Spherical Aberration Correction Research Articles

Atomic scale imaging of magnetic circular dichroism by achromatic electron microscopy.

In order to obtain a fundamental understanding of the interplay between charge, spin, orbital and lattice degrees of freedom in magnetic materials and to predict and control their physical properties1-3, experimental techniques are required that are capable of accessing local magnetic information with atomic-scale spatial resolution. Here, we show that a combination of electron energy-loss magnetic chiral dichroism 4 and chromatic-aberration-corrected transmission electron microscopy, which reduces the focal spread of inelastically scattered electrons by orders of magnitude when compared with the use of spherical aberration correction alone, can achieve atomic-scale imaging of magnetic circular dichroism and provide element-selective orbital and spin magnetic moments atomic plane by atomic plane. This unique capability, which we demonstrate for Sr2FeMoO6, opens the door to local atomic-level studies of spin configurations in a multitude of materials that exhibit different types of magnetic coupling, thereby contributing to a detailed understanding of the physical origins of magnetic properties of materials at the highest spatial resolution.

Aberration correction for low voltage optimized transmission electron microscopy

Further development of low voltage electron microscopy leads to an aberration correction of the device in order to improve its spatial resolution. The integration of a corrector to a desktop transmission electron microscope with exclusively low-voltage design seems to be a challenging task. The benefits and potential of the Rose hexapole corrector implemented to such a system are critically considered in this paper. The feasibility of miniaturized corrector suitable for desktop LVEM is especially discussed, including the aspect of corrector contribution to chromatic aberration that appears to be crucial. Optimal corrector parameters and resolution limits of such a system are proposed.•Improved spatial resolution•Spherical aberration correction•Permanent magnet transfer lenses

Two-dimensional Gaussian fitting for precise measurement of lattice constant deviation from a selected-area diffraction map.

Unlike X-ray diffraction or Raman techniques, which suffer from low spatial resolution, transmission electron microscopy can be used to obtain strain maps of nanoscaled materials and devices. Convergent-beam electron diffraction (CBED) and nanobeam electron diffraction (NBED) techniques detect the deviation of a lattice constant (i.e. an indicator of strain) within 0.01%; however, their use is restricted to beam-insensitive samples. Selected-area electron diffraction (SAED) does not have such limitations but has low spatial resolution and precision. The use of a spherical aberration corrector and a nanosized selected-area aperture improves the spatial resolution, but the precision is still low. In this study, a two-dimensional stage-scanning system is used to acquire arrays of diffraction patterns at different positions of the sample under fixed beam conditions. Data processing with iterative nonlinear least-squares fitting enabled the spot displacement for each point of the scan area to be measured with precision comparable to that of the CBED or NBED technique. The precise strain determination, in combination with the simplicity of the measurement process, makes the nanosized SAED technique competitive with other methods for strain mapping at nanoscale dimensions.

Single-Site AuI Catalyst for Silane Oxidation with Water.

Single-site Au anchored on mpg-C3 N4 (519 ppm Au loading) is developed as a highly active, selective, and stable catalyst for the oxidation of silanes with water with a turnover frequency as high as 50 200 h-1 , far exceeding most known catalysts based on total gold content. Other hydrosilanes bearing unsaturated functional groups also lead to corresponding silanols under mild reaction conditions without formation of any side products in good or excellent yields. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Au atoms stabilized by mpg-C3 N4 . The coordination of the catalytically active AuI by three nitrogen or carbon atoms in the tri-s-triazine repeating units not only prevents the Au atoms from aggregation, but also renders the surface AuI highly active, which is completely different than homogeneous AuI species.

Study of the specific features of single-crystal boron microstructure

A complex study of the structure of β-boron single crystal grown by the floating-zone method, with sizes significantly exceeding the analogs known in the literature, has been performed. The study includes X-ray diffraction analysis and X-ray diffractometry (measurement of pole figures and rocking curves), performed on both laboratory and synchrotron sources; atomic-resolution scanning transmission electron microscopy with spherical aberration correction; and energy-dispersive microanalysis. X-ray diffraction analysis using synchrotron radiation has been used to refine the β-boron structure and find impurity Si atoms. The relative variations in the unit-cell parameters a and c for the crystal bulk are found to be δa/a ≈ 0.4 and δc/c ≈ 0.1%. X-ray diffractometry has revealed that the single-crystal growth axis coincides with the [\(2\bar 2013\)] crystallographic axis and makes an angle of 21.12° with the [0001] threefold axis. Electron microscopy data have confirmed that the sample under study is a β-boron crystal, which may contain 0.3–0.4 at % Si as an impurity. Planar defects (stacking faults and dislocations) are found. The results of additional measurements of the temperature dependence of the thermal conductivity of the crystal in the range of 50–300 K are indicative of its high structural quality.

