Primary Beam Energy Research Articles

EXPERIMENTAL DATA GENERALIZATION OF DELTA ELECTRON YIELD INDUCED BY HIGH ENERGY ELECTRON INTERACTION WITH AMORPHOUS AND SINGLE-CRYSTAL TARGETS

The generalized experimental results of delta electron yield obtained at the NSC KIPT electron accelerators in the energy range from 0.5 MeV to 1.6 GeV are presented. Thin foils of Be, Al, Si, Ni, and Nb were used as experimental targets. It was established in general that delta electron yield is roportional to the product √T∙Z/A, where T is the thickness of the sample in g/cm2 and it has a linear dependence. It is shown that the main factor of delta elec- tron yield increasing is not primary beam energy, but the electron density of the experimental target

Monte‐Carlo Study on Temperature Effect on Scanning Electron Microscopy Contrast for One Spherical Nanoparticle in Multiframe Stacking Mode

Modern scanning electron imaging (SEM) has become an essential tool in various fields. In order to obtain high‐quality images with minimal vibration and drift, the multi‐frame stacking technique is commonly used. However, one aspect that has been overlooked in this process is the electron beam‐induced temperature effect. This study aims to explore the impact of the temperature effect on SEM contrast for a single spherical nanoparticle, specifically a gold nanosphere on a carbon substrate. Through Monte‐Carlo simulation, we investigated how the number of frames in multi‐frame stacking mode affects two types of electron signals: secondary electrons (SE) and backscattering electrons (BSE). Our findings revealed that the SEM contrast is indeed sensitive to the number of frames used in the stacking process. It is observed that the SE contrast decreases while the BSE contrast increases compared to cases without considering temperature effects. It is also found that when using the large primary electron beam energy, the impact of temperature effect was less significant. The electron‐solid interaction theory was utilized to systematically explain the underlying mechanism. This study not only sheds light on how temperature effects can influence SEM imaging but also provides valuable insights for optimizing image acquisition techniques.

Secondary electron emission measurements from imidazolium-based ionic liquids

Abstract The electron-induced secondary electron emission (SEE) yields of imidazolium-based ionic liquids are presented for primary electron beam energies between 30 and 1000 eV. These results are important for understanding plasma synthesis of nanoparticles in plasma discharges with an ionic liquid electrode. Due to their low vapor pressure and high conductivity, ionic liquids can produce metal nanoparticles in low-pressure plasmas through reduction of dissolved metal salts. In this work, the low vapor pressure of ionic liquids is exploited to directly measure SEE yields by bombarding the liquid with electrons and measuring the resulting currents. The ionic liquids studied are [BMIM][Ac], [EMIM][Ac], and [BMIM][BF4]. The SEE yields vary significantly over the energy range, with maximum yields of around 2 at 200 eV for [BMIM][Ac] and [EMIM][Ac], and 1.8 at 250 eV for [BMIM][BF4]. Molecular orbital calculations indicate that the acetate anion is the likely electron donor for [BMIM][Ac] and [EMIM][Ac], while in [BMIM][BF4], the electrons likely originate from the [BMIM]$^+$ cation. The differences in SEE yields are attributed to varying ionization potentials and molecular structures of the ionic liquids. These findings are essential for accurate modeling of plasma discharges and understanding SEE mechanisms in ionic liquids.

Comparison of Monte Carlo Tools for Displacement Calculations for Protons and Heavy Ions Irradiation on Iron and EUROFER97

Abstract Ion irradiation of structural materials for the current and future generation nuclear reactors is a widespread technique used to simulate neutron irradiation in the context of material science research. During the designing phase of irradiation experiments Monte Carlo transport codes are often employed to quantify the radiation exposure, by estimating the displacements per atom (dpa) quantity. From the available displacement calculation codes, four popular choices were selected: cern-fluka, mcnp, phits, and srim. These codes will be used to simulate the irradiation effects of proton and Fe ions on pure iron (G379) and EUROFER97 alloy (a common material in fusion applications) targets. Results coming from the different software are presented in the form of damage profiles and of number of displacements as a function of the primary beam energy. This study identifies discrepancies between the codes' outputs and provides optimized simulation setup parameters.

