Focused Ion Beam Milling Research Articles

Extensive Angular Sampling Enables the Sensitive Localization of Macromolecules in Electron Tomograms.

Cryo-electron tomography provides 3D images of macromolecules in their cellular context. To detect macromolecules in tomograms, template matching (TM) is often used, which uses 3D models that are often reliable for substantial parts of the macromolecules. However, the extent of rotational searches in particle detection has not been investigated due to computational limitations. Here, we provide a GPU implementation of TM as part of the PyTOM software package, which drastically speeds up the orientational search and allows for sampling beyond the Crowther criterion within a feasible timeframe. We quantify the improvements in sensitivity and false-discovery rate for the examples of ribosome identification and detection. Sampling at the Crowther criterion, which was effectively impossible with CPU implementations due to the extensive computation times, allows for automated extraction with high sensitivity. Consequently, we also show that an extensive angular sample renders 3D TM sensitive to the local alignment of tilt series and damage induced by focused ion beam milling. With this new release of PyTOM, we focused on integration with other software packages that support more refined subtomogram-averaging workflows. The automated classification of ribosomes by TM with appropriate angular sampling on locally corrected tomograms has a sufficiently low false-discovery rate, allowing for it to be directly used for high-resolution averaging and adequate sensitivity to reveal polysome organization.

Surface treatments and substrate-coating interface effects on damage accumulation kinetics in hard-coated WC-Co hardmetals under cyclic multi-axial high-temperature loading

Coated hardmetals are commonly used tool materials for metal cutting applications. For these applications, the substrate- and the coating surface qualities are improved by grinding, polishing, or blasting. The focus of the current work was to study the influence of different combinations of substrate-coating surface processing techniques on the induced damage in Al2O3/TiCN hard-coated WC-12 wt% hardmetal substrates and the depth to which the damage reaches into the substrate. The substrate and coating surfaces were prepared by grinding, polishing, dry blasting, wet blasting, or remaining in the deposited state. Investigations were performed using cyclic indentation with a novel ball-in-cone test method in a vacuum at 700 °C, under conditions that imitate the combined shear-compression loads that occur at the cutting edges of metal cutting tools. Additionally, finite element simulations were performed to characterize the stress state arising during ball-in-cone testing. The kinetics of defect formation and accumulation in the hardmetal substrate as a function of the loading situation during the ball-in-cone test will also be discussed. The defects that formed in the substrate during cyclic loading were studied using scanning electron microscopy in cross-sections prepared by focused ion beam milling. A larger increase in defect frequency was observed for rougher coating surfaces and substrate-coating interfaces than for smoother ones. Furthermore, 6 μm thick coatings exhibited a higher defect frequency after cyclic loading than 15 μm thick coatings. Most of the observed defects were in the nm-size range close to the substrate-coating interfaces and tended to have increased in size after cyclic loading. The ball-in-cone test set-up enables the study of the damage mechanisms in coated hardmetal substrates with different treatments prior to and after deposition under tunable milling-like stress and temperature conditions.

The effect of crystal anisotropy on fracture toughness and strength of ZrB2 microcantilevers

AbstractThe influence of crystal anisotropy on the micromechanical properties of ceramic grains plays an important role in the design of the macromechanical performance of bulk polycrystalline samples. To this end, the effect of crystal orientation on fracture toughness and strength was investigated by microcantilever bending experiments combined with finite element method (FEM) simulations in grains of a polycrystalline ZrB2 sample. The sample was prepared by hot pressing and the crystal orientations were determined by electron backscatter diffraction after careful surface preparation. The bending tests were carried out on notched and unnotched microcantilevers cut from specific grains along the prismatic (⊥ to c‐axis), basal (∥ to c‐axis), and intermediate (45° to c‐axis) directions of ZrB2 crystals using focused ion beam milling. The fracture toughness and strength were determined by FEM‐derived analytical solutions. The fracture strength was similar with values of about 11–12 GPa in every direction. Enhanced plasticity was found in the intermediate direction of unnotched beams as compared to the other two brittle orientations. The fracture toughness was found to be 30% higher in the intermediate direction (4.1 MPa m0.5) than those measured for the basal (3.1 MPa m0.5) and prismatic directions (3.3 MPa m0.5). These findings were explained by the orientation dependence of slip system activations which provide a new way in the design of textured polycrystalline ZrB2 ceramics toward enhanced damage tolerance.

