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1.
Nano Lett ; 18(5): 3088-3095, 2018 05 09.
Artigo em Inglês | MEDLINE | ID: mdl-29631404

RESUMO

Polar domains arise in insulating ferroelectrics when free carriers are unable to fully screen surface-bound charges. Recently discovered binary and ternary polar metals exhibit broken inversion symmetry coexisting with free electrons that might be expected to suppress the electrostatic driving force for domain formation. Contrary to this expectation, we report the first direct observation of polar domains in single crystals of the polar metal Ca3Ru2O7. By a combination of mesoscale optical second-harmonic imaging and atomic-resolution scanning transmission electron microscopy, the polar domains are found to possess a quasi-two-dimensional slab geometry with a lateral size of ∼100 µm and thickness of ∼10 nm. Electronic structure calculations show that the coexistence of electronic and parity-lifting orders arise from anharmonic lattice interactions, which support 90° and 180° polar domains in a metal. Using in situ transmission electron microscopy, we also demonstrate a strain-tuning route to achieve ferroelastic switching of polar metal domains.

2.
Phys Rev Lett ; 120(9): 096101, 2018 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-29547337

RESUMO

Using time- and spatially resolved hard x-ray diffraction microscopy, the striking structural and electrical dynamics upon optical excitation of a single crystal of BaTiO_{3} are simultaneously captured on subnanoseconds and nanoscale within individual ferroelectric domains and across walls. A large emergent photoinduced electric field of up to 20×10^{6} V/m is discovered in a surface layer of the crystal, which then drives polarization and lattice dynamics that are dramatically distinct in a surface layer versus bulk regions. A dynamical phase-field modeling method is developed that reveals the microscopic origin of these dynamics, leading to gigahertz polarization and elastic waves traveling in the crystal with sonic speeds and spatially varying frequencies. The advances in spatiotemporal imaging and dynamical modeling tools open up opportunities for disentangling ultrafast processes in complex mesoscale structures such as ferroelectric domains.

3.
Nano Lett ; 17(5): 2802-2808, 2017 05 10.
Artigo em Inglês | MEDLINE | ID: mdl-28288273

RESUMO

Two-dimensional materials offer a remarkably rich materials platform to study the origin of different material behaviors at the atomic level, and doping provides a key means of tailoring such materials' functional properties. The local atomic structure around such dopants can be critically important in determining the material's behavior as it could modulate scattering, catalytic activity, electronic and magnetic properties, and so forth. Here, using aberration-corrected scanning transmission electron microscopy (STEM) with sub-Ångstrom resolution in conjunction with density functional theory calculations, we demonstrate a strong coupling between Mo dopants and two types of defects in WS2 monolayers: sulfur monovacancies and grain boundaries. Although Mo does occupy a transition metal lattice site, it is not an ideal substitutional dopant: ∼80% of the S vacancies identified by STEM colocalize with Mo dopants, an affinity that appears to be enhanced by symmetry breaking of a partially occupied midgap defect state. Although a Mo dopant by itself does not considerably distort the WS2 lattice, it induces substantial lattice deformation by apparently facilitating the charging of a sulfur monovacancy paired with it, which is consistent with the results of first-principles calculations. This coupling of foreign substitutional dopants with vacancies could potentially be exploited to control the distribution and location of chalcogenide vacancies within transition metal dichalcogenides (TMD), by segregating vacancies into regions of high Mo concentration that are purposely placed away from active regions of TMD-based devices.

4.
J Am Chem Soc ; 139(7): 2833-2841, 2017 02 22.
Artigo em Inglês | MEDLINE | ID: mdl-28161942

RESUMO

One synthetic modality for materials discovery proceeds by forming mixtures of two or more compounds. In transition metal oxides (TMOs), chemical substitution often obeys Vegard's principle, and the resulting structure and properties of the derived phase follow from its components. A change in the assembly of the components into a digital nanostructure, however, can stabilize new polymorphs and properties not observed in the constituents. Here we formulate and demonstrate a crystal-chemistry design approach for realizing digital TMOs without inversion symmetry by combining two centrosymmetric compounds, utilizing periodic anion-vacancy order to generate multiple polyhedra that together with cation order produce a polar structure. We next apply this strategy to two brownmillerite-structured TMOs known to display centrosymmetric crystal structures in their bulk, Ca2Fe2O5 and Sr2Fe2O5. We then realize epitaxial (SrFeO2.5)1/(CaFeO2.5)1 thin film superlattices possessing both anion-vacancy order and Sr and Ca chemical order at the subnanometer scale, confirmed through synchrotron-based diffraction and aberration corrected electron microscopy. Through a detailed symmetry analysis and density functional theory calculations, we show that A-site cation ordering lifts inversion symmetry in the superlattice and produces a polar compound. Our results demonstrate how control of anion and cation order at the nanoscale can be utilized to produce acentric structures markedly different than their constituents and open a path toward novel structure-based property design.

