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1.
Adv Mater ; 33(39): e2103000, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34397123

RESUMO

The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm-2 , 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge-spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge-spin-lattice decoupling to activate and subsequently stabilize nonequilibrium phase. The cooperativity triggered by ultrahigh-strain-rate (above 106 s- 1 ) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.

2.
Eye Contact Lens ; 47(8): 442-444, 2021 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-33900215

RESUMO

OBJECTIVES: Decreased blink rate during video display viewing (VDV) has been reported; however, patients with tear dysfunction often complain of more frequent blinking. The objectives were to compare blink rates during conversation and VDV in normal and dry eyes and correlate blink rates with signs and symptoms. METHODS: Blink rate was measured with an infrared blink sensor for 2 minutes during conversation and for 2 minutes while watching a video clip (VDV) in patients without dry eye disease (control, n=18) and in patients with tear dysfunction from meibomian gland dysfunction (MGD, n=23), conjunctivochalasis (CCh, n=19), and aqueous tear deficiency (n=34; non-Sjögren syndrome n=18 and Sjögren syndrome n=16). Patients completed visual analogue questionnaires assessing irritation frequency and severity and blink frequency and underwent an ocular surface evaluation. Group comparisons and correlations were calculated. RESULTS: Compared with control, conversational and VDV blink rates were significantly higher in CCh and aqueous tear deficiency (P≤0.005). Self-reported blink frequency was higher in all tear dysfunction groups compared with control. The VDV blink rate was significantly lower than the conversation blink rate in the control group (P=0.006) but not in any of the tear dysfunction groups. Conversational and VDV blink rates were significantly correlated with irritation frequency and severity. CONCLUSIONS: Blink rate decreases during VDV in normal eyes; however, this blink rate suppression was not observed in patients with tear dysfunction, perhaps because of their irritation symptoms or tear instability.


Assuntos
Síndromes do Olho Seco , Ceratoconjuntivite Seca , Disfunção da Glândula Tarsal , Piscadela , Síndromes do Olho Seco/diagnóstico , Humanos , Glândulas Tarsais , Lágrimas
3.
Nano Lett ; 2021 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-33886320

RESUMO

Magnetoelectrics are witnessing an ever-growing success toward the voltage-controlled magnetism derived from inorganic materials. However, these inorganic materials have predominantly focused on the ferroelectromagnetism at solid-to-solid interfaces and suffered several drawbacks, including the interface-sensitive coupling mediators, high-power electric field, and limited chemical tunability. Here, we report a promising design strategy to shift the paradigm of next-generation molecular magnetoelectrics, which relies on the integration between molecular magnetism and electric conductivity though an in situ cross-linking strategy. Following this approach, we demonstrate a versatile and efficient synthesis of flexible molecular-based magnetoelectronics by cross-linking of magnetic coordination networks that incorporate conducting chain building blocks. The as-grown compounds feature an improved critical temperature up to 337 K and a room-temperature magnetism control of low-power electric field. It is envisaged that the cross-linking of molecular interfaces is a feasible method to couple and modulate magnetism and electron conducting systems.

5.
Struct Dyn ; 7(3): 034305, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32637460

RESUMO

Understanding guest exchange processes in metal-organic frameworks is an important step toward the rational design of functional materials with tailor-made properties. The dehydration of the flexible metal-organic framework [Co(AIP)(bpy)0.5(H2O)]•2H2O was studied by novel in situ dynamic x-ray diffraction techniques. The complex mechanism of dehydration, along with the as-yet unreported metastable structures, was determined. The structural information obtained by the application of these techniques helps to elucidate the important guest-host interactions involved in shaping the structural landscape of the framework lattice and to highlight the importance of utilizing this technique in the characterization of functional framework materials.

6.
Molecules ; 25(11)2020 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-32516980

RESUMO

Photochromic compounds have a lengthy history of study and a profusion of applications that stand to gain from these studies. Among the classes of photochromic compounds, diarylethenes show desirable properties including high fatigue resistance and thermal stability, thus meeting some of the most important criteria necessary to enter the realm of practical applications. Recently, photochromic diarylethenes containing quinone functionalities have demonstrated interesting optical and solid-state properties. When properly interfaced with suitable electron withdrawing groups on the aryl component, both the ring-opening and ring-closing reactions can be achieved with visible light; this is in contrast to most other diarylethenes where UV light is required for ring closure. Unfortunately, quantitative conversion from open to closed forms is not possible. In this work, we examine the relative energies of conformations of solid-state structures observed by X-ray crystallography and evaluate their thermal stabilities based on density functional theory (DFT) calculations. Time-dependent DFT (TD-DFT) is used to model the UV-vis absorption spectra of these quinone diarylethenes. We show that spectral overlap between open and closed forms is a major hindrance to full photoconversion.


