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1.
J Stroke Cerebrovasc Dis ; 33(6): 107683, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38513767

RESUMO

BACKGROUND AND OBJECTIVES: The prognosis of patients with spontaneous intracerebral hemorrhage (ICH) is often influenced by hematoma volume, a well-established predictor of poor outcome. However, the optimal intraventricular hemorrhage (IVH) volume cutoff for predicting poor outcome remains unknown. METHODS: We analyzed 313 patients with spontaneous ICH not undergoing evacuation, including 7 cases with external ventricular drainage (EVD). These patients underwent a baseline CT scan, followed by a 24-hour CT scan for measurement of both hematoma and IVH volume. We defined hematoma growth as hematoma growth > 33 % or 6 mL at follow-up CT, and poor outcome as modified Rankin Scale score≥3 at three months. Cutoffs with optimal sensitivity and specificity for predicting poor outcome were identified using receiver operating curves. RESULTS: The receiver operating characteristic analysis identified 6 mL as the optimal cutoff for predicting poor outcome. IVH volume> 6 mL was observed in 53 (16.9 %) of 313 patients. Patients with IVH volume>6 mL were more likely to be older and had higher NIHSS score and lower GCS score than those without. IVH volume>6 mL (adjusted OR 2.43, 95 % CI 1.13-5.30; P = 0.026) was found to be an independent predictor of poor clinical outcome at three months in multivariable regression analysis. CONCLUSIONS: Optimal IVH volume cutoff represents a powerful tool for improving the prediction of poor outcome in patients with ICH, particularly in the absence of clot evacuation or common use of EVD. Small amounts of intraventricular blood are not independently associated with poor outcome in patients with intracerebral hemorrhage. The utilization of optimal IVH volume cutoffs may improve the clinical trial design by targeting ICH patients that will obtain maximal benefit from therapies.


Assuntos
Valor Preditivo dos Testes , Tomografia Computadorizada por Raios X , Humanos , Masculino , Feminino , Idoso , Pessoa de Meia-Idade , Prognóstico , Estudos Retrospectivos , Hemorragia Cerebral Intraventricular/diagnóstico por imagem , Hemorragia Cerebral Intraventricular/fisiopatologia , Hemorragia Cerebral Intraventricular/terapia , Hemorragia Cerebral Intraventricular/diagnóstico , Hemorragia Cerebral/diagnóstico por imagem , Hemorragia Cerebral/terapia , Hemorragia Cerebral/diagnóstico , Hemorragia Cerebral/fisiopatologia , Fatores de Risco , Fatores de Tempo , Idoso de 80 Anos ou mais , Avaliação da Deficiência , Hematoma/diagnóstico por imagem , Hematoma/diagnóstico , Curva ROC
2.
Ann Clin Transl Neurol ; 11(2): 368-376, 2024 02.
Artigo em Inglês | MEDLINE | ID: mdl-38009388

RESUMO

OBJECTIVE: To assess the prevalence and factors associated with early cognitive impairment in intracerebral hemorrhage (ICH) patients and to describe short-term recovery trajectories among ICH patients with early cognitive impairment. METHODS: We prospectively enrolled ICH patients without baseline dementia in our institutions. Cognitive function was assessed using mini-mental state examination (MMSE), and functional outcome was evaluated at discharge, 3, and 6 months after symptoms onset using the modified Rankin Scale (mRS). We used multinomial logistic regression models to investigate potential risk factors and generalized linear models to analyze the functional outcome data. RESULTS: Out of 181 patients with ICH, 167 were included in the final analysis. Early cognitive impairment occurred in 60.48% of patients with ICH. Age (odds ratio [OR] per 1-year increase, 1.037; 95% confidence interval [CI], 1.003-1.071; p = 0.034), National Institutes of Health Stroke Scale (NIHSS) score (OR per 1-point increase, 1.146; 95% CI, 1.065-1.233; p < 0.001) and lobar ICH location (OR, 4.774; 95% CI, 1.810-12.593; p = 0.002) were associated with early cognitive impairment in ICH patients. Patients with ≥10 years of education were less likely to experience early cognitive impairment (OR, 0.323; 95% CI, 0.133-0.783; p = 0.012). Participants with early cognitive impairment had a higher risk of poor outcome (OR, 4.315; 95% CI, 1.503-12.393; p = 0.005) than those without. Furthermore, there was a significantly faster functional recovery rate for those without early cognitive impairment compared with those with at 3 and 6 months (p < 0.05). INTERPRETATION: Early cognitive impairment was prevalent and associated with poor outcomes in ICH patients, which decelerated short-term functional recovery.


