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We report the first study on the thermal behavior of the stiffness of individual carbon nanotubes, which is achieved by measuring the resonance frequency of their fundamental mechanical bending modes. We observe a reduction of the Young's modulus over a large temperature range with a slope -(173±65) ppm/K in its relative shift. These findings are reproduced by two different theoretical models based on the thermal dynamics of the lattice. These results reveal how the measured fundamental bending modes depend on the phonons in the nanotube via the Young's modulus. An alternative description based on the coupling between the measured mechanical modes and the phonon thermal bath in the Akhiezer limit is discussed.
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Progress in nanotechnology requires new approaches to materials synthesis that make it possible to control material functionality down to the smallest scales. An objective of materials research is to achieve enhanced control over the physical properties of materials such as ferromagnets, ferroelectrics and superconductors. In this context, complex oxides and inorganic perovskites are attractive because slight adjustments of their atomic structures can produce large physical responses and result in multiple functionalities. In addition, these materials often contain ferroelastic domains. The intrinsic symmetry breaking that takes place at the domain walls can induce properties absent from the domains themselves, such as magnetic or ferroelectric order and other functionalities, as well as coupling between them. Moreover, large domain wall densities create intense strain gradients, which can also affect the material's properties. Here we show that, owing to large local stresses, domain walls can promote the formation of unusual phases. In this sense, the domain walls can function as nanoscale chemical reactors. We synthesize a two-dimensional ferromagnetic phase at the domain walls of the orthorhombic perovskite terbium manganite (TbMnO3), which was grown in thin layers under epitaxial strain on strontium titanate (SrTiO3) substrates. This phase is yet to be created by standard chemical routes. The density of the two-dimensional sheets can be tuned by changing the film thickness or the substrate lattice parameter (that is, the epitaxial strain), and the distance between sheets can be made as small as 5 nanometres in ultrathin films, such that the new phase at domain walls represents up to 25 per cent of the film volume. The general concept of using domain walls of epitaxial oxides to promote the formation of unusual phases may be applicable to other materials systems, thus giving access to new classes of nanoscale materials for applications in nanoelectronics and spintronics.
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We report on a nanomechanical engineering method to monitor matter growth in real time via e-beam electromechanical coupling. This method relies on the exceptional mass sensing capabilities of nanomechanical resonators. Focused electron beam-induced deposition (FEBID) is employed to selectively grow platinum particles at the free end of singly clamped nanotube cantilevers. The electron beam has two functions: it allows both to grow material on the nanotube and to track in real time the deposited mass by probing the noise-driven mechanical resonance of the nanotube. On the one hand, this detection method is highly effective as it can resolve mass deposition with a resolution in the zeptogram range; on the other hand, this method is simple to use and readily available to a wide range of potential users because it can be operated in existing commercial FEBID systems without making any modification. The presented method allows one to engineer hybrid nanomechanical resonators with precisely tailored functionalities. It also appears as a new tool for studying the growth dynamics of ultrathin nanostructures, opening new opportunities for investigating so far out-of-reach physics of FEBID and related methods.
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Performing magnetization studies on individual nanoparticles is a highly demanding task, especially when measurements need to be carried out under large sweeping magnetic fields or variable temperature. Yet, characterization under varying ambient conditions is paramount in order to fully understand the magnetic behavior of these objects, e.g., the formation of nonuniform states or the mechanisms leading to magnetization reversal and thermal stability. This, in turn, is necessary for the integration of magnetic nanoparticles and nanowires into useful devices, e.g., spin-valves, racetrack memories, or magnetic tip probes. Here, we show that nanosuperconducting quantum interference devices based on high critical temperature superconductors are particularly well suited for this task. We have successfully characterized a number of individual Co nanowires grown through focused electron beam induced deposition and subsequently annealed at different temperatures. Magnetization measurements performed under sweeping magnetic fields (up to â¼100 mT) and variable temperature (1.4-80 K) underscore the intrinsic structural and chemical differences between these nanowires. These point to significant changes in the crystalline structure and the resulting effective magnetic anisotropy of the nanowires, and to the nucleation and subsequent vanishing of antiferromagnetic species within the nanowires annealed at different temperatures.