Assuntos
Química Computacional , Cristalografia por Raios X , Etilenos/química , Naftoquinonas/química , Luz , Conformação Molecular , Estrutura Molecular , Processos Fotoquímicos , Raios Ultravioleta
7.
Molecules ; 25(10)2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32414058

RESUMO

Complexes of Fe(III) that contain a triazacyclononane (TACN) macrocycle, two pendant hydroxyl groups, and a third ancillary pendant show promise as MRI contrast agents. The ancillary group plays an important role in tuning the solution relaxivity of the Fe(III) complex and leads to large changes in MRI contrast enhancement in mice. Two new Fe(III) complexes, one with a third coordinating hydroxypropyl pendant, Fe(L2), and one with an anionic non-coordinating sulfonate group, Fe(L1)(OH2), are compared. Both complexes have a deprotonated hydroxyl group at neutral pH and electrode potentials representative of a stabilized trivalent iron center. The r1 relaxivity of the Fe(L1)(OH2) complex is double that of the saturated complex, Fe(L2), at 4.7 T, 37 °C in buffered solutions. However, variable-temperature 17O-NMR experiments show that the inner-sphere water of Fe(L1)(OH2) does not exchange rapidly with bulk water under these conditions. The pendant sulfonate group in Fe(L1)(OH2) confers high solubility to the complex in comparison to Fe(L2) or previously studied analogues with benzyl groups. Dynamic MRI studies of the two complexes showed major differences in their pharmacokinetics clearance rates compared to an analogue containing a benzyl ancillary group. Rapid blood clearance and poor binding to serum albumin identify Fe(L1)(OH2) for development as an extracellular fluid contrast agent.


Assuntos
Meios de Contraste , Compostos Férricos , Compostos Macrocíclicos , Imageamento por Ressonância Magnética , Animais , Meios de Contraste/química , Meios de Contraste/farmacocinética , Meios de Contraste/farmacologia , Compostos Férricos/química , Compostos Férricos/farmacocinética , Compostos Férricos/farmacologia , Compostos Macrocíclicos/química , Compostos Macrocíclicos/farmacocinética , Compostos Macrocíclicos/farmacologia , Camundongos , Camundongos Endogâmicos BALB C
8.
Sci Rep ; 10(1): 2933, 2020 02 19.
Artigo em Inglês | MEDLINE | ID: mdl-32076085

RESUMO

To compare goblet cell (GC) number and area in the covered superior (SB) versus exposed temporal (TB) bulbar conjunctiva in control versus aqueous tear deficient eyes (ATD) and evaluate correlation with tear MUC5AC protein. SB and TB impression cytology performed on control eyes, Sjögren syndrome (SS) ATD, and non-SS ATD was stained with period acid Schiff. GC number and area were measured with image analysis software. Protein-normalized MUC5AC level was measured in Schirmer strip-collected tears. Compared to control conjunctiva, GC number and area were significantly lower in SS, non-SS, and combined ATD groups in exposed TB, and were also significantly lower in SS and combined ATD groups in covered SB. In all ATD, GC number and area were significantly correlated, but differences between SB and TB were non-significant. Normalized tear MUC5AC protein was lower in all ATD groups versus control eyes, and correlated only with GC area. GCs are significantly decreased in the covered and exposed conjunctiva in SS. GC area may be a better disease measure than number for ATD. Correlation between tear MUC5AC concentration and GC area suggests tear MUC5AC mucin can be used as a disease-relevant biomarker for conjunctiva GC health.


