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1.
ACS Omega ; 4(3): 5442-5450, 2019 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-31459709

RESUMO

Single-crystalline SnSe has attracted much attention because of its record high figure-of-merit ZT ≈ 2.6; however, this high ZT has been associated with the low mass density of samples which leaves the intrinsic ZT of fully dense pristine SnSe in question. To this end, we prepared high-quality fully dense SnSe single crystals and performed detailed structural, electrical, and thermal transport measurements over a wide temperature range along the major crystallographic directions. Our single crystals were fully dense and of high purity as confirmed via high statistics 119Sn Mössbauer spectroscopy that revealed <0.35 at. % Sn(IV) in pristine SnSe. The temperature-dependent heat capacity (C p) provided evidence for the displacive second-order phase transition from Pnma to Cmcm phase at T c ≈ 800 K and a small but finite Sommerfeld coefficient γ0 which implied the presence of a finite Fermi surface. Interestingly, despite its strongly temperature-dependent band gap inferred from density functional theory calculations, SnSe behaves like a low-carrier-concentration multiband metal below 600 K, above which it exhibits a semiconducting behavior. Notably, our high-quality single-crystalline SnSe exhibits a thermoelectric figure-of-merit ZT ∼1.0, ∼0.8, and ∼0.25 at 850 K along the b, c, and a directions, respectively.

2.
Adv Mater ; 31(37): e1901077, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31339199

RESUMO

Twisting between two stacked monolayers modulates periodic potentials and forms the Moiré electronic superlattices, which offers an additional degree of freedom to alter material property. Considerable unique observations, including unconventional superconductivity, coupled spin-valley states, and quantized interlayer excitons are correlated to the electronic superlattices but further study requires reliable routes to study the Moiré in real space. Scanning tunneling microscopy (STM) is ideal to precisely probe the Moiré superlattice and correlate coupled parameters among local electronic structures, strains, defects, and band alignment at atomic scale. Here, a clean route is developed to construct twisted lattices using synthesized monolayers for fundamental studies. Diverse Moiré superlattices are predicted and successfully observed with STM at room temperature. Electrical tuning of the Moiré superlattice is achieved with stacked TMD on graphite.

3.
Ultramicroscopy ; 196: 180-185, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30423505

RESUMO

Scanning tunneling microscope (STM) is a powerful tool for studying the structural and electronic properties of materials at the atomic scale. The combination of low temperature and high magnetic field for STM and related spectroscopy techniques allows us to investigate the novel physical properties of materials at these extreme conditions with high energy resolution. Here, we present the construction and the performance of an ultrahigh vacuum 3He fridge-based STM system with a 7 Tesla superconducting magnet. It features a double deck sample stage on the STM head so we can clean the tip by field emission or prepare a spin-polarized tip in situ without removing the sample from the STM. It is also capable of in situ sample and tip exchange and preparation. The energy resolution of scanning tunneling spectroscopy at T = 310 mK is determined to be 400 mK by measuring the superconducting gap with a niobium tip on a gold surface. We demonstrate the performance of this STM system by imaging the bicollinear magnetic order of Fe1+xTe at T = 5 K.

4.
Nat Commun ; 9(1): 5431, 2018 12 21.
Artigo em Inglês | MEDLINE | ID: mdl-30575727

RESUMO

In a superconductor Cooper pairs condense into a single state and in so doing support dissipation free charge flow and perfect diamagnetism. In a magnetic field the minimum kinetic energy of the Cooper pairs increases, producing an orbital pair breaking effect. We show that it is possible to significantly quench the orbital pair breaking effect for both parallel and perpendicular magnetic fields in a thin film superconductor with lateral nanostructure on a length scale smaller than the magnetic length. By growing an ultra-thin (2 nm thick) single crystalline Pb nanowire network, we establish nm scale lateral structure without introducing weak links. Our network suppresses orbital pair breaking for both perpendicular and in-plane fields with a negligible reduction in zero-field resistive critical temperatures. Our study opens a frontier in nanoscale superconductivity by providing a strategy for maintaining pairing in strong field environments in all directions with important technological implications.