Optimization of monochromated TEM for ultimate resolution imaging and ultrahigh resolution electron energy loss spectroscopy

The performance of a monochromated transmission electron microscope with Wien type monochromator is optimized to achieve an extremely narrow energy spread of electron beam and an ultrahigh energy resolution with spectroscopy. The energy spread in the beam is improved by almost an order of magnitude as compared to specified values. The optimization involves both the monochromator and the electron energy loss detection system. We demonstrate boosted capability of optimized systems with respect to ultra-low loss EELS and sub-angstrom resolution imaging (in a combination with spherical aberration correction).

Towards a holographic approach to spherical aberration correction in scanning transmission electron microscopy.

Recent progress in phase modulation using nanofabricated electron holograms has demonstrated how the phase of an electron beam can be controlled. In this paper, we apply this concept to the correction of spherical aberration in a scanning transmission electron microscope and demonstrate an improvement in spatial resolution. Such a holographic approach to spherical aberration correction is advantageous for its simplicity and cost-effectiveness.

Adaptive optical versus spherical aberration corrections for in vivo brain imaging.

Adjusting the objective correction collar is a widely used approach to correct spherical aberrations (SA) in optical microscopy. In this work, we characterized and compared its performance with adaptive optics in the context of in vivo brain imaging with two-photon fluorescence microscopy. We found that the presence of sample tilt had a deleterious effect on the performance of SA-only correction. At large tilt angles, adjusting the correction collar even worsened image quality. In contrast, adaptive optical correction always recovered optimal imaging performance regardless of sample tilt. The extent of improvement with adaptive optics was dependent on object size, with smaller objects having larger relative gains in signal intensity and image sharpness. These observations translate into a superior performance of adaptive optics for structural and functional brain imaging applications in vivo, as we confirmed experimentally.

Three-dimensional visualization of dislocations in a ferromagnetic material by magnetic-field-free electron tomography

In conventional transmission electron microscopy, specimens to be observed are placed in between the objective lens pole piece and therefore exposed to a strong magnetic field about 2 T. For a ferromagnetic specimen, magnetization of the specimen causes isotropic and anisotropic defocusing, deflection of the electron beam as well as deformation of the specimen, which all become more severe when the specimen tilted. Therefore electron tomography on a ferromagnetic crystalline specimen is highly challenging because tilt-series data sets must be acquired without changing the excitation condition of a specific diffraction spot. In this study, a scanning transmission electron microscopy (STEM) tomography method without magnetizing a ferromagnetic specimen has been developed for three-dimensional (3D) visualization of dislocations in α-Fe, which is a typical ferromagnetic material. Magnetic-field-free environment down to 0.38 ± 0.07 mT at the specimen position is realized by demagnetizing the objective lens pole piece of a commercial STEM instrument. By using a spherical aberration corrector with the magnetic-field-free environment, an “aberration corrected Low-Mag STEM mode” with no objective lens field reaches a convergence semi angle ∼1 mrad and a spatial resolution ∼5 nm, and shows an adequate performance of imaging dislocations under a two-beam excitation condition for a low-index diffracted beam. The illumination condition for the aberration corrected Low-Mag STEM mode gives no overlap between the direct beam disk (spot) and neighboring diffraction disks. An electron channeling contrast imaging technique, in which an annular detector was located at a doughnut area between the direct beam and the neighboring diffracted beams, was effectively employed with the aberration corrected Low-Mag STEM mode to keep image intensity high enough even at large specimen-tilt angles. The resultant tomographic observation visualized 3D dislocation arrangements and active slip planes in a deformed α-Fe specimen.

Uncoordinated Amine Groups of Metal-Organic Frameworks to Anchor Single Ru Sites as Chemoselective Catalysts toward the Hydrogenation of Quinoline.

Here we report a precise control of isolated single ruthenium site supported on nitrogen-doped porous carbon (Ru SAs/N-C) through a coordination-assisted strategy. This synthesis is based on the utilization of strong coordination between Ru3+ and the free amine groups (-NH2) at the skeleton of a metal-organic framework, which plays a critical role to access the atomically isolated dispersion of Ru sites. Without the assistance of the amino groups, the Ru precursor is prone to aggregation during the pyrolysis process, resulting in the formation of Ru clusters. The atomic dispersion of Ru on N-doped carbon can be verified by the spherical aberration correction electron microscopy and X-ray absorption fine structure measurements. Most importantly, this single Ru sites with single-mind N coordination can serve as a semihomogeneous catalyst to catalyze effectively chemoselective hydrogenation of functionalized quinolones.

Atomic and nanoscale imaging of a cellulose nanofiber and Pd nanoparticles composite using lower-voltage high-resolution TEM.

