The helium ion microscope (HIM) has emerged as an instrument of choice for patterning, imaging and, more recently, analytics at the nanoscale. Here, we review secondary electron imaging on the HIM and the various methodologies and hardware components that have been developed to confer analytical capabilities to the HIM. Secondary electron–based imaging can be performed at resolutions down to 0.5 nm with high contrast, with high depth of field, and directly on insulating samples. Analytical methods include secondary electron hyperspectral imaging (SEHI), scanning transmission ion microscopy (STIM), backscattering spectrometry and, in particular, secondary ion mass spectrometry (SIMS). The SIMS system that was specifically designed for the HIM allows the detection of all elements, the differentiation between isotopes, and the detection of trace elements. It provides mass spectra, depth profiles, and 2D or 3D images with lateral resolutions down to 10 nm.

This work reports the strong correlation between the conductivity of fused porphyrins thin films and the porphyrin substituents.

This paper is a review on the combination between Helium Ion Microscopy (HIM) and Secondary Ion Mass Spectrometry (SIMS), which is a recently developed technique that is of particular relevance in the context of the quest for high-resolution high-sensitivity nano-analytical solutions. We start by giving an overview on the HIM-SIMS concept and the underlying fundamental principles of both HIM and SIMS. We then present and discuss instrumental aspects of the HIM and SIMS techniques, highlighting the advantage of the integrated HIM-SIMS instrument. We give an overview on the performance characteristics of the HIM-SIMS technique, which is capable of producing elemental SIMS maps with lateral resolution below 20 nm, approaching the physical resolution limits, while maintaining a sub-nanometric resolution in the secondary electron microscopy mode. In addition, we showcase different strategies and methods allowing to take profit of both capabilities of the HIM-SIMS instrument (high-resolution imaging using secondary electrons and mass filtered secondary sons) in a correlative approach. Since its development HIM-SIMS has been successfully applied to a large variety of scientific and technological topics. Here, we will present and summarise recent applications of nanoscale imaging in materials research, life sciences and geology.

and are important in various technological fields such as energy, electronics, medicine, and many more. [1][2][3][4][5] However, as a consequence of industrial processes and man-made pollution, unwanted nanoparticle size distributions and concentrations [6] give rise to concerns with respect to human health and environmental pollution. While the nanoparticles' physicochemical properties (size, shape, surface chemistry, etc.) determine the quality of products, [7,8] such characteristics are also important in order to evaluate the biological impact of nanoparticles at a molecular, cellular, and systemic level for any risk assessment for environmental and human health. [9] Characterizing nanoparticles in a dynamic context and on a case-by-case basis, microscopic imaging techniques including those that use focused electron or ion beams in scanning electron microscopes (SEMs) or helium ion microscopes [10] (HIMs) to generate nanometer scale spatial resolution are frequently applied in the scientific community. Given the substantial information content of digital images, these techniques often benefit from, or require, automated high-throughput data analysis that enables the accurate identification of large numbers of particles in a robust way.Nanoparticles occur in various environments as a consequence of man-made processes, which raises concerns about their impact on the environment and human health. To allow for proper risk assessment, a precise and statistically relevant analysis of particle characteristics (such as size, shape, and composition) is required that would greatly benefit from automated image analysis procedures. While deep learning shows impressive results in object detection tasks, its applicability is limited by the amount of representative, experimentally collected and manually annotated training data. Here, an elegant, flexible, and versatile method to bypass this costly and tedious data acquisition process is presented. It shows that using a rendering software allows to generate realistic, synthetic training data to train a state-of-the art deep neural network. Using this approach, a segmentation accuracy can be derived that is comparable to man-made annotations for toxicologically relevant metal-oxide nanoparticle ensembles which were chosen as examples. The presented study paves the way toward the use of deep learning for automated, highthroughput particle detection in a variety of imaging techniques such as in microscopies and spectroscopies, for a wide range of applications, including the detection of micro-and nanoplastic particles in water and tissue samples.