5.
ACS Nano ; 12(2): 1089-1095, 2018 02 27.
Artigo em Inglês | MEDLINE | ID: mdl-29384356

RESUMO

We map electronic states, band gaps, and interface-bound charges at termination-engineered BiFeO3/La0.7Sr0.3MnO3 interfaces using atomically resolved cross-sectional scanning tunneling microscopy. We identify a delicate interplay of different correlated physical effects and relate these to the ferroelectric and magnetic interface properties tuned by engineering the atomic layer stacking sequence at the interfaces. This study highlights the importance of a direct atomically resolved access to electronic interface states for understanding the intriguing interface properties in complex oxides.

6.
Nanotechnology ; 28(25): 255301, 2017 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-28548051

RESUMO

Focused ion beam (FIB) systems have become powerful diagnostic and modification tools for nanoscience and nanotechnology. Gas field ion sources (GFISs) built from atomic-size emitters offer the highest brightness among all ion sources and thus can improve the spatial resolution of FIB systems. Here we show that the Ir/W(111) single-atom tip (SAT) can emit high-brightness Xe+ ion beams with a high current stability. The ion emission current versus extraction voltage was analyzed from 150 K up to 309 K. The optimal emitter temperature for maximum Xe+ ion emission was ∼150 K and the reduced brightness at the Xe gas pressure of 1 × 10-4 torr is two to three orders of magnitude higher than that of a Ga liquid metal ion source, and four to five orders of magnitude higher than that of a Xe inductively coupled plasma ion source. Most surprisingly, the SAT emitter remained stable even when operated at 309 K. Even though the ion current decreased with increasing temperature, the current at room temperature (RT) could still reach over 1 pA when the gas pressure was higher than 1 × 10-3 torr, indicating the feasibility of RT-Xe-GFIS for application to FIB systems. The operation temperature of Xe-SAT-GFIS is considerably higher than the cryogenic temperature required for the helium ion microscope (HIM), which offers great technical advantages because only simple or no cooling schemes can be adopted. Thus, Xe-GFIS-FIB would be easy to implement and may become a powerful tool for nanoscale milling and secondary ion mass spectroscopy.

7.
Nano Lett ; 17(2): 1154-1160, 2017 02 08.
Artigo em Inglês | MEDLINE | ID: mdl-28094957

RESUMO

The presence of the PbI2 passivation layers at perovskite crystal grains has been found to considerably affect the charge carrier transport behaviors and device performance of perovskite solar cells. This work demonstrates the application of a novel light-modulated scanning tunneling microscopy (LM-STM) technique to reveal the interfacial electronic structures at the heterointerfaces between CH3NH3PbI3 perovskite crystals and PbI2 passivation layers of individual perovskite grains under light illumination. Most importantly, this technique enabled the first observation of spatially resolved mapping images of photoinduced interfacial band bending of valence bands and conduction bands and the photogenerated electron and hole carriers at the heterointerfaces of perovskite crystal grains. By systematically exploring the interfacial electronic structures of individual perovskite grains, enhanced charge separation and reduced back recombination were observed when an optimal design of interfacial PbI2 passivation layers consisting of a thickness less than 20 nm at perovskite crystal grains was applied.