5.
Nat Mater ; 15(11): 1166-1171, 2016 11.
Artigo em Inglês | MEDLINE | ID: mdl-27571451

RESUMO

The spectrum of two-dimensional (2D) and layered materials 'beyond graphene' offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (∼5.0-6.0 eV), has clearly established that 2D nitrides are key to advancing 2D devices. A gap, however, remains between the theoretical prediction of 2D nitrides 'beyond hBN' and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of 2D nitrides that are difficult to prepare via traditional synthesis.

6.
Clin Infect Dis ; 62(11): 1380-1389, 2016 06 01.
Artigo em Inglês | MEDLINE | ID: mdl-26962078

RESUMO

BACKGROUND: When combined with ceftazidime, the novel non-ß-lactam ß-lactamase inhibitor avibactam provides a carbapenem alternative against multidrug-resistant infections. Efficacy and safety of ceftazidime-avibactam plus metronidazole were compared with meropenem in 1066 men and women with complicated intra-abdominal infections from 2 identical, randomized, double-blind phase 3 studies (NCT01499290 and NCT01500239). METHODS: The primary end point was clinical cure at test-of-cure visit 28-35 days after randomization, assessed by noninferiority of ceftazidime-avibactam plus metronidazole to meropenem in the microbiologically modified intention-to-treat (mMITT) population (in accordance with US Food and Drug Administration guidance), and the modified intention-to-treat and clinically evaluable populations (European Medicines Agency guidance). Noninferiority was considered met if the lower limit of the 95% confidence interval for between-group difference was greater than the prespecified noninferiority margin of -12.5%. RESULTS: Ceftazidime-avibactam plus metronidazole was noninferior to meropenem across all primary analysis populations. Clinical cure rates with ceftazidime-avibactam plus metronidazole and meropenem, respectively, were as follows: mMITT population, 81.6% and 85.1% (between-group difference, -3.5%; 95% confidence interval -8.64 to 1.58); modified intention-to-treat, 82.5% and 84.9% (-2.4%; -6.90 to 2.10); and clinically evaluable, 91.7% and 92.5% (-0.8%; -4.61 to 2.89). The clinical cure rate with ceftazidime-avibactam plus metronidazole for ceftazidime-resistant infections was comparable to that with meropenem (mMITT population, 83.0% and 85.9%, respectively) and similar to the regimen's own efficacy against ceftazidime-susceptible infections (82.0%). Adverse events were similar between groups. CONCLUSIONS: Ceftazidime-avibactam plus metronidazole was noninferior to meropenem in the treatment of complicated intra-abdominal infections. Efficacy was similar against infections caused by ceftazidime-susceptible and ceftazidime-resistant pathogens. The safety profile of ceftazidime-avibactam plus metronidazole was consistent with that previously observed with ceftazidime alone. CLINICAL TRIALS REGISTRATION: NCT01499290 and NCT01500239.


Assuntos
Antibacterianos , Compostos Azabicíclicos , Ceftazidima , Infecções Intra-Abdominais/tratamento farmacológico , Metronidazol , Tienamicinas , Adolescente , Adulto , Idoso , Idoso de 80 Anos ou mais , Antibacterianos/administração & dosagem , Antibacterianos/efeitos adversos , Antibacterianos/uso terapêutico , Compostos Azabicíclicos/administração & dosagem , Compostos Azabicíclicos/efeitos adversos , Compostos Azabicíclicos/uso terapêutico , Ceftazidima/administração & dosagem , Ceftazidima/efeitos adversos , Ceftazidima/uso terapêutico , Combinação de Medicamentos , Feminino , Humanos , Infecções Intra-Abdominais/epidemiologia , Masculino , Meropeném , Metronidazol/administração & dosagem , Metronidazol/efeitos adversos , Metronidazol/uso terapêutico , Pessoa de Meia-Idade , Tienamicinas/administração & dosagem , Tienamicinas/efeitos adversos , Tienamicinas/uso terapêutico , Resultado do Tratamento , Adulto Jovem
7.
Phys Rev Lett ; 112(18): 187602, 2014 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-24856722