Structural characterization of thin-walled microbubble cavities

Whispering gallery mode (WGM) microbubble cavities are a versatile optofluidic sensing platform owing to their hollow core geometry. To increase the light–matter interaction and, thereby, achieve higher sensitivity, thin-walled microbubbles are desirable. However, a lack of knowledge about the precise geometry of hollow microbubbles prevents us from having an accurate theoretical model to describe the WGMs and their response to external stimuli. In this work, we provide a complete characterization of the wall structure of a microbubble and propose a theoretical model for the WGMs in this thin-walled microcavity based on the optical waveguide approach. Structural characterization of the wavelength-scale wall is enabled by focused ion beam milling and scanning electron microscopy imaging. The proposed theoretical model is verified by finite element method simulations. Our approach can readily be extended to other low-dimensional micro-/nanophotonic structures.

Ultralow-energy amorphization of contaminated silicon samples investigated by molecular dynamics.

Ion beam processes related to focused ion beam milling, surface patterning, and secondary ion mass spectrometry require precision and control. Quality and cleanliness of the sample are also crucial factors. Furthermore, several domains of nanotechnology and industry use nanoscaled samples that need to be controlled to an extreme level of precision. To reduce the irradiation-induced damage and to limit the interactions of the ions with the sample, low-energy ion beams are used because of their low implantation depths. Yet, low-energy ion beams come with a variety of challenges. When such low energies are used, the residual gas molecules in the instrument chamber can adsorb on the sample surface and impact the ion beam processes. In this paper we pursue an investigation on the effects of the most common contaminant, water, sputtered by ultralow-energy ion beams, ranging from 50 to 500 eV and covering the full range of incidence angles, using molecular dynamics simulations with the ReaxFF potential. We show that the expected sputtering yield trends are maintained down to the lowest sputtering yields. A region of interest with low damage is obtained for incidence angles around 60° to 75°. We also demonstrate that higher energies induce a larger removal of the water contaminant and, at the same time, induce an increased amorphization, which leads to a trade-off between sample cleanliness and damage.

How to avoid FIB-milling artefacts in micro fracture? A new geometry for interface fracture

Focused ion beam (FIB) based small-scale fracture studies have been well established in recent years despite the ongoing discussion of possible artefacts caused by FIB milling. Stable crack growth geometries—where the FIB-prepared notch stably propagates through the sample—have the potential to ameliorate some of the FIB-based challenges. In this work, we propose a new sample geometry for testing interface toughness at the micron scale which results in intrinsically stable crack growth. This geometry is straightforward to fabricate using established FIB-based methods and testing setups. We prove the stability of crack growth by finite element modelling and by experimentally applying the approach on a hard coating–silicon interface. We observe that even with small imperfections, the FIB-milled notch propagates towards the interface and the natural crack stably grows along the interface.

The origin of microstructural alterations in M50 bearing steel undergoing rolling contact fatigue

M50 bearing steel designed for aerospace applications exhibits unique microstructural alterations at the subsurface during rolling contact fatigue (RCF). In this work, three types of microstructural alterations, light etching region (LER), white etching band (WEB) and white etching area (WEA) are systematically studied. A hardness profile at the subsurface is obtained by microindentation with material softening being detected. It is found that the material softening is associated with the formation of WEBs. The microstructural nature of the three types of microstructural alterations is revealed by detailed characterisation using focused ion beam milling and transmission electron microscopy. It is found that LERs, WEBs and WEAs are a manifestation of the decay of the parent martensite and all consist of dislocation cells or fine grains, indicative of plastic deformation. Through subsurface stress field analysis, LER, WEBs and WEAs are found to be caused by different stress components. The similarities and differences of the microstructural alterations in M50 and in widely studied 100Cr6 are discussed where the stability of carbides is believed to play a key role. The difference in material response in the microstructural alterations in M50 is further analysed and modelled based on Kocks and Mecking theory, with different types of activated dislocation slip systems found to be the root cause for such difference. Based on the material response analysis for WEBs, a material softening model for M50 during RCF is established by considering residual plastic strain accumulation, yielding prediction results in agreement with experimental measurement.