Assuntos
Compostos de Cálcio , Chumbo/química , Imagem Óptica/métodos , Óxidos , Energia Solar , Titânio , Eletrônica , Ouro/química , Iluminação/métodos , Microscopia de Tunelamento/instrumentação , Propriedades de Superfície
8.
Nanotechnology ; 28(9): 095706, 2017 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-28135205

RESUMO

We elucidate that the tip sharpness in scanning tunneling microscopy (STM) can be characterized through the number of field-emission (FE) resonances. A higher number of FE resonances indicates higher sharpness. We observe empty quantum well (QW) states in Pb islands on Cu(111) under different tip sharpness levels. We found that QW states observed by sharper tips always had lower energies, revealing negative energy shifts. This sharpness-induced energy shift originates from an inhomogeneous electric field in the STM gap. An increase in sharpness increases the electric field inhomogeneity, that is, enhances the electric field near the tip apex, but weakens the electric field near the sample. As a result, higher sharpness can increase the electronic phase in vacuum, causing the lowering of QW state energies. Moreover, the behaviors of negative energy shift as a function of state energy are entirely different for Pb islands with a thickness of two and nine atomic layers. This thickness-dependent behavior results from the electrostatic force in the STM gap decreasing with increasing tip sharpness. The variation of the phase contributed from the expansion deformation induced by the electrostatic force in a nine-layer Pb island is significantly greater, sufficient to effectively negate the increase of electronic phase in vacuum.

9.
Adv Mater ; 28(41): 9142-9151, 2016 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-27571277

RESUMO

A novel artificially created MnO2 monolayer system is demonstrated in atomically controlled epitaxial perovskite heterostructures. With careful design of different electrostatic boundary conditions, a magnetic transition as well as a metal-insulator transition of the MnO2 monolayer is unveiled, providing a fundamental understanding of dimensionality-confined strongly correlated electron systems and a direction to design new electronic devices.

10.
Nano Lett ; 16(7): 4490-500, 2016 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-27351447

RESUMO

Dopants play a critical role in modulating the electric properties of semiconducting materials, ranging from bulk to nanoscale semiconductors, nanowires, and quantum dots. The application of traditional doping methods developed for bulk materials involves additional considerations for nanoscale semiconductors because of the influence of surfaces and stochastic fluctuations, which may become significant at the nanometer-scale level. Monolayer doping is an ex situ doping method that permits the post growth doping of nanowires. Herein, using atom-probe tomography (APT) with subnanometer spatial resolution and atomic-ppm detection limit, we study the distributions of boron and phosphorus in ex situ doped silicon nanowires with accurate control. A highly phosphorus doped outer region and a uniformly boron doped interior are observed, which are not predicted by criteria based on bulk silicon. These phenomena are explained by fast interfacial diffusion of phosphorus and enhanced bulk diffusion of boron, respectively. The APT results are compared with scanning tunneling spectroscopy data, which yields information concerning the electrically active dopants. Overall, comparing the information obtained by the two methods permits us to evaluate the diffusivities of each different dopant type at the nanowire oxide, interface, and core regions. The combined data sets permit us to evaluate the electrical activation and compensation of the dopants in different regions of the nanowires and understand the details that lead to the sharp p-i-n junctions formed across the nanowire for the ex situ doping process.

11.
Nanotechnology ; 27(17): 175705, 2016 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-26983371

RESUMO

Field emission (FE) resonance (or Gundlach oscillation) in scanning tunneling microscopy (STM) is a phenomenon in which the FE electrons emitted from the microscope tip couple into the quantized standing-wave states within the STM tunneling gap. Although the occurrence of FE resonance peaks can be semi-quantitatively described using the triangular potential well model, it cannot explain the experimental observation that the number of resonance peaks may change under the same emission current. This study demonstrates that the aforementioned variation can be adequately explained by introducing a field enhancement factor that is related to the local electric field at the tip apex. The peak number of FE resonances increases with the field enhancement factor. The peak intensity of the FE resonance on the reconstructed Au(111) surface varies in the face-center cubic, hexagonal-close-packed, and ridge regions, thus providing the contrast in the mapping through FE resonances. The mapping contrast is demonstrated to be nearly independent of the tip-sample distance, implying that the FE electron beam is not divergent because of a self-focus function intrinsically involved in the STM configuration.

