical resistivity ([Formula: see text]) study, we give evidence of a pronounced Fermi liquid (FL) behavior with sizable mass renormalization, [Formula: see text], up to unusually high temperatures â¼70 K in the layered system (Cu2/3V1/3)V2S4. At low temperature, a marked upturn of both C and [Formula: see text] is suppressed by magnetic field, which suggests a picture of Kondo coupling between conduction electrons in the VS2 layers and impurity spins of the V3+ ions located between layers. This picture opens the possibility of controlling electronic correlations and the FL to non-FL crossover in simple layered materials. For instance, we envisage that the coupling between layers provided by the impurity spins may realize a two-channel Kondo state.
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We probe the effect of heteroatom substitution on the spin crossover (SCO) properties of dinuclear materials of the type [Fe2(NCX)4(R-trz)5]·S (X = S, Se; S = solvent; R-trz = (E)-N-(furan-2-ylmethylene)-4H-1,2,4-triazol-4-amine (furtrz); (E)-N-(thiophen-2-ylmethylene)-4H-1,2,4-triazole-4-amine (thtrz)). For the furtrz family ([Fe2(NCX)4(furtrz)5]·furtrz·MeOH; X = S (furtrz-S) and X = Se (furtrz-Se)) gradual and incomplete one-step SCO transitions are observed (furtrz-S (T1/2 = 172 K) and furtrz-Se (T1/2 = 205 K)) and a structural evolution from [HS-HS] to [HS-LS] per dinuclear species. Contrasting this, within the thtrz family ([Fe2(NCX)4(thtrz)5]·4MeOH; X = S (thtrz-S) and X = Se (thtrz-Se)) more varied SCO transitions are observed, with thtrz-S being SCO-inactive (high spin) and thtrz-Se showing a rare complete two-step SCO transition (T1/2(1,2) = 170, 200 K) in which the FeII sites transition from [HS-HS] to [HS-LS] to [LS-LS] per dinuclear unit with no long range ordering of spin-states at the intermediate plateau. Detailed structure-function analyses have been conducted within this growing dinuclear family to rationalise these diverse spin-switching properties.
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We demonstrate computational ghost imaging at X-ray wavelengths with only one single-pixel detector. We show that, by using a known designed mask as a diffuser that induces intensity fluctuations in the probe beam, it is possible to compute the propagation of the electromagnetic field in the absence of the investigated object. We correlate these calculations with the measured data when the object is present in order to reconstruct the images of 50 µm and 80 µm slits. Our results open the possibilities for X-ray high-resolution imaging with partially coherent X-ray sources and can lead to a powerful tool for X-ray three-dimensional imaging.
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Cycles of Cdc53/Cullin1 rubylation (a.k.a NEDDylation) protect ubiquitin-E3 SCF (Skp1-Cullin1-F-box protein) complexes from self-destruction and play an important role in mediating the ubiquitination of key protein substrates involved in cell cycle progression, development, and survival. Cul1 rubylation is balanced by the COP9 signalosome (CSN), a multi-subunit derubylase that shows 1:1 paralogy to the 26S proteasome lid. The turnover of SCF substrates and their relevance to various diseases is well studied, yet, the extent by which environmental perturbations influence Cul1 rubylation/derubylation cycles per se is still unclear. In this study, we show that the level of cellular oxidation serves as a molecular switch, determining Cullin1 rubylation/derubylation ratio. We describe a mutant of the proteasome lid subunit, Rpn11 that exhibits accumulated levels of Cullin1-Rub1 conjugates, a characteristic phenotype of csn mutants. By dissecting between distinct phenotypes of rpn11 mutants, proteasome and mitochondria dysfunction, we were able to recognize the high reactive oxygen species (ROS) production during the transition of cells into mitochondrial respiration, as a checkpoint of Cullin1 rubylation in a reversible manner. Thus, the study adds the rubylation cascade to the list of cellular pathways regulated by redox homeostasis.