Assuntos
Síndromes do Olho Seco/metabolismo , Síndromes do Olho Seco/patologia , Células Caliciformes/metabolismo , Células Caliciformes/patologia , Mucina-5AC/metabolismo , Lágrimas/metabolismo , Adulto , Idoso , Estudos de Casos e Controles , Contagem de Células , Feminino , Humanos , Masculino , Pessoa de Meia-Idade
9.
J Org Chem ; 85(4): 2646-2653, 2020 02 21.
Artigo em Inglês | MEDLINE | ID: mdl-31896258

RESUMO

Diarylethene photochromes show promise for use in advanced organic electronic and photonic materials with burgeoning considerations for biological applications; however, these compounds typically require UV light for photoswitching in at least one direction, thus limiting their appeal. We here introduce a naphthoquinone-based diarylethene that switches between open and closed forms with visible light. The synthesis of this quinone diarylethene relies on Suzuki methodology, allowing for the inclusion of functional groups not otherwise accessible with current synthetic routes.

10.
Am J Ophthalmol ; 210: 86-96, 2020 02.
Artigo em Inglês | MEDLINE | ID: mdl-31647931

RESUMO

PURPOSE: Noncompliance during prospective studies can bias results and limit conclusions. The current study retrospectively investigated the relationship between study subject characteristics and rates of noncompliance in interventional trials involving common causes of blindness. DESIGN: Retrospective analysis of 10 randomized clinical trials. METHODS: Subjects were enrolled in investigator-initiated trials studying proliferative diabetic retinopathy, neovascular age-related macular degeneration, diabetic macular edema, and retinal venous occlusive disease. Records were reviewed for hypothesized risk factors of noncompliance and rates of noncompliance, which were defined as at least 1 missed visit or exiting the study early. Demographic information, systemic medical history, and ocular medical history, including visual acuity and central retinal thicknesses, were examined retrospectively using Student t test, Pearson χ2 test, and logistic regression. RESULTS: Of 390 subjects included, 212 (54.4%) were compliant with all scheduled study visits and 178 (45.6%) met criteria for noncompliance, with 53 (13.6%) subjects exiting early. Regression models identified 17 variables that were significant in determining subject noncompliance. Among those, distance, comorbidities, diabetic status, concomitant medications, previous clinic visits, length of study, disease under study, and severe adverse events were highly significant risk factors of noncompliance. CONCLUSION: The current research identified a substantial proportion of subjects who met the criteria for noncompliance within the trials analyzed. The factors identified in the current work are consistent with published clinical observations and the results of previous clinical trials. These results highlight the importance of considering study design and medical history when designing prospective clinical trials in an attempt to minimize data loss.


Assuntos
Cooperação do Paciente/estatística & dados numéricos , Pacientes Desistentes do Tratamento/estatística & dados numéricos , Doenças Retinianas/terapia , Humanos , Estudos Prospectivos , Ensaios Clínicos Controlados Aleatórios como Assunto , Análise de Regressão
11.
Sci Rep ; 9(1): 5650, 2019 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-30948739

RESUMO

Supercapacitors are beneficial as energy storage devices and can obtain high capacitance values greater than conventional capacitors and high power densities compared to batteries. However, in order to improve upon the overall cost, energy density, and charge-discharge rates, the electrode material of supercapacitors needs to be fine-tuned with an inexpensive, high conducting source. We prepared a Co(III) complex and polypyrrole (PPy) composite thin films (CoN4-PPy) that was electrochemically deposited on the surface of a glassy carbon working electrode. Cyclic voltammetry studies indicate the superior performance of CoN4-PPy in charge storage in acidic electrolyte compared to alkaline and organic solutions. The CoN4-PPy material generated the highest amount of specific capacitance (up to 721.9 F/g) followed by Co salt and PPy (Co-PPy) material and PPy alone. Cyclic performance studies showed the excellent electrochemical stability of the CoN4-PPy film in the acidic medium. Simply electrochemically depositing an inexpensive Co(III) complex with a high electrically conducting polymer of PPy delivered a superior electrode material for supercapacitor applications. Therefore, the results indicate that novel thin films derived from Co(III) metal complex and PPy can store a large amount of energy and maintain high stability over many cycles, revealing its excellent potential in supercapacitor devices.