12.
Sci Adv ; 2(11): e1600894, 2016 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-28138520

RESUMO

The search for topological superconductors (TSCs) is one of the most urgent contemporary problems in condensed matter systems. TSCs are characterized by a full superconducting gap in the bulk and topologically protected gapless surface (or edge) states. Within each vortex core of TSCs, there exists the zero-energy Majorana bound states, which are predicted to exhibit non-Abelian statistics and to form the basis of the fault-tolerant quantum computation. To date, no stoichiometric bulk material exhibits the required topological surface states (TSSs) at the Fermi level (EF) combined with fully gapped bulk superconductivity. We report atomic-scale visualization of the TSSs of the noncentrosymmetric fully gapped superconductor PbTaSe2. Using quasi-particle scattering interference imaging, we find two TSSs with a Dirac point at E ≅ 1.0 eV, of which the inner TSS and the partial outer TSS cross EF, on the Pb-terminated surface of this fully gapped superconductor. This discovery reveals PbTaSe2 as a promising candidate for TSC.

13.
Nanotechnology ; 26(5): 055705, 2015 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-25590566

RESUMO

Focused ion beam (FIB) deposition produces unwanted particle contamination beyond the deposition point. This is due to the FIB having a Gaussian distribution. This work investigates the spatial extent of this contamination and its influence on the electrical properties of nano-electronic devices. A correlation study is performed on carbon-nanotube (CNT) devices manufactured using FIB deposition. The devices are observed using transmission electron microscopy (TEM) and these images are correlated with device electrical characteristics. To discover how far Pt-nanoparticle contamination occurs along a CNT after FIB electrical contact deposition careful TEM inspections are performed. The results show FIB deposition efficiently improves electrical contact; however, the practice is accompanied by serious particle contamination near deposition points. These contaminants include metal particles and amorphous elements originating from precursor gases and residual water molecules in the vacuum chamber. Pt-contamination extends for approximately 2 µm from the point of FIB contact deposition. These contaminants cause current fluctuations and alter the transport characteristics of devices. It is recommended that nano-device fabrication occurs at a distance greater than 2 µm from the FIB deposition of an electrical contact.

14.
J Chem Phys ; 141(11): 114701, 2014 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-25240362

RESUMO

Using ultrahigh-vacuum low-temperature scanning tunneling microscopy and spectroscopy combined with first principles density functional theory calculations, we have investigated structural and electronic properties of pristine and potassium (K)-deposited picene thin films formed in situ on a Ag(111) substrate. At low coverages, the molecules are uniformly distributed with the long axis aligned along the [112̄] direction of the substrate. At higher coverages, ordered structures composed of monolayer molecules are observed, one of which is a monolayer with tilted and flat-lying molecules resembling a (11̄0) plane of the bulk crystalline picene. Between the molecules and the substrate, the van der Waals interaction is dominant with negligible hybridization between their electronic states; a conclusion that contrasts with the chemisorption exhibited by pentacene molecules on the same substrate. We also observed a monolayer picene thin film in which all molecules were standing to form an intermolecular π stacking. Two-dimensional delocalized electronic states are found on the K-deposited π stacking structure.

15.
ACS Nano ; 8(8): 8357-62, 2014 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-25030217

RESUMO

The bottom-up synthesis of nanoscale building blocks is a versatile approach for the formation of a vast array of materials with controlled structures and compositions. This approach is one of the main driving forces for the immense progress in materials science and nanotechnology witnessed over the past few decades. Despite the overwhelming advances in the bottom-up synthesis of nanoscale building blocks and the fine control of accessible compositions and structures, certain aspects are still lacking. In particular, the transformation of symmetric nanostructures to asymmetric nanostructures by highly controlled processes while preserving the modified structural orientation still poses a significant challenge. We present a one-step ex situ doping process for the transformation of undoped silicon nanowires (i-Si NWs) to p-type/n-type (p-n) parallel p-n junction configuration across NWs. The vertical p-n junctions were measured by scanning tunneling microscopy (STM) in concert with scanning tunneling spectroscopy (STS), termed STM/S, to obtain the spatial electronic properties of the junction formed across the NWs. Additionally, the parallel p-n junction configuration was characterized by off-axis electron holography in a transmission electron microscope to provide an independent verification of junction formation. The doping process was simulated to elucidate the doping mechanisms involved in the one-step p-i-n junction formation.