RESUMO

Rotations of oxygen octahedra are ubiquitous, but they cannot break inversion symmetry in simple perovskites. However, in a layered oxide structure, this is possible, as we demonstrate here in A-site ordered Ruddlesden-Popper NaRTiO4 (R denotes rare-earth metal), previously believed to be centric. By revisiting this series via synchrotron x-ray diffraction, optical second-harmonic generation, piezoresponse force microscopy, and first-principles phonon calculations, we find that the low-temperature phase belongs to the acentric space group P42(1)m, which is piezoelectric and nonpolar. The mechanism underlying this large new family of acentric layered oxides is prevalent, and could lead to many more families of acentric oxides.

8.
Adv Mar Biol ; 69: 289-324, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-25358303

RESUMO

The Republic of Kiribati's Phoenix Islands Protected Area (PIPA), located in the equatorial central Pacific, is the largest and deepest UNESCO World Heritage site on earth. Created in 2008, it was the first Marine Protected Area (MPA) of its kind (at the time of inception, the largest in the world) and includes eight low-lying islands, shallow coral reefs, submerged shallow and deep seamounts and extensive open-ocean and ocean floor habitat. Due to their isolation, the shallow reef habitats have been protected de facto from severe exploitation, though the surrounding waters have been continually fished for large pelagics and whales over many decades. PIPA was created under a partnership between the Government of Kiribati and the international non-governmental organizations-Conservation International and the New England Aquarium. PIPA has a unique conservation strategy as the first marine MPA to use a conservation contract mechanism with a corresponding Conservation Trust established to be both a sustainable financing mechanism and a check-and-balance to the oversight and maintenance of the MPA. As PIPA moves forward with its management objectives, it is well positioned to be a global model for large MPA design and implementation in similar contexts. The islands and shallow reefs have already shown benefits from protection, though the pending full closure of PIPA (and assessments thereof) will be critical for determining success of the MPA as a refuge for open-ocean pelagic and deep-sea marine life. As global ocean resources are continually being extracted to support a growing global population, PIPA's closure is both timely and of global significance.


Assuntos
Conservação dos Recursos Naturais , Pesqueiros , Programas Governamentais , Animais , Comportamento Cooperativo , Ecossistema , Governo Federal , Peixes , Geografia , Micronésia , Organizações , Parcerias Público-Privadas
9.
Adv Mater ; 36(24): e2312673, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38441355

RESUMO

The drive toward non-von Neumann device architectures has led to an intense focus on insulator-to-metal (IMT) and the converse metal-to-insulator (MIT) transitions. Studies of electric field-driven IMT in the prototypical VO2 thin-film channel devices are largely focused on the electrical and elastic responses of the films, but the response of the corresponding TiO2 substrate is often overlooked, since it is nominally expected to be electrically passive and elastically rigid. Here, in-operando spatiotemporal imaging of the coupled elastodynamics using X-ray diffraction microscopy of a VO2 film channel device on TiO2 substrate reveals two new surprises. First, the film channel bulges during the IMT, the opposite of the expected shrinking in the film undergoing IMT. Second, a microns thick proximal layer in the substrate also coherently bulges accompanying the IMT in the film, which is completely unexpected. Phase-field simulations of coupled IMT, oxygen vacancy electronic dynamics, and electronic carrier diffusion incorporating thermal and strain effects suggest that the observed elastodynamics can be explained by the known naturally occurring oxygen vacancies that rapidly ionize (and deionize) in concert with the IMT (MIT). Fast electrical-triggering of the IMT via ionizing defects and an active "IMT-like" substrate layer are critical aspects to consider in device applications.

10.
Opt Lett ; 37(6): 1032-4, 2012 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-22446214

RESUMO

We report changes in the Raman spectra at ferroelectric domain walls in near-stoichiometric LiNbO3 and stoichiometric LiTaO3. We find a decrease of intensity for the regular bulk Raman peaks along with increases of intensity in spectral regions that correspond to phonons, which propagate at an angle with respect to the incident light. In the backscattering geometry, such modes are not supported in the bulk crystal due to momentum conservation. We confirm that these changes are due to the domain wall itself and are independent of intrinsic defects or charging effects.