Assuntos
Hemorragia Cerebral , Disfunção Cognitiva , Estados Unidos , Humanos , Hemorragia Cerebral/complicações , Hemorragia Cerebral/epidemiologia , Disfunção Cognitiva/epidemiologia , Disfunção Cognitiva/etiologia , Fatores de Risco , Cognição , Recuperação de Função Fisiológica
3.
Front Aging Neurosci ; 15: 1264124, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38020784

RESUMO

Background and purpose: Intracerebral hemorrhage (ICH) is a severe form of stroke that remains understudied in the young adults. We aimed to investigate the clinical presentation, and risk factors associated with ICH in this age group and compare them to older patients. Methods: Our study included ICH patients admitted between March 2016 and December 2021 in the First Affiliated Hospital of Chongqing Medical University from our ongoing prospective cohort database. Demographic characteristics, etiology, risk factors, and clinical outcomes were compared between elderly and young patients. Furthermore, logistic regression analysis was employed to explore risk factors associated with the functional outcome at 3-months. Results: We selected 1,003 patients (mean age, 59.9 ±13.8 years old), 746 (74.4%) patients were aged >50 years. The logistic regression analysis showed young patients have a higher proportion of secondary ICH, higher white blood cell count and higher body mass index (BMI), but less diabetes mellitus. Of all patients, predictors of 3-month functional independence was first-ever ICH and age ≤50 years. The history of nephropathy and stroke, higher baseline NIHSS score, larger hematoma volume, and the presence of hydrocephalus were associated with poor outcomes. And the white blood cell count could significantly influence the prognosis among young ICH patients. Three-month functional outcome based on modified Rankin scale score was better in young patients than the elderly (OR, 1.232; 95% CI, 1.095-1.388; p < 0.001). Conclusions: The highest incidence of ICH occurs in the age groups of 50-59 and 60-69. ICH in young adults had higher white blood cell and BMI compared to the elderly, and differs in etiological distribution. The young patients also had similar short-term mortality but more favorable functional outcomes than the elderly. Furthermore, NIHSS score and larger hematoma volumes were associated with poor outcome in all patients.

4.
Adv Mater ; 35(44): e2306029, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37611614

RESUMO

Domain switching is crucial for achieving desired functions in ferroic materials that are used in various applications. Fast control of domains at sub-nanosecond timescales remains a challenge despite its potential for high-speed operation in random-access memories, photonic, and nanoelectronic devices. Here, ultrafast laser excitation is shown to transiently melt and reconfigure ferroelectric stripe domains in multiferroic bismuth ferrite on a timescale faster than 100 picoseconds. This dynamic behavior is visualized by picosecond- and nanometer-resolved X-ray diffraction and time-resolved X-ray diffuse scattering. The disordering of stripe domains is attributed to the screening of depolarization fields by photogenerated carriers resulting in the formation of charged domain walls, as supported by phase-field simulations. Furthermore, the recovery of disordered domains exhibits subdiffusive growth on nanosecond timescales, with a non-equilibrium domain velocity reaching up to 10 m s-1 . These findings present a new approach to image and manipulate ferroelectric domains on sub-nanosecond timescales, which can be further extended into other complex photoferroic systems to modulate their electronic, optical, and magnetic properties beyond gigahertz frequencies. This approach could pave the way for high-speed ferroelectric data storage and computing, and, more broadly, defines new approaches for visualizing the non-equilibrium dynamics of heterogeneous and disordered materials.