Photoluminescence Enhancement of InSe by Coupling with Circular Bragg Grating

AbstractIndium selenide (InSe) has attracted tremendous research interest due to its excellent optical and electronic properties. The direct bandgap of bulk InSe promises efficient carrier recombination in the near‐infrared (NIR) spectral range, holding great potential for NIR‐based optoelectronic device applications. However, the lowest energy transition in InSe involves out‐of‐plane optical dipoles, with resulting photoluminescence (PL) transmitted mainly along the layer plane. This limits both optical excitation and detection efficiency along the surface normal for practical device operation. To circumvent this issue, here, bulk InSe flake is coupled with circular Bragg grating (CBG) fabricated on silicon substrate by focused ion beam milling. A maximal 60‐fold PL enhancement is achieved, with Purcell effect‐facilitated carrier recombination and improved light out‐coupling via CBG contributing jointly. The same device architecture is further demonstrated to boost the second harmonic generation by a factor of 34. The results provide an effective way to enhance the optical performance of III–VI layered nanomaterials for both linear and nonlinear optoelectronic device applications.

Layered metals as polarized transparent conductors

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr2RuO4 and Tl2Ba2CuO6+δ are optically transparent even at macroscopic thicknesses >2 μm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens.

Quantification of gallium cryo-FIB milling damage in biological lamellae

Cryogenic electron microscopy (cryo-EM) can reveal the molecular details of biological processes in their native, cellular environment at atomic resolution. However, few cells are sufficiently thin to permit imaging with cryo-EM. Thinning of frozen cells to <500nm lamellae by focused-ion-beam (FIB) milling has enabled visualization of cellular structures with cryo-EM. FIB milling represents a significant advance over prior approaches because of its ease of use, scalability, and lack of large-scale sample distortions. However, the amount of damage it causes to a thinned cell section has not yet been determined. We recently described an approach for detecting and identifying single molecules in cryo-EM images of cells using 2D template matching (2DTM). 2DTM is sensitive to small differences between a molecular model (template) and the detected structure (target). Here, we use 2DTM to demonstrate that under the standard conditions used for machining lamellae of biological samples, FIB milling introduces a layer of variable damage that extends to a depth of 60nm from each lamella surface. This layer of damage limits the recovery of information for insitu structural biology. We find that the mechanism of FIB milling damage is distinct from radiation damage during cryo-EM imaging. By accounting for both electron scattering and FIB milling damage, we estimate that FIB milling damage with current protocols will negate the potential improvements from lamella thinning beyond 90nm.

Plasmonic Biosensor on the End-Facet of a Dual-Core Single-Mode Optical Fiber.

Optical biosensors target widespread applications, such as drug discovery, medical diagnostics, food quality control, and environmental monitoring. Here, we propose a novel plasmonic biosensor on the end-facet of a dual-core single-mode optical fiber. The concept uses slanted metal gratings on each core, interconnected by a metal stripe biosensing waveguide to couple the cores via the propagation of surface plasmons along the end facet. The scheme enables operation in transmission (core-to-core), thereby eliminating the need to separate the reflected light from the incident light. Importantly, this simplifies and reduces the cost of the interrogation setup because a broadband polarization-maintaining optical fiber coupler or circulator is not required. The proposed biosensor enables remote sensing because the interrogation optoelectronics can be located remotely. In vivo biosensing and brain studies are also enabled because the end-facet can be inserted into a living body, once properly packaged. It can also be dipped into a vial, precluding the need for microfluidic channels or pumps. Bulk sensitivities of 880 nm/RIU and surface sensitivities of 1 nm/nm are predicted under spectral interrogation using cross-correlation analysis. The configuration is embodied by robust and experimentally realizable designs that can be fabricated, e.g., using metal evaporation and focused ion beam milling.