16.
Nanotechnology ; 25(25): 255703, 2014 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-24896069

RESUMO

We demonstrate that the Raman intensities of G and 2D bands of a suspended graphene can be enhanced using a gold tip with an apex size of 2.3 µm. The enhancement decays with the tip-graphene distance exponentially and remains detectable at a distance of 1.5 µm. Raman mappings show that the enhanced area is comparable to the apex size. Application of a bias voltage to the tip can attract the graphene so that Raman signals are intensified. The exponential enhancement-distance relationship enables the measurement of the graphene deformation, and the Young's modulus of graphene is estimated to be 1.48 TPa.

17.
Nanoscale ; 6(10): 5484-90, 2014 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-24728234

RESUMO

In this study we prepared molybdenum trioxide (MoO3) nanorods having average lengths of 0.5-1.5 µm and widths of approximately 100-200 nm through a one-step mechanical break-down process involving favorable fracturing along the crystal direction. We controlled the dimensions of the as-prepared nanorods by applying various imposing times (15-90 min). The nanorods prepared over a reaction time of 90 min were, on average, much shorter and narrower relative to those obtained over 30 min. Evaluations of lithium-ion storage properties revealed that the electrochemical performance of these nanorods was much better than that of bulk materials. As cathodes, the nanorods could deliver a high specific capacity (>315 mA h g(-1)) with losses of less than 2% in the first cycle at a rate of 30 mA g(-1); as anodes, the specific capacity was 800 mA h g(-1) at a rate of 50 mA g(-1). Relative to α-MoO3 microparticles, these nanorods displayed significantly enhanced lithium-ion storage properties with higher reversible capacities and better rate performance, presumably because their much shorter diffusion lengths and higher specific surface areas allowed more-efficient insertion/deinsertion of lithium ions during the charge/discharge process. Accordingly, enhanced physical and/or chemical properties can be obtained through appropriate nanostructuring of materials.

18.
ACS Nano ; 8(2): 1784-91, 2014 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-24471977

RESUMO

We demonstrate a polymer-free method that can routinely transfer relatively large-area graphene to any substrate with advanced electrical properties and superior atomic and chemical structures as compared to the graphene sheets transferred with conventional polymer-assisted methods. The graphene films that are transferred with polymer-free method show high electrical conductance and excellent optical transmittance. Raman spectroscopy and X-ray/ultraviolet photoelectron spectroscopy also confirm the presence of high quality graphene sheets with little contamination after transfer. Atom-resolved images can be obtained using scanning tunneling microscope on as-transferred graphene sheets without additional cleaning process. The mobility of the polymer-free graphene monolayer is as high as 63,000 cm(2) V(-1) s(-1), which is 50% higher than the similar sample transferred with the conventional method. More importantly, this method allows us to place graphene directly on top of devices made of soft materials, such as organic and polymeric thin films, which widens the applications of graphene in soft electronics.

19.
Anal Sci ; 29(9): 885-92, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24025572

RESUMO

Toxocarosis is a zoonosis caused by the transmission of the Toxocara canis (T. canis) larvae to humans. Its infectious third-stage larvae can invade the brains of paratenic hosts. The resultant brain damage can result in cerebral toxocarosis (CT). Astrocytes have important neurotrophic and neuroprotective functions in the brain. Substantial studies have shown that astrocyte apoptosis may contribute to the pathogenesis of many acute and chronic neurodegenerative disorders. We propose an alternation detection method, a combination of the astigmatic detection microscopy (ADM) and atomic force microscopy (AFM) techniques, to investigate the apoptosis of astrocytes triggered with T. canis larval excretory/secretory (Tc E/S) antigen. The variation in the pathology of a cell's morphological changes was investigated with ADM and AFM analyses and then confirmed by western blotting. The results showed that the round cells increased as the concentration of Tc E/S antigen and incubated time increased. In addition, the mean height of apoptotic cells was approximately twice that of untreated normal cells, which meant there was correlation between the Tc E/S antigen treatment and cell height. For each cleaved caspase-3 in the cells cocultured with Tc E/S antigen and incubated for 9 h, the corresponding intensities increased about 34-fold (34.4 ± 1.8) compared with those of the control cells. This method can provide researchers with a perspective for understanding the limited information on the mechanism of astroglial injury and death during a T. canis larval invasion in a brain infection.


