Phase plates (PPs) in transmission electron microscopy (TEM) improve the contrast of weakly scattering objects under in-focus imaging conditions. A well-established PP type is the Zernike (Z)PP, which consists of a thin amorphous carbon (aC) film with a microscaled hole in the centre. The mean inner potential of the aC film is exploited to shift the phase of the scattered electrons while the unscattered electrons in the zero-order beam propagate through the hole and remain unaffected. However, the abrupt thickness increase at the hole edge induces an abrupt change of the phase-shift distribution and leads to fringing, that is, intensity oscillations around imaged objects, in TEM images. In this work, we have used focused-ion-beam milling to fabricate ZPPs with abrupt and graded thickness profiles around the centre hole. Depending on the thickness gradient and inner hole radius, graded-ZPP-TEM images of an aC/vacuum interface and bundles of carbon nanotubes (CNTs) show strongly reduced fringing. Image simulations were performed with ZPP-phase-shift distributions derived from measured thickness profiles of graded ZPPs, which show good agreement with the experimental images. Fringing artefacts, that is, intensity oscillations around imaged objects, are strongly reduced for Zernike phase plates with a graded thickness profile around the centre hole. Focused-ion-beam milling is used to fabricate graded Zernike phase plates with specific inner hole radius and thickness gradients. The phase-shift distribution is obtained from measured thickness profiles around the centre hole. Image simulations based on experimentally measured thickness/phase-shift distributions show good agreement with experimental Zernike phase-plate TEM images.
In light optics, beams with orbital angular momentum (OAM) can be produced by employing a properly-tuned two-cylinder-lens arrangement, also called π/2 mode converter. It is not possible to convey this concept directly to the beam in an electron microscope due to the non-existence of cylinder lenses in commercial transmission electron microscopes (TEMs). A viable work-around are readily-available electron optical elements in the form of quadrupole lenses. In a proof-of-principle experiment in 2012, it has been shown that a single quadrupole in combination with a Hilbert phase-plate produces a spatially-confined, transient vortex mode. Here, an analogue to an optical π/2 mode converter is realized by repurposing a CEOS DCOR probe corrector in an aberration corrected TEM in a way that it resembles a dual cylinder lens using two quadrupoles. In order to verify the presence of OAM in the output beam, a fork dislocation grating is used as an OAM analyser. The possibility to use magnetic quadrupole fields instead of, e.g., prefabricated fork dislocation gratings to produce electron beams carrying OAM enhances the beam brightness by almost an order of magnitude and delivers switchable high-mode purity vortex beams without unwanted side-bands.
For quantitative electron microscopy the comparison of measured and simulated data is essential. Monte Carlo (MC) simulations are well established to calculate the high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) intensities on a non-atomic scale. In this work we focus on the importance of the screening parameter in differential screened Rutherford cross-sections for MC simulations and on the contribution of the screening parameter to the atomic-number dependence of the HAADF-STEM intensity at electron energies ≤ 30 keV. Materials investigated were chosen to cover a wide range of atomic numbers Z to study the Z dependence of the screening parameter. Comparison of measured and simulated HAADF-STEM intensities with different screening parameters known from the literature were tested and failed to generally describe the experimental data. Hence, the screening parameter was adapted to obtain the best match between experimental and MC-simulated HAADF-STEM intensities. The Z dependence of the HAADF-STEM intensity was derived.