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Using focused electron-beam-induced deposition, we fabricate a vertical, platinum-coated cobalt nanowire with a controlled three-dimensional structure. The latter is engineered to feature bends along the height: these are used as pinning sites for domain walls, which are obtained at remanence after saturation of the nanostructure in a horizontally applied magnetic field. The presence of domain walls is investigated using x-ray magnetic circular dichroism (XMCD) coupled to photoemission electron microscopy (PEEM). The vertical geometry of our sample combined with the low incidence of the x-ray beam produce an extended wire shadow which we use to recover the wire's magnetic configuration. In this transmission configuration, the whole sample volume is probed, thus circumventing the limitation of PEEM to surfaces. This article reports on the first study of magnetic nanostructures standing perpendicular to the substrate with XMCD-PEEM. The use of this technique in shadow mode enabled us to confirm the presence of a domain wall without direct imaging of the nanowire.
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LaNiO3 (LNO) thin films of 14 nm and 35 nm thicknesses grown epitaxially on LaAlO3 (LAO) and (LaAlO3)0.3(Sr2TaAlO6)0.7 (LSAT) substrates are studied using High Resolution Transmission Electron Microscopy (HRTEM) and High Angle Annular Dark Field (HAADF) imaging. The strain state of the films is studied using Geometric Phase Analysis (GPA). Results show the successful in-plane adaptation of the films to the substrates, both in the compressive (LAO) and tensile (LSAT) cases. Through the systematic analysis of HRTEM superstructure contrast modulation along different crystal orientations, localized regions of the monoclinic LaNiO2.5 phase are detected in the 35 nm films.
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We report thermoelectric power experiments in e-doped thin films of SrTiO3 (STO) which demonstrate that the electronic band degeneracy can be lifted through defect management during growth. We show that even small amounts of cationic vacancies, combined with epitaxial stress, produce a homogeneous tetragonal distortion of the films, resulting in a Kondo-like resistance upturn at low temperature, large anisotropic magnetoresistance, and nonlinear Hall effect. Ab initio calculations confirm a different occupation of each band depending on the degree of tetragonal distortion. The phenomenology reported in this Letter for tetragonally distorted e-doped STO thin films, is similar to that observed in LaAlO3/STO interfaces and magnetic STO quantum wells.
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Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-in-nanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells.
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Remanent state and magnetization reversal processes of a series of cobalt antidot arrays with a fixed hole diameter (d ≈ 55 nm) and an array periodicity (p) ranging between 95 and 524 nm were studied by in situ Lorentz microscopy (LM) as a function of the magnetic field. At remanence, defocused LM images showed the periodicity dependence of the magnetic states inside the lattice. A remarkable transition was observed in the type of domain structures as a function of p: for the large periodicities (p > 300 nm), conventional 90° and 180° domain walls were formed, whereas in small-period antidot arrays (p ⦠160 nm) magnetic superdomain walls (SDWs) were nucleated to separate regions with different average magnetization direction, the so-called magnetic superdomains. In the SDW regime, a low-frequency Fourier filtering method was implemented to allow a quantitative analysis of the LM images by the transport of intensity equation method. In situ LM experiments under applied magnetic fields were performed to study the reversal magnetization process in a particular array (p = 160 nm), and clear differences were observed as a function of the magnetic field orientation. The switching process under magnetic fields parallel to the horizontal antidot rows occurs in two stages: the system first nucleates and propagates horizontal SDWs, parallel to the field. Then, at higher magnetic fields, vertical SDWs, perpendicular to the field, appear before saturation. When the magnetic field is applied at 45° with respect to the antidot rows, both horizontal and vertical SDWs are nucleated and propagated simultaneously. All the experiments were successfully correlated with micromagnetic simulations. The current study sheds new light on the magnetization reversal processes of antidot arrays and opens new possibilities of exploiting the potential of high-resolution in situ LM and new data analysis procedures to probe magnetization processes in nanomagnetism, particularly in periodic arrays of nanomagnets.
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Boosting large-scale superconductor applications require nanostructured conductors with artificial pinning centres immobilizing quantized vortices at high temperature and magnetic fields. Here we demonstrate a highly effective mechanism of artificial pinning centres in solution-derived high-temperature superconductor nanocomposites through generation of nanostrained regions where Cooper pair formation is suppressed. The nanostrained regions identified from transmission electron microscopy devise a very high concentration of partial dislocations associated with intergrowths generated between the randomly oriented nanodots and the epitaxial YBa(2)Cu(3)O(7) matrix. Consequently, an outstanding vortex-pinning enhancement correlated to the nanostrain is demonstrated for four types of randomly oriented nanodot, and a unique evolution towards an isotropic vortex-pinning behaviour, even in the effective anisotropy, is achieved as the nanostrain turns isotropic. We suggest a new vortex-pinning mechanism based on the bond-contraction pairing model, where pair formation is quenched under tensile strain, forming new and effective core-pinning regions.