Assuntos
Antígenos de Helmintos/imunologia , Apoptose/imunologia , Astrócitos/citologia , Astrócitos/imunologia , Encefalopatias/parasitologia , Toxocara canis/imunologia , Toxocaríase/parasitologia , Animais , Antígenos de Helmintos/química , Encefalopatias/imunologia , Células Cultivadas , Ratos , Toxocara canis/química , Toxocaríase/imunologia
20.
ACS Appl Mater Interfaces ; 5(15): 7509-16, 2013 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-23834261

RESUMO

To develop a drug delivery system (DDS), it is critical to address challenging tasks such as the delivery of hydrophobic and amphiphilic compounds, cell uptake, and the metabolic fate of the drug delivery carrier. Low-density lipoprotein (LDL) has been acknowledged as the human serum transporter of natively abundant lipoparticles such as cholesterol, triacylglycerides, and lipids. Apolipoprotein B (apo B) is the only protein contained in LDL, and possesses a binding moiety for the LDL receptor that can be internalized and degraded naturally by the cell. Therefore, synthetic/reconstituting apoB lipoparticle (rABL) could be an excellent delivery carrier for hydrophobic or amphiphilic materials. Here, we synthesized rABL in vitro, using full-length apoB through a five-step solvent exchange method, and addressed its potential as a DDS. Our rABL exhibited good biocompatibility when evaluated with cytotoxicity and cell metabolic response assays, and was stable during storage in phosphate-buffered saline at 4 °C for several months. Furthermore, hydrophobic superparamagnetic iron oxide nanoparticles (SPIONPs) and the anticancer drug M4N (tetra-O-methyl nordihydroguaiaretic acid), used as an imaging enhancer and lipophilic drug model, respectively, were incorporated into the rABL, leading to the formation of SPIONPs- and M4N- containing rABL (SPIO@rABL and M4N@rABL, respectively). Fourier transform infrared spectroscopy suggested that rABL has a similar composition to that of LDL, and successfully incorporated SPIONPs or M4N. SPIO@rABL presented significant hepatic contrast enhancement in T2-weighted magnetic resonance imaging in BALB/c mice, suggesting its potential application as a medical imaging contrast agent. M4N@rABL could reduce the viability of the cancer cell line A549. Interestingly, we developed solution-phase high-resolution transmission electron microscopy to observe both LDL and SPIO@rABL in the liquid state. In summary, our LDL-based DDS, rABL, has significant potential as a novel DDS for hydrophobic and amphiphilic materials, with good cell internalization properties and metabolicity.


Assuntos
Apolipoproteínas B/química , Sistemas de Liberação de Medicamentos , Lipoproteínas/química , Animais , Antineoplásicos/administração & dosagem , Materiais Biocompatíveis , Linhagem Celular Tumoral , Química Farmacêutica/métodos , Colesterol/química , Compostos Férricos/química , Interações Hidrofóbicas e Hidrofílicas , Magnetismo , Teste de Materiais , Camundongos , Camundongos Endogâmicos BALB C , Microscopia Eletrônica de Transmissão/métodos , Microscopia de Fluorescência/métodos , Nanopartículas/química , Nanotecnologia/métodos , Espectroscopia de Infravermelho com Transformada de Fourier/métodos , Tensoativos/química , Fatores de Tempo
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