Mapping of the Electrostatic Potentials in a Fully Processed Led Device with nm-Scale Resolution by In Situ off-Axis Electron Holography.

The optoelectronic properties of a fully processed red emitting AlGaInP micro-diode device is measured using standard I-V and luminescence measurements. A thin specimen is then prepared for in situ transmission electron microscopy analysis by focused ion beam milling, then the changes of electrostatic potential as a function of applied forward bias voltage are mapped by off-axis electron holography. We demonstrate that the quantum wells in the diode sit on a potential gradient until the threshold forward bias voltage for light emission is reached; at which point the quantum wells are aligned at the same potential. From simulations, a similar effect for the band structure can be demonstrated, where the quantum wells are aligned at the same energy level, and contain electrons and holes that are available for radiative recombination at this threshold voltage. We demonstrate that off-axis electron holography can be used to directly measure the potential distribution in optoelectronic devices, and is a powerful tool to help better understand their performance and to improve simulations.

Influence of the aspect ratio of the micro-cantilever on the determined Young’s modulus using the Euler-Bernoulli equation

Micro-cantilever bending experiments can be used to determine fundamental material properties, such as fracture stress and fracture toughness. Furthermore, the Young’s modulus can be calculated from the slope of the load-displacement curve using the classical Euler-Bernoulli equation. However, in literature it can be frequently found that applying this technique, the Young’s modulus is significantly underestimated, especially when using micro-cantilevers with aspect ratios (bending length/width) < 6. In order to investigate the influence of the aspect ratio on the determination of the Young’s modulus, SiO2 and single crystalline α-Al2O3 micro-cantilevers with aspect ratios ranging from ∼ 3.5–6.5 were fabricated using focused ion beam milling and tested with a nanoindenter system. In addition to the quasi-static tests, dynamic micro-cantilever bending tests were performed by using an excitation frequency on top of a quasi-static loading and the results of both techniques were compared to each other. Finally, finite element analysis was used to simulate the static-micro-cantilever bending experiments and investigate the influence of shear deformation, flexing of the support and the geometry of the micro-cantilever on the load-displacement curves.

Electrochemical-Shock Synthesis of Nanoparticles from Sub-femtoliter Nanodroplets

ConspectusNanoparticles have witnessed immense development in the past several decades due to their intriguing physicochemical properties. The modern chemist is interested not only in methods of synthesizing nanoparticles with tunable properties but also in the chemistry that nanoparticles can drive. While several methods exist to synthesize nanoparticles, it is often advantageous to put nanoparticles on a variety of conductive substrates for multiple applications (such as energy storage and conversion). Despite enjoying over 200 years of development, electrodeposition of nanoparticles suffers from a lack of control over nanoparticle size and morphology. There have been heroic efforts to address these issues over time. With an understanding that structure-function studies are imperative to understand the chemistry of nanoparticles, new methods are necessary to electrodeposit a variety of nanoparticles with control over macromorphology and also microstructure.This Account details our group's efforts in overcoming challenges of classical nanoparticle electrodeposition by electrodepositing nanoparticles from water nanodroplets. When a nanodroplet full of metal salt precursor is incident on the electrode biased sufficiently negative to drive electroplating, nanoparticles form at a fast rate (on the order of microseconds to milliseconds). We start with the general nuts-and-bolts of the experiment (nanodroplet formation and methods for electrodeposition). The deposition of new nanomaterials often requires one to develop new methods of measurement, and we detail new measurement tools for quantifying nanoparticle porosity and nanopore tortuosity within single nanoparticles. We achieve nanopore characterization by using Focused Ion Beam milling and Scanning Electron Microscopy. Owing to the small size of the nanodroplets and fast mass transfer (the contents of a femtoliter droplet can be electrolyzed in only a few milliseconds), the use of nanodroplets also allows the electrodeposition of high entropy alloy nanoparticles at room temperature.We detail how a deep understanding of ion transfer mechanisms can be used to expand the library of possible metals that can be deposited. Furthermore, simple ion changes in the dispersed droplet phase can decrease the cost per experiment by orders of magnitude. Finally, electrodeposition in aqueous nanodroplets can also be combined with stochastic electrochemistry for a variety of interesting studies. We detail the quantification of the growth kinetics of single nanoparticles in single aqueous nanodroplets. Nanodroplets can also be used as tiny reactors to trap only a few molecules of a metal salt precursor. Upon reduction to the zerovalent metal, electrocatalysis at very small metal clusters can be probed and evaluated with time using steady-state electrochemical measurements. Overall, this burgeoning synthetic tool is providing unexpected avenues of tunability of metal nanoparticles on conductive substrates.