5.
Proc Natl Acad Sci U S A ; 120(28): e2303312120, 2023 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-37410867

RESUMO

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO3/SrTiO3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca2RuO4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca2RuO4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials.


Assuntos
Filmes Cinematográficos , Refração Ocular , Aprendizado de Máquina não Supervisionado
6.
Nat Mater ; 22(7): 873-879, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37231245

RESUMO

The interconversion between electrical and mechanical energies is pivotal to ferroelectrics to enable their applications in transducers, actuators and sensors. Ferroelectric polymers exhibit a giant electric-field-induced strain (>4.0%), markedly exceeding the actuation strain (≤1.7%) of piezoelectric ceramics and crystals. However, their normalized elastic energy densities remain orders of magnitude smaller than those of piezoelectric ceramics and crystals, severely limiting their practical applications in soft actuators. Here we report the use of electro-thermally induced ferroelectric phase transition in percolative ferroelectric polymer nanocomposites to achieve high strain performance in electric-field-driven actuation materials. We demonstrate a strain of over 8% and an output mechanical energy density of 11.3 J cm-3 at an electric field of 40 MV m-1 in the composite, outperforming the benchmark relaxor single-crystal ferroelectrics. This approach overcomes the trade-off between mechanical modulus and electro-strains in conventional piezoelectric polymer composites and opens up an avenue for high-performance ferroelectric actuators.


Assuntos
Eletricidade , Nanocompostos , Polímeros
7.
Nano Lett ; 23(7): 2551-2556, 2023 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-36971545

RESUMO

We study the thermodynamics of nanoscale polar structures in PbTiO3/SrTiO3 ferroelectric superlattices induced by above-bandgap optical excitation using a phase-field model explicitly considering both structural and electronic processes. We demonstrate that the light-excited carriers provide the charge compensation of polarization bound charges and the lattice thermal energy, both of which are key to the thermodynamic stabilization of a previously observed supercrystal, a three-dimensionally periodic nanostructure, within a window of substrate strains, while different mechanical and electrical boundary conditions can stabilize a number of other nanoscale polar structures by balancing the competing short-range exchange interactions responsible for the domain wall energy and long-range electrostatic and elastic interactions. The insights into the light-induced formation and richness of nanoscale structures from this work offer theoretical guidance for exploring and manipulating the thermodynamic stability of nanoscale polar structures employing a combination of thermal, mechanical, and electrical stimuli as well as light.

8.
Neurol Sci ; 44(2): 621-629, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36301361

RESUMO

OBJECTIVE: Dysphagia is one of the most common complications of acute ischemic stroke, and prediction of dysphagia is crucial for post-stroke treatment. We aimed to identify predictors of dysphagia and swallowing function recovery following ischemic stroke and to investigate dysphagia-associated lesion location. METHODS: We prospectively enrolled patients with acute ischemic stroke confirmed on diffusion-weighted imaging. All patients received swallowing evaluation within 48 h after admission. Follow-up oral intake ability was measured on 7 and 30 days after stroke onset. Voxel-based lesion-symptom mapping was performed to determine locations associated with dysphagia. RESULTS: Of 126 patients included in the final analysis, 23 patients (18.3%) were classified as initial dysphagia. The presence of facial palsy (P = 0.008) and larger white matter hyperintensity (WMH) volume (P = 0.003) was associated with initial dysphagia. Initial risk of aspiration assessed by Any2 score (P = 0.001) at baseline was identified as independent predictor for dysphagia at day 7. Patients with higher Any2 score (P < 0.001), aphasia (P = 0.013), and larger WMH volume (P = 0.010) were less likely to have a full swallowing function recovery at 1 month. Acute infarcts in right corona radiata and right superior longitudinal fasciculus were correlated with impaired recovery of swallowing ability at 1 month. CONCLUSIONS: Initial risk of aspiration was identified as risk factor for short-term and long-term dysphagia. Aphasia and larger WMH volume were revealed to be significant predictors for swallowing function recovery at 1 month. Right corona radiata was identified as an essential brain area for dysphagia.