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Applications based on the movement of domain walls (DWs) in magnetic nanowires (NWs) require a good DW conduit behavior, i.e. a significant difference between DW nucleation and propagation fields. In this work, we have systematically studied how this property evolves in cobalt NWs grown by focused electron beam induced deposition (FEBID) as a function of global gallium irradiation, for irradiation doses up to 1.24 × 10(17) ions cm(-2). Whereas for high doses the DW conduit is lost, below 6.42 × 10(15) ions cm(-2) the difference between the two fields increases with irradiation, becoming up to â¼9 times larger than for non-irradiated wires, due to a strong increase in the nucleation field, while the propagation field remains approximately constant. This behavior stems from two effects. The first effect is a decrease in the magnetic volume of the parasitic halo around the NW, typically present in FEBID nanostructures, leading to the disappearance of weak nucleation centers. The second effect is the formation of a 20 nm outer shell with Co crystals about twice the size of those forming the NW core, causing a net increase of the local magnetocrystalline anisotropy. The results presented here are important for the potential use of magnetic NWs grown by FEBID in DW-based devices, and might also be of interest for magnetic NWs fabricated by other techniques.
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Strain engineering enables modification of the properties of thin films using the stress from the substrates on which they are grown. Strain may be relaxed, however, and this can also modify the properties thanks to the coupling between strain gradient and polarization known as flexoelectricity. Here we have studied the strain distribution inside epitaxial films of the archetypal ferroelectric PbTiO(3), where the mismatch with the substrate is relaxed through the formation of domains (twins). Synchrotron X-ray diffraction and high-resolution scanning transmission electron microscopy reveal an intricate strain distribution, with gradients in both the vertical and, unexpectedly, the horizontal direction. These gradients generate a horizontal flexoelectricity that forces the spontaneous polarization to rotate away from the normal. Polar rotations are a characteristic of compositionally engineered morphotropic phase boundary ferroelectrics with high piezoelectricity; flexoelectricity provides an alternative route for generating such rotations in standard ferroelectrics using purely physical means.
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Magnetic properties of Au nanoparticles deposited on an archaeal S layer are reported. X-ray magnetic circular dichroism and superconducting quantum interference device magnetometries demonstrate that the particles are strongly paramagnetic, without any indication of magnetic blocking down to 16 mK. The average magnetic moment per particle is M(part)=2.36(7) µ(B). This contribution originates at the particle's Au 5d band, in which an increased number of holes with respect to the bulk value is observed. The magnetic moment per Au atom is 25 times larger than any measured in other Au nanoparticles or any other configurations up to date.
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Ultra-small magnetic nanoparticles consisting of NiCo and FeNi alloys enclosed within graphitic shells (NiCo/G and FeNi/G) have been synthesized. The particles, which retained the face centered cubic (fcc) symmetry of the original bulk metals, together with the graphitic coating were characterized by means of aberration corrected scanning transmission electron microscopy (STEM), obtaining mean particle sizes of 2.6 nm and 6.2 nm for NiCo/G and FeNi/G, respectively. Due to the enhancement of the thermal stability by the graphite shell, the graphite coated FeNi and NiCo were stable under oxygen atmosphere up to 170 °C. The effectiveness of the graphite shell was confirmed when unprotected bimetallic FeNi and NiCo were prepared and chemical characterization revealed that more than 60 at.% of the samples was oxygen due to the massive oxidation of the bimetallic nanoparticles.
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Grafite/química , Nanopartículas de Magnetita/química , Metais/química , Substâncias Macromoleculares/química , Campos Magnéticos , Teste de Materiais , Conformação Molecular , Propriedades de SuperfícieRESUMO
We report magnetic, dynamic and transport properties of discontinuous metal-insulator multilayers Fe/MgO grown on amorphous Corning glass and single-crystalline MgO (001) substrates. The films of structure Substrate/MgO (3 nm)/[Fe (0.6 nm)/MgO (3.0 nm)] x 10 were prepared in ultra-high vacuum conditions using Pulsed Laser Deposition. It was shown that conditions of epitaxial growth are favorable for MgO substrates. As a result a substantial increase of tunneling magnetoresistance caused by spin-filtering effect was observed and reasonably theoretically explained. The value of TMR - 9.2% at room temperature in 18 kOe magnetic field is three times higher comparing to that for the samples grown on Corning glass substrates.