Scanning transmission electron microscopy (STEM) at low primary electron energies has received increasing attention in recent years because knock-on damage can be avoided and high contrast for weakly scattering materials is obtained. However, the broadening of the electron beam in the sample is pronounced at low electron energies, which degrades resolution and limits the maximum specimen thickness. In this work, we have studied electron beam broadening in materials with atomic numbers Z between 10 and 32 (MgO, Si, SrTiO3 , Ge) and thicknesses up to 900 nm. Beam broadening is directly measured using a multisegmented STEM detector installed in a scanning electron microscope at electron energies between 15 and 30 keV. For experimental reasons, the electron beam diameter is defined to contain only 68% of the total intensity instead of the commonly used 90% of the total beam intensity. The measured beam diameters can be well described with calculated ones based on a recently published model by Gauvin and Rudinsky. Using the concept of anomalous diffusion the Hurst exponent H is introduced that varies between 0.5 and 1 for different scattering regimes depending on t/Λel with the specimen thickness t and the elastic mean free path length Λel . The calculations also depend on the fraction of the beam intensity that defines the electron beam diameter. A Hurst exponent H of 1 is characteristic for the ballistic scattering regime with t/Λel â 0 and can be excluded for the experimental conditions of our study with 6 ⦠t/Λel ⦠30. We deduced H = 0.75 from measured beam diameters which is larger than H = 0.5 that is expected under diffusion conditions. The deviation towards larger H values can be rationalised by our definition of electron diameter that contains only 68% of the total beam intensity and requires therefore larger sample thicknesses before the diffusion regime is reached. Our results clearly deviate from previous analytical approaches to describe beam broadening (Goldstein et al., Reed, Williams et al., Kohl and Reimer). Measured beam diameters are compared with simulated ones, which are obtained by solving the electron transport equation. This approach is advantageous compared to the commonly used Monte Carlo simulations because it is an exact solution of the electron transport equation and requires less computer time. Simulated beam diameter agree well with the experimental data and yield H = 0.80. LAY DESCRIPTION: In scanning transmission electron microscopy (STEM), a focused electron beam is scanned over an electron-transparent sample and an image is formed by detecting the intensity of the transmitted electrons by a STEM detector. STEM resolution is ultimately limited by the electron beam diameter and can be better than 0.1 nm for the best microscopes. However, the electron-beam diameter increases with increasing specimen thickness because electrons are scattered by the interaction of the specimen material and electrons. Electron scattering leads to a change of the electron propagation direction and reduces focusing of the electron beam. The associated electron-beam broadening degrades the lateral resolution of STEM and generally limits the maximum specimen thickness that can be imaged with good resolution. STEM is up to now mainly performed at high electron energies of 80 keV and above. Lower electron energies are beneficial for the study of weakly scattering and radiation-sensitive materials but electron beam broadening becomes more pronounced with decreasing electron energies. Knowledge of beam broadening is therefore particularly important for the interpretation of STEM images that are taken with low-energy electrons. In this work we have studied electron-beam broadening in different materials with thicknesses up to 900 nm at low electron energies between 15 and 30 keV. Beam broadening is directly measured with a newly developed technique. We compare measured beam diameters with different models on beam broadening from literature and find that only a recently published model is well suited to describe the experimental results under our experimental conditions. In addition, beam broadening is simulated by modelling electron propagation in the specimen. The simulation results agree well with the measured beam diameters.
This work is concerned with Al/Al-oxide(AlOx)/Al-layer systems which are important for Josephson-junction-based superconducting devices such as quantum bits. The device performance is limited by noise, which has been to a large degree assigned to the presence and properties of two-level tunneling systems in the amorphous AlOx tunnel barrier. The study is focused on the correlation of the fabrication conditions, nanostructural and nanochemical properties and the occurrence of two-level tunneling systems with particular emphasis on the AlOx-layer. Electron-beam evaporation with two different processes and sputter deposition were used for structure fabrication, and the effect of illumination by ultraviolet light during Al-oxide formation is elucidated. Characterization was performed by analytical transmission electron microscopy and low-temperature dielectric measurements. We show that the fabrication conditions have a strong impact on the nanostructural and nanochemical properties of the layer systems and the properties of two-level tunneling systems. Based on the understanding of the observed structural characteristics, routes are suggested towards the fabrication of Al/AlOx/Al-layers systems with improved properties.
Thin-film phase plates (PP) have become a valuable tool for the imaging of organic objects in transmission electron microscopy (TEM). The thin film usually consists of amorphous carbon (aC), which undergoes rapid aging under intense illumination with high-energy electrons. The limited lifetime of aC film PPs calls for alternative PP materials with improved material stability. This work presents thin-film PPs fabricated from the metallic glass alloy Zr0.65Al0.075Cu0.275 (ZAC), which was identified as a promising PP material with beneficial properties, such as a large inelastic mean free path. An adverse effect of the ZAC alloy is the formation of a surface oxide layer in ambient air, which reduces the electrical conductivity and causes electrostatic charging in the electron beam. To avoid surface oxidation, the ZAC alloy is enclosed by thin aC layers. The resulting aC/ZAC/aC layer system is used to fabricate Zernike and Hilbert PPs. Phase-contrast TEM imaging is demonstrated for a sample of carbon nanotubes, which show strong contrast enhancement in PP TEM images.