We have examined the advanced application of transmission electron microscopy (TEM) for the structural characterization of a composite of cellulose nanofiber (CNF) and palladium (Pd) nanoparticles. In the present study, we focused on electron-irradiation damage and optimization of high-resolution TEM imaging of the composite. The investigation indicates that the CNF breaks even under low-electron-dose conditions at an acceleration voltage of 200 kV. We then applied lower-voltage TEM at 60 kV using a spherical aberration corrector and a monochromator, in order to reduce electron-irradiation damage and improve the spatial resolution. The TEM observation achieved high-resolution imaging and revealed the existence of small Pd nanoparticles, around 2 nm in diameter, supported on the CNF. It is considered that the use of a monochromator in combination with spherical aberration correction contributed to the atomic and nanoscale imaging of the composite, owing to the improvement of the information limit under a lower-acceleration voltage.

The objective lens of the electron microscope with correction of spherical and axial chromatic aberrations.

The paper describes the principle of operation of a relatively simple aberration corrector for the transmission electron microscope objective lens. The electron-optical system of the aberration corrector consists of the two main elements: an electrostatic mirror with rotational symmetry and a magnetic deflector formed by the round-shaped magnetic poles. The corrector operation is demonstrated by calculations on the example of correction of basic aberrations of the well-known objective lens with a bell-shaped distribution of the axial magnetic field. Two of the simplest versions of the corrector are considered: a corrector with a two-electrode electrostatic mirror and a corrector with a three-electrode electrostatic mirror. It is shown that using the two-electrode mirror one can eliminate either spherical or chromatic aberration of the objective lens, without changing the value of its linear magnification. Using a three-electrode mirror, it is possible to eliminate spherical and chromatic aberrations of the objective lens simultaneously, which is especially important in designing electron microscopes with extremely high resolution.

Correction of spherical aberration in multi-focal multiphoton microscopy with spatial light modulator.

We demonstrate that high-quality images of the deep regions of a thick sample can be obtained from its surface by multi-focal multiphoton microscopy (MMM). The MMM system incorporates a spatial light modulator to separate the excitation beam into a multi-focal excitation beam and modulate the pre-distortion wavefront to correct spherical aberration (SA) caused by a refractive index mismatch between the immersion medium and the biological sample. When fluorescent beads in transparent epoxy resin were observed using four SA-corrected focal beams, the fluorescence signal of the obtained images was ~52 times higher than that obtained without SA correction until a depth of ~1100 μm, similar to the result for single-focal multiphoton microscopy (SMM). The MMM scanning time was four times less than that for SMM, and MMM showed an improved fluorescence intensity and depth resolution for an image of blood vessels in the brain of a mouse stained with a fluorescent dye.

A short story of imaging and spectroscopy of two-dimensional materials by scanning transmission electron microscopy

Here we present a short historical account of when single adatom impurities where first identified in two-dimensional materials by scanning transmission electron microscopy (STEM). We also present a study of the graphene low-loss (below 50eV) response as a function of number of layers using electron energy-loss spectroscopy (EELS). The study shows that as few as three layers of graphene behave as bulk graphite for losses above 10eV We also show examples of how point and extended defects can easily be resolved and structural dynamics can be readily capture by using aberration-corrected STEM imaging. Finally, we show that the new generation of monochromators has opened up possibilities to explore new physics with an electron microscope. All these capabilities were enabled by the development of spherical aberration correctors and monochromators, where Ondrej Krivanek has played a key role.

Atomic resolution imaging of YAlO3: Ce in the chromatic and spherical aberration corrected PICO electron microscope

The application of combined chromatic and spherical aberration correction in high-resolution transmission electron microscopy enables a significant improvement of the spatial resolution down to 50 pm. We demonstrate that such a resolution can be achieved in practice at 200kV. Diffractograms of images of gold nanoparticles on amorphous carbon demonstrate corresponding information transfer. The Y atom pairs in [010] oriented yttrium orthoaluminate are successfully imaged together with the Al and the O atoms. Although the 57 pm pair separation is well demonstrated separations between 55 pm and 80 pm are measured. This observation is tentatively attributed to structural relaxations and surface reconstruction in the very thin samples used. Quantification of the resolution limiting effective image spread is achieved based on an absolute match between experimental and simulated image intensity distributions.

Fast data preprocessing with Graphics Processing Units for inverse problem solving in light-scattering measurements

Utilising Compute Unified Device Architecture (CUDA) platform for Graphics Processing Units (GPUs) enables significant reduction of computation time at a moderate cost, by means of parallel computing. In the paper [Jakubczyk et al., Opto-Electron. Rev., 2016] we reported using GPU for Mie scattering inverse problem solving (up to 800-fold speed-up). Here we report the development of two subroutines utilising GPU at data preprocessing stages for the inversion procedure: (i) A subroutine, based on ray tracing, for finding spherical aberration correction function. (ii) A subroutine performing the conversion of an image to a 1D distribution of light intensity versus azimuth angle (i.e. scattering diagram), fed from a movie-reading CPU subroutine running in parallel. All subroutines are incorporated in PikeReader application, which we make available on GitHub repository. PikeReader returns a sequence of intensity distributions versus a common azimuth angle vector, corresponding to the recorded movie. We obtained an overall ∼400-fold speed-up of calculations at data preprocessing stages using CUDA codes running on GPU in comparison to single thread Matlab-only code running on CPU.