Assuntos
Transtornos de Deglutição , AVC Isquêmico , Acidente Vascular Cerebral , Humanos , Transtornos de Deglutição/etiologia , Transtornos de Deglutição/complicações , Deglutição , AVC Isquêmico/complicações , Acidente Vascular Cerebral/complicações , Acidente Vascular Cerebral/diagnóstico por imagem , Acidente Vascular Cerebral/patologia , Encéfalo
9.
Nano Lett ; 22(23): 9275-9282, 2022 12 14.
Artigo em Inglês | MEDLINE | ID: mdl-36450036

RESUMO

Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg1/3Nb2/3O3-0.32PbTiO3 (PMN-0.32PT) by probing its atomic-scale response via femtosecond-resolution, electron-scattering approaches. By combining these structural measurements with dynamic phase-field simulations, we show that femtosecond light pulses drive a change in both the magnitude and direction of the polarization vector within polar nanodomains on few-picosecond time scales. This study defines new opportunities for dynamic reconfigurable control of the polarization in nanoscale relaxor ferroelectrics.


Assuntos
Elétrons
10.
Adv Mater ; 34(49): e2202841, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36189841

RESUMO

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi2 Te4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. By quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

11.
Nat Commun ; 13(1): 6340, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36284138

RESUMO

Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO3/SrRuO3 interface, a two-unit-cell thick SrTiO3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s-1. Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.

12.
Nat Commun ; 13(1): 4867, 2022 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-35982033

RESUMO

Polymer-ceramic piezoelectric composites, combining high piezoelectricity and mechanical flexibility, have attracted increasing interest in both academia and industry. However, their piezoelectric activity is largely limited by intrinsically low crystallinity and weak spontaneous polarization. Here, we propose a Ti3C2Tx MXene anchoring method to manipulate the intermolecular interactions within the all-trans conformation of a polymer matrix. Employing phase-field simulation and molecular dynamics calculations, we show that OH surface terminations on the Ti3C2Tx nanosheets offer hydrogen bonding with the fluoropolymer matrix, leading to dipole alignment and enhanced net spontaneous polarization of the polymer-ceramic composites. We then translated this interfacial bonding strategy into electrospinning to boost the piezoelectric response of samarium doped Pb (Mg1/3Nb2/3)O3-PbTiO3/polyvinylidene fluoride composite nanofibers by 160% via Ti3C2Tx nanosheets inclusion. With excellent piezoelectric and mechanical attributes, the as-electrospun piezoelectric nanofibers can be easily integrated into the conventional shoe insoles to form a foot sensor network for all-around gait patterns monitoring, walking habits identification and Metatarsalgi prognosis. This work utilizes the interfacial coupling mechanism of intermolecular anchoring as a strategy to develop high-performance piezoelectric composites for wearable electronics.


Assuntos
Nanofibras , Polímeros
13.
Adv Sci (Weinh) ; 9(13): e2105550, 2022 05.
Artigo em Inglês | MEDLINE | ID: mdl-35277947

RESUMO

Piezoelectric nanocomposites with oxide fillers in a polymer matrix combine the merit of high piezoelectric response of the oxides and flexibility as well as biocompatibility of the polymers. Understanding the role of the choice of materials and the filler-matrix architecture is critical to achieving desired functionality of a composite towards applications in flexible electronics and energy harvest devices. Herein, a high-throughput phase-field simulation is conducted to systematically reveal the influence of morphology and spatial orientation of an oxide filler on the piezoelectric, mechanical, and dielectric properties of the piezoelectric nanocomposites. It is discovered that with a constant filler volume fraction, a composite composed of vertical pillars exhibits superior piezoelectric response and electromechanical coupling coefficient as compared to the other geometric configurations. An analytical regression is established from a linear regression-based machine learning model, which can be employed to predict the performance of nanocomposites filled with oxides with a given set of piezoelectric coefficient, dielectric permittivity, and stiffness. This work not only sheds light on the fundamental mechanism of piezoelectric nanocomposites, but also offers a promising material design strategy for developing high-performance polymer/inorganic oxide composite-based wearable electronics.