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Proteínas Cullin/metabolismo , Mitocondrias/metabolismo , Complejo de la Endopetidasa Proteasomal/metabolismo , Estrés Fisiológico , Respiración de la Célula , Mitocondrias/genética , Modelos Biológicos , Especies Reactivas de Oxígeno/metabolismo , Enzimas Activadoras de Ubiquitina/metabolismo , UbiquitinaciónRESUMEN
In this study we exploit the flexible nature of porous coordination polymers (PCPs) with integrated spin crossover (SCO) properties to manipulate the multistability of spin-state switching profiles. We previously reported the two-dimensional Hofmann-type framework [Fe(thtrz)2Pd(CN)4]·EtOH,H2O (1·EtOH,H2O), N-thiophenylidene-4 H-1,2,4-triazol-4-amine), displaying a distinctive two-step SCO profile driven by extreme elastic frustration. Here, we reveal a reversible release mechanism for this elastic frustration via stepwise guest removal from the parent phase (1·EtOH,H2O â 1·H2O â 1·Ø). Parallel variable temperature structural and magnetic susceptibility measurements reveal a synergistic framework flexing and "on-off" switching of multistep SCO character concomitant with the onset of guest evacuation. In particular, the two-step SCO properties in 1·EtOH,H2O are deactivated such that both the partially solvated (1·H2O) and desolvated (1·Ø) phases show abrupt and hysteretic one-step SCO behaviors with differing transition temperatures (1·H2O: T1/2↓: 215 T1/2↑: 235 K; 1·Ø: T1/2↓: 170 T1/2↑: 182 K). This "on-off" elastic frustration switching is also reflected in the light-induced excited spin state trapping (LIESST) properties of 1·EtOH,H2O and 1·Ø, with nonquantitative (ca. 50%, i.e., LS â 1:1 HS:LS) and quantitative (ca. 100%, LS â HS) photoinduced spin state conversion achieved under light irradiation (510 nm at 10 K), respectively. Conversely, the two-step SCO properties are retained in the water saturated phase 1·3H2O but with a subtle shift in transition temperatures. Comparative analysis of this and related materials reveals the distinct roles that indirect and direct guest interactions play in inducing, stabilizing, and quantifying elastic frustration and the importance of lattice flexibility in these porous framework architectures.
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A comparative investigation of crystal growth from solution and on-surface assembly in vacuo between copper and three 4'-(2-R-pyrimidin-5-yl)-4,2':6',4''-terpyridines, with R = H (1), Me (2), or Et (3), is presented. In solution, ligand 3 combines with copper(II) acetate or copper(I) triflate in MeOH solution to give [Cu2(OAc)4(3)]n or {[Cu(3)(OMe)(MeOH)][CF3SO3]·MeOH}n. In [Cu2(OAc)4(3)]n, paddle-wheel {Cu2(µ-OAc)4} nodes direct the assembly of one-dimensional (1D) zigzag chains which pack into two-dimensional (2D) sheets. In {[Cu(3)(OMe)(MeOH)][CF3SO3]·MeOH}n, the solvent is a ligand and also generates {Cu2(µ-OMe)2} units which function as planar 4-connecting nodes to generate a 2D (4,4) net with ligand 3. On Au(111) or Cu(111) surfaces in vacuo, no additional solvent or anions are involved in the assembly. The different substituents in 1, 2, or 3 allow precise molecular resolution imaging in scanning tunneling microscopy. On Au(111), 1 and 2 assemble into close-packed assemblies, while 3 forms a regular porous network. The deposition of Cu adatoms results in reorganization leading to ladder-shaped surface metal-organic motifs. These on-surface coordination assemblies are independent of the 4'-substituent in the 4,2':6',4''-tpy and are reproduced on Cu(111) where Cu adatoms are available during the deposition and relaxation process at room temperature. Upon annealing at elevated temperatures, the original surface assemblies of 1 and 3 are modified and a transition from ladders into rhomboid structures is observed; for 2, a further quasi-hexagonal nanoporous network is observed.
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The syntheses and characterizations of three new ligands containing two 4,2':6',4â³-tpy or two 3,2':6',3â³-tpy metal-binding domains are reported. The ligands possess different alkyloxy functionalities attached to the central phenylene spacer: n-pentyloxy in 3, 4-phenyl-n-butoxy in 4, benzyloxy in 5. Crystal growth under ambient conditions has led to the formation of {[Co(NCS)2(3)]·0.8C6H4Cl2}n and {[Co(NCS)2(4)]·1.6H2O·1.2C6H4Cl2}n, with structures confirmed by single crystal X-ray diffraction. Both the cobalt(II) center and ligand 3 or 4 act as 4-connecting nodes and both {[Co(NCS)2(3)]·0.8C6H4Cl2}n and {[Co(NCS)2(4)]·1.6H2O·1.2C6H4Cl2}n possess a 3D cds net despite the fact that 3 and 4 contain two 4,2':6',4â³-tpy and two 3,2':6',3â³-tpy units, respectively. Taken in conjunction with previously reported data, the results indicate that the role of the alkyloxy substituent is more significant than the choice of 4,2':6',4â³- or 3,2':6',3â³-tpy isomer in determining the assembly of a particular 3D net. The combination of Co(NCS)2 with 5 resulted in the formation of the discrete molecular complex [Co(NCS)2(MeOH)2(5)2]·2CHCl3·2MeOH in which 5 acts as a monodentate ligand. The pendant phenyls and both coordinated and non-coordinated 4,2':6',4â³-tpy units are involved in efficient π-stacking interactions.