Multi-scale dissection of wing transparency in the clearwing butterfly Phanus vitreus.

Optical transparency is rare in terrestrial organisms, and often originates through loss of pigmentation and reduction in scattering. The coloured wings of some butterflies and moths have repeatedly evolved transparency, offering examples of how they function optically and biologically. Because pigments are primarily localized in the scales that cover a colourless wing membrane, transparency has often evolved through the complete loss of scales or radical modification of their shape. Whereas bristle-like scales have been well documented in glasswing butterflies, other scale modifications resulting in transparency remain understudied. The butterfly Phanus vitreus achieves transparency while retaining its scales and exhibiting blue/cyan transparent zones. Here, we investigate the mechanism of wing transparency in P. vitreus by light microscopy, focused ion beam milling, microspectrophotometry and optical modelling. We show that transparency is achieved via loss of pigments and vertical orientation in normal paddle-like scales. These alterations are combined with an anti-reflective nipple array on portions of the wing membrane being more exposed to light. The blueish coloration of the P. vitreus transparent regions is due to the properties of the wing membrane, and local scale nanostructures. We show that scale retention in the transparent patches might be explained by these perpendicular scales having hydrophobic properties.

Sidewall Electrical Damage in β-Ga2O3 Rectifiers Exposed to Ga+ Focused Ion Beams

The energy and beam current dependence of Ga+ focused ion beam milling damage on the sidewall of vertical rectifiers fabricated on n-type Ga2O3 was investigated with 5–30 kV ions and beam currents from 1.3–20 nA. The sidewall damage was introduced by etching a mesa along one edge of existing Ga2O3 rectifiers. We employed on-state resistance, forward and reverse leakage current, Schottky barrier height, and diode ideality factor from the vertical rectifiers as potential measures of the extent of the ion-induced sidewall damage. Rectifiers of different diameters were exposed to the ion beams and the “zero-area” parameters extracted by extrapolating to zero area and normalizing for milling depth. Forward currents degraded with exposure to any of our beam conductions, while reverse current was unaffected. On-state resistance was found to be most sensitive of the device parameters to Ga+ beam energy and current. Beam current was the most important parameter in creating sidewall damage. Use of subsequent lower beam energies and currents after an initial 30 kV mill sequence was able to reduce residual damage effects but not to the point of initial lower beam current exposures.

Scalable fabrication of hemispherical solid immersion lenses in silicon carbide through grayscale hard-mask lithography

Grayscale lithography allows the creation of micrometer-scale features with spatially controlled height in a process that is fully compatible with standard lithography. Here, solid immersion lenses are demonstrated in silicon carbide using a fabrication protocol combining grayscale lithography and hard-mask techniques to allow nearly hemispherical lenses of 5μm radius to be etched into the substrate. Lens performance was benchmarked by studying the enhancement obtained in the optical collection efficiency for single quantum emitters hosted in silicon carbide. Enhancement by a factor of 4.4 ± 1.0 was measured for emitters not registered to the center of the lens, consistent with devices fabricated through other methods. The grayscale hard-mask technique is highly reproducible, scalable, and compatible with CMOS technology, and device aspect ratios can be tuned after resist patterning by controlling the chemistry of the subsequent dry etch. These results provide a reproducible, low-cost, high-throughput and industrially relevant alternative to focused ion beam milling for the creation of high-aspect-ratio, rounded microstructures for quantum technology, and microphotonic applications.