Resolution in scanning transmission electron microscopy (STEM) is ultimately limited by the diameter of the electron beam. The electron beam diameter is not only determined by the properties of the condenser lens system but also by electron scattering in the specimen which leads to electron-beam broadening and degradation of the resolution with increasing specimen thickness. In this work we introduce a new method to measure electron-beam broadening which is based on STEM imaging with a multi-segmented STEM detector. We focus on STEM at low electron energies between 10 and 30â¯keV and use an amorphous carbon film with known thickness as test object. The experimental results are compared with calculated beam diameters using different analytical models and Monte-Carlo simulations. We find excellent agreement of the experimental data with the recently published model by Gauvin and Rudinsky [1] for small t/λel (thickness to elastic mean free path) values which are considered in our study.
Gadolinium carbonate (Gd2(CO3)3) hollow nanospheres and their suitability for drug transport and magnetothermally-induced drug release are presented. The hollow nanospheres are prepared via a microemulsion-based synthesis using tris(tetramethylcyclopentadienyl)gadolinium(iii) and CO2 as the starting materials. Size, structure and composition of the as-prepared Gd2(CO3)3 hollow nanospheres are comprehensively validated by several independent analytical methods (HRTEM, HAADF-STEM, DLS, EDXS, XRD, FT-IR, DTA-TG). Accordingly, they exhibit an outer diameter of 26 ± 4 nm, an inner cavity of 7 ± 2 nm, and a wall thickness of 9 ± 3 nm. As a conceptual study, the nanocontainer-functionality of the Gd2(CO3)3 hollow nanospheres is validated upon filling with the anti-cancerogenic agent doxorubicin (DOX), which is straightforward via the microemulsion (ME) strategy. The resulting DOX@Gd2(CO3)3 nanocontainers provide the option of multimodal imaging including optical and magnetic resonance imaging (OI, MRI) as well as magnetothermal heating and drug release. As a proof-of-concept, we could already prove the intrinsic DOX-based fluorescence, a low systemic toxicity according to in vitro studies as well as the magnetothermal effect and a magnetothermally-induced DOX release. In particular, the latter is new for Gd-containing nanoparticles and highly promising in view of theranostic nanocontainers and synergistic physical and chemical tumor treatment.
Carbonates , Drug Carriers/chemistry , Drug Liberation , Gadolinium , Nanospheres , Doxorubicin/administration & dosage , Spectroscopy, Fourier Transform Infrared
The contrast of backscattered electron (BSE) images in scanning electron microscopy (SEM) depends on material parameters which can be exploited for composition quantification if some information on the material system is available. As an example, the In-concentration in thin InxGa1-xAs layers embedded in a GaAs matrix is analyzed in this work. The spatial resolution of the technique is improved by using thin electron-transparent specimens instead of bulk samples. Although the BSEs are detected in a comparably small angular range by an annular semiconductor detector, the image intensity can be evaluated to determine the composition and local thickness of the specimen. The measured intensities are calibrated within one single image to eliminate the influence of the detection and amplification system. Quantification is performed by comparison of experimental and calculated data. Instead of using time-consuming Monte-Carlo simulations, an analytical model is applied for BSE-intensity calculations which considers single electron scattering and electron diffusion.
Backscattered electron imaging of HT29 colon carcinoma cells in a scanning electron microscope was studied. Thin cell sections were placed on indium-tin-oxide-coated glass slides, which is a promising substrate material for correlative light and electron microscopy. The ultrastructure of HT29 colon carcinoma cells was imaged without poststaining by exploiting the high chemical sensitivity of backscattered electrons. Optimum primary electron energies for backscattered electron imaging were determined which depend on the section thickness. Charging effects in the vicinity of the SiO2 nanoparticles contained in cell sections could be clarified by placing cell sections on different substrates. Moreover, a method is presented for information depth determination of backscattered electrons which is based on the imaging of subsurface nanoparticles embedded by the cells.