Assuntos
Nanocompostos , Eletrônica , Aprendizado de Máquina , Óxidos , Polímeros
15.
J Clin Med ; 12(1)2022 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-36614867

RESUMO

The mortality of stroke increases on weekends and during off-hour periods. We investigated the effect of off-hour admission on the outcomes of intracerebral hemorrhage (ICH) patients. We retrospectively analyzed a prospective cohort of ICH patients, admitted between January 2017 and December 2019 at the First Affiliated Hospital of Chongqing Medical University. Acute ICH within 72 h after onset with a baseline computed tomography and 3-month follow-up were included in our study. Multivariable logistic regression analysis was performed for calculating the odds ratios (OR) and 95% confidence interval (CI) for the outcome measurements. Of the 656 participants, 318 (48.5%) were admitted during on-hours, whereas 338 (51.5%) were admitted during off-hours. Patients with a poor outcome had a larger median baseline hematoma volume, of 27 mL (interquartile range 11.1-53.2 mL), and a lower median time from onset to imaging, of 2.8 h (interquartile range 1.4-9.6 h). Off-hour admission was significantly associated with a poor functional outcome at 3 months, after adjusting for cofounders (adjusted OR 2.17, 95% CI 1.35-3.47; p = 0.001). We found that patients admitted during off-hours had a higher risk of poor functional outcomes at 3 months than those admitted during working hours.

16.
ACS Appl Mater Interfaces ; 13(45): 53439-53453, 2021 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-34469098

RESUMO

There has been a surge of interest in applying deep learning (DL) to microstructure generation and materials design. However, existing DL-based methods are generally limited in generating (1) microstructures with high resolution, (2) microstructures with high variability, (3) microstructures with guaranteed periodicity, and (4) highly controllable microstructures. In this study, a DL approach based on a stacked generative adversarial network (StackGAN-v2) is proposed to overcome these shortcomings. The presented modeling approach can reconstruct high-fidelity microstructures of additively manufactured piezoceramics with different resolutions, which are statistically equivalent to original microstructures either experimentally observed or numerically predicted. Advantages of the proposed modeling approach are also illustrated in terms of its capability in controlling the probability density function (PDF) of grain size, grain orientation, and micropore in a large space, which would have significant benefits in exploring the effects of these microstructure features on the piezoelectricity of piezoceramics. In the meantime, periodicity of the microstructures has been successfully introduced in the developed model, which can critically reduce the simulation volume to be considered as a representative volume element (RVE) during computational calculation of piezoelectric properties. Therefore, this DL approach can significantly accelerate the process of designing optimal microstructures when integrating with computational methods (e.g., fast Fourier spectral iterative perturbation (FSIPM)) to achieve desired piezoelectric properties. The proposed DL-based method is generally applicable to optimal design of a variety of periodic microstructures, allowing for maximum explorations of design spaces and fine manipulations of microstructural features.