11.
Opt Express ; 17(25): 23284-9, 2009 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-20052254

RESUMO

Laser-fabrication of complex, highly oriented three-dimensional ferroelectric single crystal architecture with straight lines and bends is demonstrated in lanthanum borogermanate model glass using a high repetition rate femtosecond laser. Scanning micro-Raman microscopy shows that the c-axis of the ferroelectric crystal is aligned with the writing direction even after bending. A gradual rather than an abrupt transition is observed for the changing lattice orientation through bends up to approximately 14 degrees. Thus the single crystal character of the line is preserved along the bend through lattice straining rather than formation of a grain boundary.


Assuntos
Brometos/química , Brometos/efeitos da radiação , Cristalização/métodos , Vidro/química , Vidro/efeitos da radiação , Lantânio/química , Lantânio/efeitos da radiação , Lasers , Anisotropia , Campos Eletromagnéticos , Teste de Materiais
12.
Nat Commun ; 9(1): 5220, 2018 12 06.
Artigo em Inglês | MEDLINE | ID: mdl-30523251

RESUMO

Octahedral tilts are the most ubiquitous distortions in perovskite-related structures that can dramatically influence ferroelectric, magnetic, and electronic properties; yet the paradigm of tilt epitaxy in thin films is barely explored. Non-destructively characterizing such epitaxy in three-dimensions for low symmetry complex tilt systems composed of light anions is a formidable challenge. Here we demonstrate that the interfacial tilt epitaxy can transform ultrathin calcium titanate, a non-polar earth-abundant mineral, into high-temperature polar oxides that last above 900 K. The comprehensive picture of octahedral tilts and polar distortions is revealed by reconstructing the three-dimensional electron density maps across film-substrate interfaces with atomic resolution using coherent Bragg rod analysis. The results are complemented with aberration-corrected transmission electron microscopy, film superstructure reflections, and are in excellent agreement with density functional theory. The study could serve as a broader template for non-destructive, three-dimensional atomic resolution probing of complex low symmetry functional interfaces.

13.
Eur Heart J Cardiovasc Imaging ; 18(1): 11-18, 2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-26985077

RESUMO

AIM: To investigate the efficacy of low-density lipoprotein (LDL) transport simulation in reconstructed arteries derived from computed tomography coronary angiography (CTCA) to predict coronary segments that are prone to progress. METHODS AND RESULTS: Thirty-two patients admitted with an acute coronary event who underwent 64-slice CTCA after percutaneous coronary intervention and at 3-year follow-up were included in the analysis. The CTCA data were used to reconstruct the coronary anatomy of the untreated vessels at baseline and follow-up, and LDL transport simulation was performed in the baseline models. The computed endothelial shear stress (ESS), LDL concentration, and CTCA-derived plaque characteristics were used to identify predictors of substantial disease progression (defined as an increase in the plaque burden at follow-up higher than two standard deviations of the intra-observer variability of the expert who performed the analysis). Fifty-eight vessels were analysed. High LDL concentration [odds ratio (OR): 2.16; 95% confidence interval (CI): 1.64-2.84; P = 0.0054], plaque burden (OR: 1.40; 95% CI: 1.13-1.72; P = 0.0017), and plaque area (OR: 3.46; 95% CI: 2.20-5.44; P≤ 0.0001) were independent predictors of a substantial disease progression at follow-up. The ESS appears as a predictor of disease progression in univariate analysis but was not an independent predictor when the LDL concentration was entered into the multivariate model. The accuracy of the model that included the LDL concentration was higher than the accuracy of the model that included the ESS (65.1 vs. 62.5%). CONCLUSIONS: LDL transport modelling appears a better predictor of atherosclerotic disease progression than the ESS, and combined with the atheroma characteristics provided by CTCA is able to detect with a moderate accuracy segments that will exhibit a significant plaque burden increase at mid-term follow-up.