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A comparative investigation of the coordination assemblies formed between Co(NCS)2 and two monotopic 4,2':6',4''-terpyridine (4,2':6',4"-tpy) ligands or two related ditopic ligands is reported. Crystals were grown by layering MeOH solutions of Co(NCS)2 over a CHCl3 or 1,2-C6H4Cl2 solution of the respective ligand at room temperature. With 4'-(2-methylpyrimidin-5-yl)-4,2':6',4"-terpyridine (6), the 1D-coordination polymer {[Co2(NCS)4(MeOH)4(6)2]â2MeOHâ8H2O}n assembles with 6 coordinating only through the outer N-donors of the 4,2':6',4"-tpy unit; coordination by the MeOH solvent blocks two cobalt coordination sites preventing propagation in a higher-dimensional network. A combination of Co(NCS)2 and 1-(4,2':6',4"-terpyridin-4'-yl)ferrocene (7) leads to {[Co(NCS)2(7)2]â4CHCl3}n which contains a (4,4) net; the 2D-sheets associate through π-stacking interactions between ferrocenyl and pyridyl units. A 3D-framework is achieved through use of the ditopic ligand 1,4-bis(npropoxy)-2,5-bis(4,2':6',4"-terpyridin-4'-yl)benzene (8) which acts as a 4-connecting node in {[Co(NCS)2(8)2].2C6H4Cl2}n; the combination of metal and ligand planar 4-connecting nodes results in a {65.8} cds net. For a comparison with the coordinating abilities of the previously reported 1,4-bis(noctoxy)-2,5-bis(4,2':6',4"-terpyridin-4'-yl)benzene (3), a more flexible analogue 9 was prepared. {[Co(NCS)2(9)]â2CHCl3}n contains a (4,4) net defined by both metal and ligand planar 4-connecting nodes. The noctoxy tails of 9 protrude from each side of the (4,4) net and thread through adjacent sheets; the arene-attached noctoxy chains associate through a combination of van der Waals and C-H...π interactions.
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With the aim of improving the photoconversion efficiencies of heteroleptic [Cu(Lanchor)(Lancillary)](+) dyes in n-type dye-sensitized solar cells (DSCs), the previously favoured anchor ((6,6'-dimethyl-[2,2'-bipyridine]-4,4'-diyl)bis(4,1-phenylene))bis(phosphonic acid) (1) has been replaced by analogues 2 and 3 containing 2-thienyl spacers between the 2,2'-bipyridine metal-binding domain and the phosphonic acid anchoring groups. The synthesis and characterization of 2 and 3 (2-thienyl spacer with phosphonic acid in the 5- and 4-positions, respectively) are reported. A stepwise, on-surface method was used to assemble [Cu(Lanchor)(Lancillary)](+) dyes onto FTO/TiO2 electrodes with Lanchor = 1, 2 or 3, and Lancillary = 6,6'-bis(trifluoromethyl)-2,2'-bipyridine (4), 6-trifluoromethyl-2,2'-bipyridine (5), 6,6'-dimethyl-2,2'-bipyridine (6), and 6-methyl-2,2'-bipyridine (7). Changing the solvent in the dye-bath from CH2Cl2 to acetone had only a small effect on the photoconversion efficiencies of [Cu(1)(4)](+), [Cu(1)(5)](+) and [Cu(1)(6)](+); the optimal dye in this series was [Cu(1)(5)](+). Comparable DSC performances were achieved by using either anchor 1 or 2, but there is improved electron injection if the phosphonic acid group is in the 4- rather than 5-position of the thienyl ring (i.e. anchor 3 is superior to 2). Similar open-circuit voltages (VOC) are achieved on going from 1 to 3 with a given Lancillary; although there is typically a gain in short-circuit current denisty (JSC) on going from 1 or 3 to 2, there is an ≈50-60 mV drop in VOC on introducing 2 as the anchor. The best photoconversion efficiencies are obtained for the dye [Cu(3)(5)](+) (η = 2.40% relative to an N719 reference of 5.76%). The conclusions reached from plots of current-density (J) against potential (V), and external quantum efficiency spectra are supported by electrochemical impedance spectroscopic measurements.
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The recently discovered metal-malonate compounds of formulae Na2M(H2C3O4)2·2H2O with M = Mn, Fe, Co, Ni are investigated for their magnetic properties. While the Cu-based material is a weak ferromagnet, all other members present antiferromagnetic interactions. Neutron powder diffraction experiments reveal the establishment of a long range magnetic order at low temperature in the Pbca Shubnikov magnetic group. The magnetic structures are characterized by antiferromagnetic layers perpendicular to [001]. These layers are stacked antiparallel (M = Fe) or parallel (M = Mn, Ni) in the (a, c) plane. Magnetic moments are collinear to b for the former and to c for the latter. The M = Co malonate exhibits a non-collinear magnetic structure intermediate between the two latter, with components along b and c. Density functional theory calculations indicate that the dominant magnetic interaction, J1, occurs along a malonate group via a carboxylate and links two transition metals within the same layer, while other interactions (inter- or intra-layer) are much weaker, so that these compounds present the dominant characteristics of 2D-antiferromagnets.