17.
Adv Mater ; 33(36): e2102421, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34302393

RESUMO

Domain wall motion in ferroics, similar to dislocation motion in metals, can be tuned by well-concepted microstructural elements. In demanding high-power applications of piezoelectric materials, the domain wall motion is considered as a lossy hysteretic mechanism that should be restricted. Current applications for so-called hard piezoelectrics are abundant and hinge on the use of an acceptor-doping scheme. However, this mechanism features severe limitations due to enhanced mobility of oxygen vacancies at moderate temperatures. By analogy with metal technology, the authors present here a new solution for electroceramics, where precipitates are utilized to pin domain walls and improve piezoelectric properties. Through a sequence of sintering, nucleation, and precipitate growth, intragranular precipitates leading to a fine domain structure are developed as shown by transmission electron microscopy, piezoresponse force microscopy, and phase-field simulation. This structure impedes the domain wall motion as elucidated by electromechanical characterization. As a result, the mechanical quality factor is increased by ≈50% and the hysteresis in electrostrain is suppressed considerably. This is even achieved with slightly increased piezoelectric coefficient and electromechanical coupling factor. This novel process can be smoothly implemented in industrial production processes and is accessible to simple laboratory experimentation for microstructure optimization and implementation in various ferroelectric systems.

18.
Nature ; 592(7854): 376-380, 2021 04.
Artigo em Inglês | MEDLINE | ID: mdl-33854251

RESUMO

The collective dynamics of topological structures1-6 are of interest from both fundamental and applied perspectives. For example, studies of dynamical properties of magnetic vortices and skyrmions3,4 have not only deepened our understanding of many-body physics but also offered potential applications in data processing and storage7. Topological structures constructed from electrical polarization, rather than electron spin, have recently been realized in ferroelectric superlattices5,6, and these are promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics underlying the functionality of such complex extended nanostructures. Here, using terahertz-field excitation and femtosecond X-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders-of-magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices3. A previously unseen tunable mode, hereafter referred to as a vortexon, emerges in the form of transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond timescales. Its frequency is considerably reduced (softened) at a critical strain, indicating a condensation (freezing) of structural dynamics. We use first-principles-based atomistic calculations and phase-field modelling to reveal the microscopic atomic arrangements and corroborate the frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens opportunities for electric-field-driven data processing in topological structures with ultrahigh speed and density.

19.
Adv Mater ; 32(49): e2005431, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-33150671

RESUMO

Both experimental results and theoretical models suggest the decisive role of the filler-matrix interfaces on the dielectric, piezoelectric, pyroelectric, and electrocaloric properties of ferroelectric polymer nanocomposites. However, there remains a lack of direct structural evidence to support the so-called interfacial effect in dielectric nanocomposites. Here, a chemical mapping of the interfacial coupling between the nanofiller and the polymer matrix in ferroelectric polymer nanocomposites by combining atomic force microscopy-infrared spectroscopy (AFM-IR) with first-principles calculations and phase-field simulations is provided. The addition of ceramic fillers into a ferroelectric polymer leads to augmentation of the local conformational disorder in the vicinity of the interface, resulting in the local stabilization of the all-trans conformation (i.e., the polar ß phase). The formation of highly polar and inhomogeneous interfacial regions, which is further enhanced with a decrease of the filler size, has been identified experimentally and verified by phase-field simulations and density functional theory (DFT) calculations. This work offers unprecedented structural insights into the configurational disorder-induced interfacial effect and will enable rational design and molecular engineering of the filler-matrix interfaces of electroactive polymer nanocomposites to boost their collective properties.

20.
Science ; 369(6501): 292-297, 2020 07 17.
Artigo em Inglês | MEDLINE | ID: mdl-32675370

RESUMO

High-performance piezoelectric materials are critical components for electromechanical sensors and actuators. For more than 60 years, the main strategy for obtaining large piezoelectric response has been to construct multiphase boundaries, where nanoscale domains with local structural and polar heterogeneity are formed, by tuning complex chemical compositions. We used a different strategy to emulate such local heterogeneity by forming nanopillar regions in perovskite oxide thin films. We obtained a giant effective piezoelectric coefficient [Formula: see text] of ~1098 picometers per volt with a high Curie temperature of ~450°C. Our lead-free composition of sodium-deficient sodium niobate contains only three elements (Na, Nb, and O). The formation of local heterogeneity with nanopillars in the perovskite structure could be the basis for a general approach to designing and optimizing various functional materials.

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