Porous and highly conjugated multiply fused porphyrin thin films are prepared from a fast and single-step chemical vapor deposition approach. While the solution-based coupling of porphyrins is usually undertaken at room temperature, the gas phase reaction of nickel(II) 5,15-(diphenyl)porphyrin and iron(III) chloride (FeCl 3 ) is investigated for temperatures as high as 200 °C. Helium ion and atomic force microscopy, supported by weight and thickness measurements, shows a drastic decrease of the fused porphyrin thin film’s density accompanied by the formation of a mesoporous morphology upon increase of the reaction temperature. The increase of the film’s porosity is attributed to formation of a greater amount of HCl (originated from both the oxidative coupling and chlorination reactions) and the release of gaseous FeCl 3 byproducts, i.e., Cl 2 , at higher deposition temperatures. In addition, high resolution mass spectrometry reveals that increase of the reaction temperature promotes a higher degree of conjugation of the fused porphyrins chains, which ensures that high electronic conductivities are maintained along with high porosity. The method reported herein could enable the engineering of fused porphyrin thin films in sensing and catalytic devices.

The structural, morphological, and chemical characterization of samples is of utmost importance for a large number of scientific fields. Furthermore, this characterization very often needs to be performed in three dimensions and at length scales down to the nanometer. Therefore, there is a stringent necessity to develop appropriate instrumentational solutions to fulfill these needs. Here we report on the deployment of magnetic sector secondary ion mass spectrometry (SIMS) on a type of instrument widely used for such nanoscale investigations, namely, focused ion beam (FIB)–scanning electron microscopy (SEM) instruments. First, we present the layout of the FIB-SEM-SIMS instrument and address its performance by using specific test samples. The achieved performance can be summarized as follows: an overall secondary ion beam transmission above 40%, a mass resolving power ( M /Δ M ) of more than 400, a detectable mass range from 1 to 400 amu, a lateral resolution in two-dimensional (2D) chemical imaging mode of 15 nm, and a depth resolution of ∼4 nm at 3.0 keV of beam landing energy. Second, we show results (depth profiling, 2D imaging, three-dimensional imaging) obtained in a wide range of areas, such as battery research, photovoltaics, multilayered samples, and life science applications. We hereby highlight the system’s versatile capability of conducting high-performance correlative studies in the fields of materials science and life sciences.

Over the last few decades, nanoparticles have become a key element in a number of scientific and technological fields, spanning from materials science to life sciences. The characterization of nanoparticles or samples containing nanoparticles, in terms of morphology, chemical composition, and other parameters, typically involves investigations with various analytical tools, requiring complex workflows and extending the duration of such studies to several days or even weeks. Here, we report on the development of a new unique in situ correlative instrument, allowing us to answer questions about the shape, size, size distribution, and chemical composition of the nanoparticles using a single probe. Combining various microscopic and analytical capabilities in one single instrument allows a considerable increase in flexibility and a reduction in the duration of such complex investigations. The new instrument is based on focused ion beam microscopy technology using a gas field ion source as a key enabler and combining it with specifically developed secondary ion mass spectrometry and scanning transmission ion microscopy technology. We will present the underlying concept, the instrument and its main components, and proof-of-concept studies performed on this novel instrument. For this purpose, different pure titanium dioxide nanoparticle samples were investigated. Furthermore, the distribution and localization of the nanoparticles in biological model systems were studied. Our results demonstrate the performance and usefulness of the instrument for nanoparticle investigations, paving the way for a number of future applications, in particular, nanotoxicological research.

A detection system based on a microchannel plate with a delay line readout structure has been developed to perform scanning transmission ion microscopy (STIM) in the helium ion microscope (HIM). This system is an improvement over other existing approaches since it combines the information of the scanning beam position on the sample with the position (scattering angle) and time of the transmission events. Various imaging modes, such as bright field and dark field or the direct image of the transmitted signal, can be created by post-processing the collected STIM data. Furthermore, the detector has high spatial and temporal resolution, is sensitive to both ions and neutral particles over a wide energy range, and shows robustness against ion beam-induced damage. A special in-vacuum movable support gives the possibility of moving the detector vertically, placing the detector closer to the sample for the detection of high-angle scattering events, or moving it down to increase the angular resolution and distance for time-of-flight measurements. With this new system, we show composition-dependent contrast for amorphous materials and the contrast difference between small-angle and high-angle scattering signals. We also detect channeling-related contrast on polycrystalline silicon, thallium chloride nanocrystals, and single-crystalline silicon by comparing the signal transmitted at different directions for the same data set.