Signal oscillations in helium scattering by bismuth atoms in the low energy range

Low Energy Ion Scattering (LEIS) analysis of bismuth selenide (Bi2Se3), a strong 3D topological insulator, revealed oscillations of the detected signal in dependence on primary ion beam energy. Bismuth is a part of the group of elements where oscillatory behaviour was already noticed, such as gallium, indium, or lead. Generally, it is ascribed to quasi-resonant charge exchange processes between primary ion and target atom. Moreover, clear differences exist between data for target atoms in elemental form and for atoms in compound form. A study of Bi signal yields in different material forms was performed for primary He+ projectiles within the energy range from 0.50 to 6.00 keV. A foil of pure Bi, Bi2Se3, Bi2O3 and thin Bi films deposited on several substrates (SiO2, CuOx) by Molecular Beam Epitaxy were analysed. The energy shift in the position of oscillations was observed when the oxygen atoms were present at the surface and bonded to Bi atoms. A description of the Bi ion yield variation is provided to facilitate the quantification process in LEIS.

Accelerator and beam physics challenges in support of FRIB experiments

The Facility for Rare Isotope Beams (FRIB), a major nuclear physics facility for research with fast, stopped and reaccelerated rare isotope beams, started operation in May 2022. Since then, a dozen nuclear physics experiments have been successfully accomplished. Typically, the experiments with rare isotope beams last a week or two. Each experiment requires a different primary beam species and energies. Shortening the accelerator and fragment separator setup time is critical to meet the demands of the FRIB Users community. Currently, the primary focus in the linac is reducing the accelerator setup time and beam power ramp-up. Many physics applications have been developed and used to set up the accelerator and beamlines. The simultaneous acceleration of multiple charge states of heavy ion beams is routinely used to minimize the beam power deposition on the charge selector slits after the stripper. This paper discusses the challenges of linac tune development for the acceleration of various ion species.

Bismuth, by high-sensitivity low energy ion scattering

Low energy ion scattering is an analytical technique with extreme surface sensitivity. It enables qualitative and quantitative elemental analysis of the outermost atomic layer. Straightforward quantification is possible by using well-defined reference samples, as the measured signal is related to known surface atomic concentration. Bi, like Pb, exhibits strong oscillatory behavior of backscattered ion yield when primary ion beam energy is varied. Here, we present the spectra of bismuth obtained by scattering of 4He+ ions in a wide range of energies (0.5–6.0 keV). These should cover a regularly used range of energies for He analysis and serve as standards or reference spectra for analysis of bismuth if the scattering angle is 145° or similar. For this purpose, high-purity foil cleaned by ion sputtering was used. The sensitivity of the instrument in use (high-sensitivity low energy ion scattering spectrometer) is defined by the 3 keV 4He+ spectrum of copper. The related atomic sensitivity and relative sensitivity factors are determined.

Assessing the Quality of Oxygen Plasma Focused Ion Beam (O-PFIB) Etching on Polypropylene Surfaces Using Secondary Electron Hyperspectral Imaging.

The development of Focused Ion Beam-Scanning Electron Microscopy (FIB-SEM) systems has provided significant advances in the processing and characterization of polymers. A fundamental understanding of ion-sample interactions is still missing despite FIB-SEM being routinely applied in microstructural analyses of polymers. This study applies Secondary Electron Hyperspectral Imaging to reveal oxygen and xenon plasma FIB interactions on the surface of a polymer (in this instance, polypropylene). Secondary Electron Hyperspectral Imaging (SEHI) is a technique housed within the SEM chamber that exhibits multiscale surface sensitivity with a high spatial resolution and the ability to identify carbon bonding present using low beam energies without requiring an Ultra High Vacuum (UHV). SEHI is made possible through the use of through-the-lens detectors (TLDs) to provide a low-pass SE collection of low primary electron beam energies and currents. SE images acquired over the same region of interest from different energy ranges are plotted to produce an SE spectrum. The data provided in this study provide evidence of SEHI's ability to be a valuable tool in the characterization of polymer surfaces post-PFIB etching, allowing for insights into both tailoring polymer processing FIB parameters and SEHI's ability to be used to monitor serial FIB polymer surfaces in situ.

Determining the oxygen detection limit with magnetic sector dynamic secondary ion mass spectrometry (SIMS)

Dynamic SIMS is often used in evaluating the concentration of impurities in solids because of its high sensitivity and depth profiling capabilities with good depth resolution and high throughput. Continuous ion beam sputtering with a high-density primary beam provides high sensitivity and reduced background contribution from residual gases within the analytical chamber. Numerical simulations along with the data acquired in the real depth profiling experiment show a good agreement of the simple model, assuming that the surface uptake of the oxygen under Cs bombardment depends on the Cs surface retention concentration. In cases where high depth resolution is desired, requiring a low primary ion beam energy, a background subtraction option will help provide better detection limits. It is proposed to perform the background subtraction based on the difference between the continuous and interleaving sputtering modes of dynamic SIMS. The experiments performed on different instruments using different sputtering rate conditions (and different impact energies) show the power function dependence of oxygen detection limit on the reversed sputter rate variation or sputtering beam density. The proposed detection limit dependence curve can be used for analytical specifications benchmarking in most magnetic sector SIMS instruments.