Assuntos
Angioplastia Coronária com Balão/métodos , Angiografia por Tomografia Computadorizada/métodos , Simulação por Computador , Angiografia Coronária/métodos , Doença da Artéria Coronariana/diagnóstico por imagem , Lipoproteínas LDL/sangue , Síndrome Coronariana Aguda/diagnóstico por imagem , Síndrome Coronariana Aguda/terapia , Idoso , Análise de Variância , Angioplastia Coronária com Balão/efeitos adversos , Estudos de Coortes , Doença da Artéria Coronariana/terapia , Progressão da Doença , Feminino , Humanos , Processamento de Imagem Assistida por Computador , Modelos Logísticos , Masculino , Pessoa de Meia-Idade , Monitorização Fisiológica/métodos , Tomografia Computadorizada Multidetectores , Análise Multivariada , Valor Preditivo dos Testes , Curva ROC , Estudos Retrospectivos , Sensibilidade e Especificidade
14.
Lancet Infect Dis ; 16(6): 661-673, 2016 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-27107460

RESUMO

BACKGROUND: Carbapenems are frequently the last line of defence in serious infections due to multidrug-resistant Gram-negative bacteria, but their use is threatened by the growing prevalence of carbapenemase-producing pathogens. Ceftazidime-avibactam is a potential new agent for use in such infections. We aimed to assess the efficacy, safety, and tolerability of ceftazidime-avibactam compared with best available therapy in patients with complicated urinary tract infection or complicated intra-abdominal infection due to ceftazidime-resistant Gram-negative pathogens. METHODS: REPRISE was a pathogen-directed, international, randomised, open-label, phase 3 trial that recruited patients from hospitals across 16 countries worldwide. Eligible patients were aged 18-90 years with complicated urinary tract infection or complicated intra-abdominal infection caused by ceftazidime-resistant Enterobacteriaceae or Pseudomonas aeruginosa. Patients were randomised (1:1) to 5-21 days of treatment with either ceftazidime-avibactam (a combination of 2000 mg ceftazidime plus 500 mg avibactam, administered via a 2-h intravenous infusion every 8 h) or best available therapy. The primary endpoint was clinical response at the test-of-cure visit, 7-10 days after last infusion of study therapy, analysed in all patients who had at least one ceftazidime-resistant Gram-negative pathogen, as confirmed by the central laboratory, and who received at least one dose of study drug. Safety endpoints were assessed in all patients who received at least one dose of study drug. This study is registered with ClinicalTrials.gov, number NCT01644643. FINDINGS: Between Jan 7, 2013, and Aug 29, 2014, 333 patients were randomly assigned, 165 to ceftazidime-avibactam and 168 to best available therapy. Of these, 154 assigned to ceftazidime-avibactam (144 with complicated urinary tract infection and ten with complicated intra-abdominal infection) and 148 assigned to best available therapy (137 with complicated urinary tract infection and 11 with complicated intra-abdominal infection) were analysed for the primary outcome. 163 (97%) of 168 patients in the best available therapy group received a carbapenem, 161 (96%) as monotherapy. The overall proportions of patients with a clinical cure at the test-of-cure visit were similar with ceftazidime-avibactam (140 [91%; 95% CI 85·6-94·7] of 154 patients) and best available therapy (135 [91%; 85·9-95·0] of 148 patients). 51 (31%) of 164 patients in the ceftazidime-avibactam group and 66 (39%) of 168 in the best available therapy group had an adverse event, most of which were mild or moderate in intensity. Gastrointestinal disorders were the most frequently reported treatment-emergent adverse events with both ceftazidime-avibactam (21 [13%] of 164 patients) and best available therapy (30 [18%] of 168 patients). No new safety concerns were identified for ceftazidime-avibactam. INTERPRETATION: These results provide evidence of the efficacy of ceftazidime-avibactam as a potential alternative to carbapenems in patients with ceftazidime-resistant Enterobacteriaceae and P aeruginosa. FUNDING: AstraZeneca.


Assuntos
Compostos Azabicíclicos/administração & dosagem , Ceftazidima/administração & dosagem , Farmacorresistência Bacteriana Múltipla , Enterobacteriaceae/efeitos dos fármacos , Infecções Intra-Abdominais/tratamento farmacológico , Pseudomonas aeruginosa/efeitos dos fármacos , Infecções Urinárias/tratamento farmacológico , Inibidores de beta-Lactamases/uso terapêutico , Idoso , Idoso de 80 Anos ou mais , Antibacterianos/uso terapêutico , Compostos Azabicíclicos/efeitos adversos , Carbapenêmicos/uso terapêutico , Ceftazidima/efeitos adversos , Combinação de Medicamentos , Feminino , Bactérias Gram-Negativas/efeitos dos fármacos , Humanos , Infecções Intra-Abdominais/microbiologia , Masculino , Pessoa de Meia-Idade , Infecções Urinárias/microbiologia , Inibidores de beta-Lactamases/administração & dosagem
15.
Nat Commun ; 7: 12572, 2016 08 31.
Artigo em Inglês | MEDLINE | ID: mdl-27578622

RESUMO

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), An+1BnO3n+1, thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Srn+1TinO3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.