Microscopy, Electron, Scanning/methods , Cell Line, Tumor , Humans , Microtomy/methods , Nanoparticles , Silicon Dioxide
Thin-film-based phase-plates are applied to enhance the contrast of weak-phase objects in transmission electron microscopy. In this work, metal-film-based phase-plates are considered to reduce contamination and electrostatic charging, which up to now limit the application of phase-plates fabricated from amorphous C-films. Their crystalline structure requires a model for the simulation of the effect of crystallinity on the phase-plate properties and the image formation process. The model established in this work is verified by experimental results obtained by the application of a textured nanocrystalline Au-film-based Hilbert phase-plate. Based on the model, it is shown that monocrystalline and textured nanocrystalline phase-plate microstructures of appropriate thickness and crystalline orientation can be a promising approach for phase-contrast transmission electron microscopy.
Microscopy, Electron, Transmission/methods , Microscopy, Phase-Contrast/methods
Transmission electron microscopy phase-contrast images taken by amorphous carbon film-based phase plates are affected by the scattering of electrons within the carbon film causing a modification of the image-wave function. Moreover, image artefacts are produced by non-centrosymmetric phase plate designs such as the Hilbert-phase plate. Various methods are presented to correct phase-contrast images with respect to the scattering of electrons and image artefacts induced by phase plates. The proposed techniques are not restricted to weak-phase objects and linear image formation. Phase-contrast images corrected by the presented methods correspond to those taken by an ideal centrosymmetric, matter-free phase plate and are suitable for object-wave reconstruction.
Electrons , Image Processing, Computer-Assisted/methods , Microscopy, Electron, Transmission/methods , Models, Theoretical , Carbon , Microscopy, Phase-Contrast/methods
High-angle annular dark-field scanning transmission electron microscopy (HAADF STEM) at low energies (≤30 keV) was used to study quantitatively electron scattering in amorphous carbon and carbon-based materials. Experimental HAADF STEM intensities from samples with well-known composition and thickness are compared with results of Monte Carlo simulations and semiempirical equations describing multiple electron scattering. A well-defined relationship is found between the maximum HAADF STEM intensity and sample thickness which is exploited (a) to derive a quantitative description for the mean quadratic scattering angle and (b) to calculate the transmitted HAADF STEM intensity as a function of the relevant materials parameters and electron energy. The formalism can be also applied to determine TEM sample thicknesses by minimizing the contrast of the sample as a function of the electron energy.
High-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) images of electron-transparent samples show dominant atomic number (Z-) contrast with a high lateral resolution. HAADF STEM at low electron energies <30 keV is applied in this work for quantitative composition analyses of InGaAs quantum wells. To determine the local composition, normalized experimental image intensities are compared with results of Monte Carlo simulations. For verification of the technique, InGaAs/GaAs quantum-well structures with known In concentration are used. Transmission electron microscopy samples with known thickness are prepared by the focused-ion-beam technique. The method can be extended to other material systems and is particularly promising for the analysis of materials that are sensitive toward knock-on damage.
A method is described for the reconstruction of the amplitude and phase of the object exit wave function by phase-plate transmission electron microscopy. The proposed method can be considered as in-line holography and requires three images, taken with different phase shifts between undiffracted and diffracted electrons induced by a suitable phase-shifting device. The proposed method is applicable for arbitrary object exit wave functions and non-linear image formation. Verification of the method is performed for examples of a simulated crystalline object wave function and a wave function acquired with off-axis holography. The impact of noise on the reconstruction of the wave function is investigated.
Zinc oxide (ZnO) nanocrystals (NCs) with high crystalline quality were prepared via radio-frequency magnetron sputtering as a SiO(2)/ZnO/SiO(2) trilayer on Si(100) and Al(2)O(3)(0001) substrates with an intermediate in situ annealing step. Transmission electron microscopy reveals a uniform dispersion of ZnO NCs in the amorphous SiO(2) matrix with typical sizes up to 16 nm with a larger fraction of smaller crystals. The size distribution analysis yields a mean grain size of 5 nm for small particles. Individual ZnO NCs show a well-defined hexagonal close packed wurtzite structure and lattice parameters close to those of bulk ZnO, confirming their high crystalline quality. Mapping of the Zn distribution by means of energy-filtered transmission electron microscopy reveals a strongly non-uniform distribution of Zn within the SiO(2) matrix, corroborating the chemical separation of ZnO NCs from surrounding SiO(2). Optical transmittance measurements confirm the findings of the electron microscopy analysis. The fabrication technique described opens up new possibilities in the preparation of ZnO NCs with high crystalline quality, including growth in monolithic optical cavities without intermediate ex situ fabrication steps.