12.
Adv Mater ; 31(11): e1807178, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30680821

RESUMO

In the continuously growing field of correlated electronic molecular crystals, there is significant interest in addressing alkali-metal-intercalated aromatic hydrocarbons, in which the possibility of high-temperature superconductivity emerges. However, searching for superconducting aromatic molecular crystals remains elusive due to their small shielding fraction volume. To exploit this potential, a design principle for percolation networks of technologically important film geometry is indispensable. Here the effect of potassium-intercalation is shown on the percolation network in self-assembled aromatic molecular crystals. It is demonstrated that one-dimensional (1D) dipole pairs, induced by dipole interaction, regulate the conductivity, as well as the electronic and optical transitions, in alkali-metal-intercalated molecular electronic crystals. A solid-solution growth methodology of aromatic molecular films with a broad range of stability is developed to uncover electronic and optical transitions of technological importance. The light-induced electron interactions enhance the charge-carrier itinerancy, leading to a switchable metal-to-insulator transition. This discovery opens a route for the development of aromatic molecular electronic solids and long-term modulation of electronic efficacy in nanotechnologically important thin films.

13.
Transgend Health ; 3(1): 109-117, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-29915810

RESUMO

Purpose: Scholars indicate that rates of mental and physical health issues (e.g., substance use, anxiety, depression) may be much higher among transgender individuals relative to the general population. This disparity may be even greater for transgender individuals in rural areas. Clinical researchers suggest using affirmative therapeutic approaches and interventions to address the health concerns of transgender individuals, specifically to connect individuals with the transgender community. However, little is known about the content of information that is shared in transgender communities in rural areas. Method: For this qualitative study, researchers asked transgender individuals in rural areas (n=10) what recommendations they would offer to other transgender individuals in rural areas regarding healthcare access. Results: Results were organized into four domains: Access care, Quality control, Difficulties, and Mentorship. Within these domains, we identified 11 sub-domains: Get physical healthcare, Get mental healthcare, Provider search, Provider vetting, Treatment verification, It will be difficult, Know who you are, Believe in yourself, Move, Connect to community, and Other. Conclusions: We discuss implications of our findings for healthcare provision in rural areas, and we provide recommendations for future research.

14.
Acta Crystallogr B Struct Sci Cryst Eng Mater ; 73(Pt 4): 669-674, 2017 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-28762977

RESUMO

Understanding the processes by which porous solid-state materials adsorb and release guest molecules would represent a significant step towards developing rational design principles for functional porous materials. To elucidate the process of liquid exchange in these materials, dynamic in situ X-ray diffraction techniques have been developed which utilize liquid-phase chemical stimuli. Using these time-resolved diffraction techniques, the ethanol solvation process in a flexible metal-organic framework [Co(AIP)(bpy)0.5(H2O)]·2H2O was examined. The measurements provide important insight into the nature of the chemical transformation in this system including the presence of a previously unreported neat ethanol solvate structure.

15.
Phys Rev E ; 96(5-1): 053301, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-29347689

RESUMO

Based on phase-field theory, we introduce a robust lattice-Boltzmann equation for modeling immiscible multiphase flows at large density and viscosity contrasts. Our approach is built by modifying the method proposed by Zu and He [Phys. Rev. E 87, 043301 (2013)PLEEE81539-375510.1103/PhysRevE.87.043301] in such a way as to improve efficiency and numerical stability. In particular, we employ a different interface-tracking equation based on the so-called conservative phase-field model, a simplified equilibrium distribution that decouples pressure and velocity calculations, and a local scheme based on the hydrodynamic distribution functions for calculation of the stress tensor. In addition to two distribution functions for interface tracking and recovery of hydrodynamic properties, the only nonlocal variable in the proposed model is the phase field. Moreover, within our framework there is no need to use biased or mixed difference stencils for numerical stability and accuracy at high density ratios. This not only simplifies the implementation and efficiency of the model, but also leads to a model that is better suited to parallel implementation on distributed-memory machines. Several benchmark cases are considered to assess the efficacy of the proposed model, including the layered Poiseuille flow in a rectangular channel, Rayleigh-Taylor instability, and the rise of a Taylor bubble in a duct. The numerical results are in good agreement with available numerical and experimental data.