18.
ACS Macro Lett ; 3(6): 510-514, 2014 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-35590717

RESUMO

A significant limitation of rechargeable lithium-ion batteries arises because most of the ionic current is carried by the anion, the ion that does not participate in energy-producing reactions. Single-ion-conducting block copolymer electrolytes, wherein all of the current is carried by the lithium cations, have the potential to dramatically improve battery performance. The relationship between ionic conductivity and morphology of single-ion-conducting poly(ethylene oxide)-b-polystyrenesulfonyllithium(trifluoromethylsulfonyl)imide (PEO-PSLiTFSI) diblock copolymers was studied by small-angle X-ray scattering and ac impedance spectroscopy. At low temperatures, an ordered lamellar phase is obtained, and the "mobile" lithium ions are trapped in the form of ionic clusters in the glassy polystyrene-rich microphase. An increase in temperature results in a thermodynamic transition to a disordered phase. Above this transition temperature, the lithium ions are released from the clusters, and ionic conductivity increases by several orders of magnitude. This morphology-conductivity relationship is very different from all previously published data on published electrolytes. The ability to design electrolytes wherein most of the current is carried by the lithium ions, to sequester them in nonconducting domains and release them when necessary, has the potential to enable new strategies for controlling the charge-discharge characteristics of rechargeable lithium batteries.

19.
Nat Commun ; 5: 4867, 2014 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-25202857

RESUMO

Dislocations have a significant effect on mechanical, electronic, magnetic and optical properties of crystals. For a dislocation to migrate in bulk crystals, collective and simultaneous movement of several atoms is needed. In two-dimensional crystals, in contrast, dislocations occur on the surface and can exhibit unique migration dynamics. Dislocation migration has recently been studied in graphene, but no studies have been reported on dislocation dynamics for two-dimensional transition metal dichalcogenides with unique metal-ligand bonding and a three-atom thickness. This study presents dislocation motion, glide and climb, leading to grain boundary migration in a tungsten disulphide monolayer. Direct atomic-scale imaging coupled with atomistic simulations reveals a strikingly low-energy barrier for glide, leading to significant grain boundary reconstruction in tungsten disulphide. The observed dynamics are unique and different from those reported for graphene. Through strain field mapping, we also demonstrate how dislocations introduce considerable strain along the grain boundaries and at the dislocation cores.

20.
ACS Nano ; 6(2): 1589-600, 2012 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-22324447

RESUMO

The main objective of this work is to study charge transport in mixtures of poly(3-hexylthiophene)-b-poly(ethylene oxide) (P3HT-PEO) block copolymers and lithium bis(trifluoromethanesulfonyl) imide salt (LiTFSI). The P3HT-rich microphase conducts electronic charge, while the PEO-rich microphase conducts ionic charge. The nearly symmetric P3HT-PEO copolymer used in this study self-assembles into a lamellar phase. In contrast, the morphologies of asymmetric copolymers with P3HT as the major component are dominated by nanofibrils. A combination of ac and dc impedance measurements was used to determine the electronic and ionic conductivities of our samples. The ionic conductivities of P3HT-PEO/LiTFSI mixtures are lower than those of mixtures of PEO homopolymer and LiTFSI, in agreement with published data obtained from other block copolymer/salt mixtures. In contrast, the electronic conductivities of the asymmetric P3HT-PEO copolymers are significantly higher than those of the P3HT homopolymer. This is unexpected because of the presence of the nonelectronically conducting PEO microphase. This implies that the intrinsic electronic conductivity of the P3HT microphase in P3HT-PEO copolymers is significantly higher than that of P3HT homopolymers.


Assuntos
Condutividade Elétrica , Lítio/química , Polietilenoglicóis/química , Polímeros/química , Tiofenos/química , Transporte de Elétrons , Imidas/química , Espalhamento a Baixo Ângulo , Temperatura , Fatores de Tempo , Difração de Raios X
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