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High-resolution monochromated electron energy loss spectroscopy (EELS) at subnanometric spatial resolution and <200 meV energy resolution has been used to assess the valence band properties of a distributed Bragg reflector multilayer heterostructure composed of InAlN lattice matched to GaN. This work thoroughly presents the collection of methods and computational tools put together for this task. Among these are zero-loss-peak subtraction and nonlinear fitting tools, and theoretical modeling of the electron scattering distribution. EELS analysis allows retrieval of a great amount of information: indium concentration in the InAlN layers is monitored through the local plasmon energy position and calculated using a bowing parameter version of Vegard Law. Also a dielectric characterization of the InAlN and GaN layers has been performed through Kramers-Kronig analysis of the Valence-EELS data, allowing band gap energy to be measured and an insight on the polytypism of the GaN layers.
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Titanium is a relevant technological material due to its extraordinary mechanical and biocompatible properties, its nanopatterning being an increasingly important requirement in many applications. We report the successful nanopatterning of titanium by means of focused electron beam induced etching using XeF(2) as a precursor gas. Etch rates up to 1.25 × 10(-3) µm(3) s(-1) and minimum pattern sizes of 80 nm were obtained. Different etching parameters such as beam current, beam energy, dwell time and pixel spacing are systematically investigated, the etching process being optimized by decreasing both the beam current and the beam energy. The etching mechanism is investigated by transmission electron microscopy. Potential applications in nanotechnology are discussed.
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We systematically study the effect of oxygen content on the magneto-transport and microstructure of Fe:O:C nanowires deposited by focused-electron-beam-induced (FEBID) deposition. The Fe/O ratio can be varied with an Fe content varying between â¼ 50 and 80 at.% with overall low C content (≈16 ± 3 at.%) by adding H(2)O during the deposition while keeping the beam parameters constant as measured by energy dispersive x-ray (EDX) spectroscopy. The room-temperature magnetic properties for deposits with an Fe content of 66-71 at.% are investigated using the magneto-optical Kerr effect (MOKE) and electric magneto-transport measurements. The nanostructure of the deposits is investigated through cross-sectional high-resolution transmission electron microscopy (HRTEM) imaging, allowing us to link the observed magneto-resistance and resistivity to the transport mechanism in the deposits. These results demonstrate that functional magnetic nanostructures can be created, paving the way for new magnetic or even spintronics devices.
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Monodispersed Fe3O4 nanoparticles with comparable size distributions have been synthesized by two different synthesis routes, co-precipitation and thermal decomposition. Thanks to the different steric stabilizations, the described samples can be considered as a model system to investigate the effects of magnetic dipolar interactions on the aggregation states of the nanoparticles. Moreover, the presence of magnetic dipolar interactions can strongly affect the nanoparticle efficiency as a hyperthermic mediator. In this paper, we present a novel way to visualize and map the magnetic dipolar interactions in different kinds of nanoparticle aggregates by the use of Lorentz microscopy, an easy and reliable in-line electron holographic technique. By exploiting Lorentz microscopy, which is complementary to the magnetic measurements, it is possible to correlate the interaction degrees of magnetic nanoparticles with their magnetic behaviors. In particular, we demonstrate that Lorentz microscopy is successful in visualizing the magnetic configurations stabilized by dipolar interactions, thus paving the way to the comprehension of the power loss mechanisms for different nanoparticle aggregates.
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Nanopartículas de Magnetita/química , Microscopia/métodos , Holografia , Temperatura Alta , Campos MagnéticosRESUMO
The Rashba effect is an interaction between the spin and the momentum of electrons induced by the spin-orbit coupling (SOC) in surface or interface states. Its potential for conversion between charge and spin currents has been theoretically predicted but never clearly demonstrated for surfaces or interfaces of metals. Here we present experiments evidencing a large spin-charge conversion by the Bi/Ag Rashba interface. We use spin pumping to inject a spin current from a NiFe layer into a Bi/Ag bilayer and we detect the resulting charge current. As the charge signal is much smaller (negligible) with only Bi (only Ag), the spin-to-charge conversion can be unambiguously ascribed to the Rashba coupling at the Bi/Ag interface. This result demonstrates that the Rashba effect at interfaces can be used for efficient charge-spin conversion in spintronics.