Low-Cost Plasmonic Platform for Photon-Emission Engineering of Two-Dimensional Semiconductors

Although the field of two-dimensional (2D) materials has democratized materials science by making high-quality samples accessible cheaply, due to the atomically thin nature of these systems, an integration with nanostructures is almost always required to obtain a significant optical response. Traditionally, these nanostructures are fabricated via electron beam lithography or focused ion beam milling, which are expensive, and large-area fabrication can be further time-consuming. In order to overcome this problem, we report the integration of 2D semiconductors on a cost-effective and large-area fabricated nanocone platform. We show that the plasmon modes of our nanocone structures lead to photoluminescence enhancement of monolayer ${\text{WSe}}_{2}$ by about eight to ten times compared with the nonplasmonic case, consistent with finite-difference time-domain simulations. Excitation power-dependent measurements reveal that our nanocone platform enables a versatile route to engineering the relative exciton trion contributions to the emission.

Spectroelectrochemical behavior of parallel arrays of single vertically oriented Pseudomonas aeruginosa cells

Pseudomonas aeruginosa is a Gram-negative opportunistic human pathogen responsible for a number of healthcare-associated infection. It is currently difficult to assess single cell behaviors of P. aeruginosa that might contribute to acquisition of antibiotic resistance, intercellular communication, biofilm development, or virulence, because mechanistic behavior is inferred from ensemble collections of cells, thus averaging effects over a population. Here, we develop and characterize a device that can capture and trap arrays of single P. aeruginosa cells in individual micropores in order to study their behaviors using spectroelectrochemistry. Focused ion beam milling is used to fabricate an array of micropores in a Au/dielectric/Au/SiO2-containing multilayer substrate, in which individual micropores are formed with dimensions that facilitate the capture of single P. aeruginosa cells in a predominantly vertical orientation. The bottom Au ring is then used as a working electrode to explore the spectroelectrochemical behavior of parallel arrays of individual P. aeruginosa cells. Application of step-potential or swept-potential waveforms produces changes in the fluorescence emission that can be imaged and correlated with applied potential. Arrays of P. aeruginosa cells typically exhibit three characteristic fluorescence behaviors that are sensitive to nutritional stress and applied potential. The device developed here enables the study of parallel collections of single bacterial cells with well-defined orientational order and should facilitate efforts to elucidate methods of bacterial communication and multidrug resistance at the single cell level.

Understanding the impact of heavy ions and tailoring the optical properties of large-area monolayer WS2 using focused ion beam

Focused ion beam (FIB) is an effective tool for precise nanoscale fabrication. It has recently been employed to tailor defect engineering in functional nanomaterials such as two-dimensional transition metal dichalcogenides (TMDCs), providing desirable properties in TMDC-based optoelectronic devices. However, the damage caused by the FIB irradiation and milling process to these delicate, atomically thin materials, especially in extended areas beyond the FIB target, has not yet been fully characterised. Understanding the correlation between lateral ion beam effects and optical properties of 2D TMDCs is crucial in designing and fabricating high-performance optoelectronic devices. In this work, we investigate lateral damage in large-area monolayer WS2 caused by the gallium focused ion beam milling process. Three distinct zones away from the milling location are identified and characterised via steady-state photoluminescence (PL) and Raman spectroscopy. The emission in these three zones have different wavelengths and decay lifetimes. An unexpected bright ring-shaped emission around the milled location has also been revealed by time-resolved PL spectroscopy with high spatial resolution. Our findings open up new avenues for tailoring the optical properties of TMDCs by charge and defect engineering via focused ion beam lithography. Furthermore, our study provides evidence that while some localised damage is inevitable, distant destruction can be eliminated by reducing the ion beam current. It paves the way for the use of FIB to create nanostructures in 2D TMDCs, as well as the design and realisation of optoelectrical devices on a wafer scale.