An instability in the growth of nonperiodic InGaAs/GaAs multiple quantum well samples, ordinarily of high-quality when grown with equal periods of order of half the wavelength of light in the material, leads to a dramatic microscopic, self-organized surface grating. This effect was discovered while growing quantum wells with two unequal barrier lengths arranged in a Fibonacci sequence to form an optical quasicrystal. A laser beam incident normal to the surface of the sample is diffracted into a propeller-shaped pattern. The sample surface has a distinctly cloudy appearance when viewed along one crystal axis but is mirror-like when the sample is rotated 90 degrees. The instability results in a five-fold increase in the absorption linewidth of the heavy-hole exciton transition. Atomic force microscopy, transmission electron microscopy, and scanning electron microscopy were used to study the samples.
In this theoretical study we analyze contrast transfer of weak-phase objects in a transmission electron microscope, which is equipped with an aberration corrector (C(s)-corrector) in the imaging lens system and a physical phase plate in the back focal plane of the objective lens. For a phase shift of pi/2 between scattered and unscattered electrons induced by a physical phase plate, the sine-type phase contrast transfer function is converted into a cosine-type function. Optimal imaging conditions could theoretically be achieved if the phase shifts caused by the objective lens defocus and lens aberrations would be equal to zero. In reality this situation is difficult to realize because of residual aberrations and varying, non-zero local defocus values, which in general result from an uneven sample surface topography. We explore the conditions--i.e. range of C(s)-values and defocus--for most favourable contrast transfer as a function of the information limit, which is only limited by the effect of partial coherence of the electron wave in C(s)-corrected transmission electron microscopes. Under high-resolution operation conditions we find that a physical phase plate improves strongly low- and medium-resolution object contrast, while improving tolerance to defocus and C(s)-variations, compared to a microscope without a phase plate.
Imaging of weak amplitude and phase objects, such as unstained vitrified biological samples, by conventional transmission electron microscopy (TEM) suffers from poor object contrast since the amplitude and phase of the scattered electron wave change only very little. In phase contrast light microscopy the imaging of weak phase objects is greatly enhanced by the use of a quarter-wave phase plate, which produces high signal contrast by shifting the phase of the scattered light. An analogous quarter-wave plate for the electron microscope, designed as an electrostatic einzel lens, was proposed by Boersch in 1947 but the small dimensions of the device have impeded its realization up to now. We here present the first fabrication and application of a miniaturized electrostatic einzel lens driven as TEM quarter-wave phase plate. Phase modulation is generated by the electrostatic field confined to the inside of a microstructured ring electrode. This field affects the phase velocity of the unscattered part of the electron wave. By varying its strength the phase shift of the primary beam can be adjusted to pi/2, producing strong phase contrast independent of spatial frequency. The phase plate proves to be mechanically stable and does not impair image quality, in particular it does not reduce the high-resolution signal. The expected residual lens effect of the einzel lens is minimal. Our microlens is supported by conducting rods arranged in a threefold symmetry. This particular geometry provides optimized single-sideband signal transfer for spatial frequencies otherwise obstructed by the supporting rods.
We report on progress in growth and applications of submonolayer (SML) quantum dots (QDs) in high-speed vertical-cavity surface-emitting lasers (VCSELs). SML deposition enables controlled formation of high density QD arrays with good size and shape uniformity. Further increase in excitonic absorption and gain is possible with vertical stacking of SML QDs using ultrathin spacer layers. Vertically correlated, tilted or anticorrelated arrangements of the SML islands are realized and allow QD strain and wavefunction engineering. Respectively, both TE and TM polarizations of the luminescence can be achieved in the edge-emission using the same constituting materials. SML QDs provide ultrahigh modal gain, reduced temperature depletion and gain saturation effects when used in active media in laser diodes. Temperature robustness up to 100 °C for 0.98 µm range vertical-cavity surface-emitting lasers (VCSELs) is realized in the continuous wave regime. An open eye 20 Gb/s operation with bit error rates better than 10-12has been achieved in a temperature range 25-85 °Cwithout current adjustment. Relaxation oscillations up to â¼30 GHz have been realized indicating feasibility of 40 Gb/s signal transmission.