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BACKGROUND: According to the World Health Organization, over one million people die annually from traffic crashes, in which over half are pedestrians, bicycle riders and two-wheel motor vehicles. In Israel, during the last decade, mortality from traffic crashes has decreased from 636 in 1998 to 288 in 2011. Professionals attribute the decrease in mortality to enforcement, improved infrastructure and roads and behavioral changes among road users, while no credit is given to the trauma system. Trauma systems which care for severe and critical casualties improve the injury outcomes and reduce mortality among road casualties. GOALS: 1) To evaluate the contribution of the Israeli Health System, especially the trauma system, on the reduction in mortality among traffic casualties. 2) To evaluate the chance of survival among hospitalized traffic casualties, according to age, gender, injury severity and type of road user. METHODS: A retrospective study based on the National Trauma Registry, 1998-2011, including hospitalization data from eight hospitals. OUTCOMES: During the study period, the Trauma Registry included 262,947 hospitalized trauma patients, of which 25.3% were due to a road accident. During the study period, a 25% reduction in traffic related mortality was reported, from 3.6% in 1998 to 2.7% in 2011. Among severe and critical (ISS 16+) casualties the reduction in mortality rates was even more significant, 41%; from 18.6% in 1998 to 11.0% in 2011. Among severe and critical pedestrian injuries, a 44% decrease was reported (from 29.1% in 1998 to 16.2% in 2011) and a 65% reduction among bicycle injuries. During the study period, the risk of mortality decreased by over 50% from 1998 to 2011 (OR 0.44 95% 0.33-0.59. In addition, a simulation was conducted to determine the impact of the trauma system on mortality of hospitalized road casualties. Presuming that the mortality rate remained constant at 18.6% and without any improvement in the trauma system, in 2011 there would have been 182 in-hospital deaths compared to the actual 108 traffic related deaths. A 41% difference was noted between the actual number of deaths and the expected number. CONCLUSIONS: This study clearly shows that without any improvement in the health system, specifically the trauma system, the number of traffic deaths would be considerably greater. Although the health system has a significant contribution on reducing mortality, it does not receive the appropriate acknowledgment or resources for its proportion in the fight against traffic accidents.
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Accidentes de Tránsito/mortalidad , Investigación sobre Servicios de Salud , Centros Traumatológicos/organización & administración , Heridas y Lesiones/terapia , Accidentes de Tránsito/estadística & datos numéricos , Adolescente , Adulto , Anciano , Niño , Preescolar , Femenino , Hospitalización , Humanos , Lactante , Recién Nacido , Israel , Masculino , Persona de Mediana Edad , Sistema de Registros , Estudios Retrospectivos , Análisis de Supervivencia , Resultado del Tratamiento , Heridas y Lesiones/epidemiología , Adulto JovenRESUMEN
The abrupt and hysteretic two-step spin crossover in a new triazole-based 2-D Hofmann-type complex shows a record breaking 120 K intermediate plateau (IP) region stabilized by negative cooperative interactions.
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We report on the high-pressure synthesis, structural study and physical properties of a new layered compound, Sr3V5S11. Single-crystals of ~0.3 mm size were synthesized at the optimized growth conditions of 6 GPa and 1600 ° C. The refinement of x-ray diffraction data indicates that the crystal structure is monoclinic (space group C2/c), with cell parameters a = 8.7165(7) Å, b = 15.1096(13) Å, c = 23.111(2) Å, and ß = 98.734(9). The structure consists of a stacking of VS2 layers with a CdI2-type structure within the ab-plane connected by trimers of face-sharing VS6 octahedra oriented along the out-of-plane direction. Salient features are a 4 + valence of the V ions in the planes and a 3 + valence in the trimers and a large stripe-like modulation of the V-V distances in the planes leading to quasi-one-dimensional properties. The magnetic susceptibility displays a large temperature-independent contribution, χ0, in addition to a moderate Curie-Weiss term. In the 300-120 K range, the electrical resistivity is described well by a semiconducting-like behaviour with a room-temperature value of ~1.2-10 mΩ cm and a modest activation energy of ~13.5 meV. At lower temperatures, a crossover to a one-dimensional variable range hopping regime is observed, supporting a scenario of a correlated 1D system.