Tecnis Symfony Intraocular Lens with a “Sweet Spot” for Tolerance to Postoperative Residual Refractive Errors

Purpose: To investigate the impact of residual astigmatism on visual acuity (VA) after the implantation of a novel extended range of vision (ERV) intraocular lens (IOL) based on the correction of spherical and chromatic aberration. Method: The study enrolled 411 patients bilaterally implanted with the ERV IOL Tecnis Symfony. Visual acuity and subjective refraction were analyzed during the 4- to 6-month follow-up. The sample of eyes was stratified for four groups according to the magnitude of postoperative refractive astigmatism and postoperative spherical equivalent. Results: The astigmatism analysis included 386 eyes of 193 patients with both eyes of each patient within the same cylinder range. Uncorrected VAs for distance, intermediate and near were better in the group of eyes with lower level of postoperative astigmatism, but even in eyes with residual cylinders up to 0.75 D, the loss of VA lines was clinically not relevant. The orientation of astigmatism did not seem to have an impact on the tolerance to the residual cylinder. The SE evaluation included 810 eyes of 405 patients, with both eyes of each patient in the same SE range. Uncorrected VAs for distance, intermediate and near, were very similar in all SE groups. Conclusion: Residual cylinders up to 0.75 D after the implantation of the Tecnis Symfony IOL have a very mild impact on monocular and binocular VA. The Tecnis Symfony IOL shows a good tolerance to unexpected refractive surprises and thus a better “sweet spot”.

Doublet liquid variable-focus lens for spherical aberration correction

A novel doublet liquid variable-focus lens with simple structure was designed and fabricated for spherical aberration correction under the condition of small focal length, which was 11.8mm to 25mm. By changing the shape of the two PDMS membranes respectively, the focal length of the proposed lens was changed and the spherical aberration was corrected. The size of the entire lens was very small and overall structure of the proposed lens was presented, as well as the design process. The ZEMAX software was used to optimize the optical parameters of the proposed lens. The deformation of the PDMS membranes was measured and fitted by spherical curve. The longitudinal spherical aberration was measured in experiments and compared with the optimal design results. In order to weaken the gravity effect, we designed the shape of the rear PDMS membrane and presented the detailed description of the fabrication process.

Transmissive liquid-crystal device for correcting primary coma aberration and astigmatism in biospecimen in two-photon excitation laser scanning microscopy.

All aberrations produced inside a biospecimen can degrade the quality of a three-dimensional image in two-photon excitation laser scanning microscopy. Previously, we developed a transmissive liquid-crystal device to correct spherical aberrations that improved the image quality of a fixed-mouse-brain slice treated with an optical clearing reagent. In this study, we developed a transmissive device that corrects primary coma aberration and astigmatism. The motivation for this study is that asymmetric aberration can be induced by the shape of a biospecimen and/or by a complicated refractive-index distribution in a sample; this can considerably degrade optical performance even near the sample surface. The device’s performance was evaluated by observing fluorescence beads. The device was inserted between the objective lens and microscope revolver and succeeded in improving the spatial resolution and fluorescence signal of a bead image that was originally degraded by asymmetric aberration. Finally, we implemented the device for observing a fixed whole mouse brain with a sloping surface shape and complicated internal refractive-index distribution. The correction with the device improved the spatial resolution and increased the fluorescence signal by ?2.4×. The device can provide a simple approach to acquiring higher-quality images of biospecimens.

Two-photon polymerization setup enables experimental mapping and correction of spherical aberrations for improved macroscopic structure fabrication.

The two-photon photopolymerization of resins by focused laser light in principle enables the fabrication of structures with details below the diffraction limit. However, the method can be highly susceptible to aberrations, which hinders the fabrication of structures that are larger than, e.g., the working distance of the microscope objective. Here, two-photon polymerization is extended to the fabrication of macroscopic structures by making use of medium numerical-aperture microscope objectives. By introducing a substrate holder movable in the axial direction it is possible to keep the focusing conditions constant and to fabricate very large structures with heights that are not limited by the working distance of the objective. Moreover, the constant focusing conditions enable us to quantify spherical aberrations by experimental mapping of the optical point-spread function, which manifests itself in the shape of singe photo-polymerized voxels. By monitoring such shapes it is possible to minimize aberrations. Effective aberration control enables us to fabricate large but detailed biomedical scaffolds with interconnected pores, e.g., in the shape of a human stirrup bone.