16.
Biophys J ; 106(12): 2555-65, 2014 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-24940773

RESUMO

The Na/K pump hydrolyzes ATP to export three intracellular Na (Nai) as it imports two extracellular K (Ko) across animal plasma membranes. Within the protein, two ion-binding sites (sites I and II) can reciprocally bind Na or K, but a third site (site III) exclusively binds Na in a voltage-dependent fashion. In the absence of Nao and Ko, the pump passively imports protons, generating an inward current (IH). To elucidate the mechanisms of IH, we used voltage-clamp techniques to investigate the [H]o, [Na]o, and voltage dependence of IH in Na/K pumps from ventricular myocytes and in ouabain-resistant pumps expressed in Xenopus oocytes. Lowering pHo revealed that Ho both activates IH (in a voltage-dependent manner) and inhibits it (in a voltage-independent manner) by binding to different sites. Nao effects depend on pHo; at pHo where no Ho inhibition is observed, Nao inhibits IH at all concentrations, but when applied at pHo that inhibits pump-mediated current, low [Na]o activates IH and high [Na]o inhibits it. Our results demonstrate that IH is a property inherent to Na/K pumps, not linked to the oocyte expression environment, explains differences in the characteristics of IH previously reported in the literature, and supports a model in which 1), protons leak through site III; 2), binding of two Na or two protons to sites I and II inhibits proton transport; and 3), pumps with mixed Na/proton occupancy of sites I and II remain permeable to protons.


Assuntos
Prótons , ATPase Trocadora de Sódio-Potássio/metabolismo , Sódio/farmacologia , Animais , Cobaias , Ventrículos do Coração/citologia , Concentração de Íons de Hidrogênio , Técnicas In Vitro , Ativação do Canal Iônico/efeitos dos fármacos , Transporte de Íons/efeitos dos fármacos , Miócitos Cardíacos/metabolismo , Ouabaína/farmacologia , Técnicas de Patch-Clamp , Xenopus
17.
Mob Genet Elements ; 2(4): 184-192, 2012 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-23087843

RESUMO

MicroRNAs coordinate networks of mRNAs, but predicting specific sites of interactions is complicated by the very few bases of complementarity needed for regulation. Although efforts to characterize the specific requirements for microRNA (miR) regulation have made some advances, no general model of target recognition has been widely accepted. In this work, we describe an entirely novel approach to miR target identification. The genomic events responsible for the creation of individual miR loci have now been described with many miRs now known to have been initially formed from transposable element (TE) sequences. In light of this, we propose that limiting miR target searches to transcripts containing a miR's progenitor TE can facilitate accurate target identification. In this report we outline the methodology behind OrbId (Origin-based identification of microRNA targets). In stark contrast to the principal miR target algorithms (which rely heavily on target site conservation across species and are therefore most effective at predicting targets for older miRs), we find OrbId is particularly efficacious at predicting the mRNA targets of miRs formed more recently in evolutionary time. After defining the TE origins of > 200 human miRs, OrbId successfully generated likely target sets for 191 predominately primate-specific human miR loci. While only a handful of the loci examined were well enough conserved to have been previously evaluated by existing algorithms, we find ~80% of the targets for the oldest miR (miR-28) in our analysis contained within the principal Diana and TargetScan prediction sets. More importantly, four of the 15 OrbId miR-28 putative targets have been previously verified experimentally. In light of OrbId proving best-suited for predicting targets for more recently formed miRs, we suggest OrbId makes a logical complement to existing, conservation based, miR target algorithms.

18.
J Chiropr Med ; 6(2): 45-55, 2007 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-19674694

RESUMO

OBJECTIVE: This study aimed to evaluate the validity of the sacral base pressure test in diagnosing sacroiliac joint dysfunction. It also determined the predictive powers of the test in determining which type of sacroiliac joint dysfunction was present. METHODS: This was a double-blind experimental study with 62 participants. The results from the sacral base pressure test were compared against a cluster of previously validated tests of sacroiliac joint dysfunction to determine its validity and predictive powers. The external rotation of the feet, occurring during the sacral base pressure test, was measured using a digital inclinometer. RESULTS: There was no statistically significant difference in the results of the sacral base pressure test between the types of sacroiliac joint dysfunction. In terms of the results of validity, the sacral base pressure test was useful in identifying positive values of sacroiliac joint dysfunction. It was fairly helpful in correctly diagnosing patients with negative test results; however, it had only a "slight" agreement with the diagnosis for kappa interpretation. CONCLUSIONS: In this study, the sacral base pressure test was not a valid test for determining the presence of sacroiliac joint dysfunction or the type of dysfunction present. Further research comparing the agreement of the sacral base pressure test or other sacroiliac joint dysfunction tests with a criterion standard of diagnosis is necessary.

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