Creation of Single Vacancies in hBN with Electron Irradiation.

Understanding electron irradiation effects is vital not only for reliable transmission electron microscopy characterization, but increasingly also for the controlled manipulation of 2D materials. The displacement cross sectionsof monolayer hexagonal boron nitride (hBN) are measured using aberration-corrected scanning transmission electron microscopy in near ultra-high vacuum at primary beam energies between 50 and 90keV. Damage rates below 80keV are up to three orders of magnitude lower than previously measured at edges under poorer residual vacuum conditions, where chemical etching appears to dominate. Notably, it is possible to create single vacancies in hBN using electron irradiation, with boron almost twice as likely as nitrogen to be ejected below 80keV. Moreover, any damage at such low energies cannot be explained by elastic knock-on, even when accounting for the vibrations of the atoms. A theoretical description is developed to account for the lowering of the displacement threshold due to valence ionization resulting from inelastic scattering of probe electrons, modeled using charge-constrained density functional theory molecular dynamics. Although significant reductions are found depending on the constrained charge, quantitative predictions for realistic ionization states are currently not possible. Nonetheless, there is potential for defect-engineering of hBN at the level of single vacancies using electronirradiation.

Combined electronic excitation and knock-on damage in monolayer MoS2

Electron irradiation-induced damage is often the limiting factor in imaging materials prone to ionization or electronic excitations due to inelastic electron scattering. Quantifying the related processes at the atomic scale has only become possible with the advent of aberration-corrected (scanning) transmission electron microscopes and two-dimensional materials that allow imaging each lattice atom. While it has been shown for graphene that pure knock-on damage arising from elastic scattering is sufficient to describe the observed damage, the situation is more complicated with two-dimensional semiconducting materials such as ${\mathrm{MoS}}_{2}$. Here, we measure the displacement cross section for sulfur atoms in ${\mathrm{MoS}}_{2}$ with primary beam energies between 55 and 90 keV, and correlate the results with existing measurements and theoretical models. Our experimental data suggests that the displacement process can occur from the ground state, or with single or multiple excitations, all caused by the same impinging electron. The results bring light to reports in the recent literature, and add necessary experimental data for a comprehensive description of electron irradiation damage in a two-dimensional semiconducting material. Specifically, the results agree with a combined inelastic and elastic damage mechanism at intermediate energies, in addition to a pure elastic mechanism that dominates above 80 keV. When the inelastic contribution is assumed to arise through impact ionization, the associated excitation lifetime is on the order of picoseconds, on par with expected excitation lifetimes in ${\mathrm{MoS}}_{2}$, whereas it drops to some tens of femtoseconds when direct valence excitation is considered.

In Situ Time-of-Flight Mass Spectrometry of Ionic Fragments Induced by Focused Electron Beam Irradiation: Investigation of Electron Driven Surface Chemistry inside an SEM under High Vacuum.

Recent developments in nanoprinting using focused electron beams have created a need to develop analysis methods for the products of electron-induced fragmentation of different metalorganic compounds. The original approach used here is termed focused-electron-beam-induced mass spectrometry (FEBiMS). FEBiMS enables the investigation of the fragmentation of electron-sensitive materials during irradiation within the typical primary electron beam energy range of a scanning electron microscope (0.5 to 30 keV) and high vacuum range. The method combines a typical scanning electron microscope with an ion-extractor-coupled mass spectrometer setup collecting the charged fragments generated by the focused electron beam when impinging on the substrate material. The FEBiMS of fragments obtained during 10 keV electron irradiation of grains of silver and copper carboxylates and shows that the carboxylate ligand dissociates into many smaller volatile fragments. Furthermore, in situ FEBiMS was performed on carbonyls of ruthenium (solid) and during electron-beam-induced deposition, using tungsten carbonyl (inserted via a gas injection system). Loss of carbonyl ligands was identified as the main channel of dissociation for electron irradiation of these carbonyl compounds. The presented results clearly indicate that FEBiMS analysis can be expanded to organic, inorganic, and metal organic materials used in resist lithography, ice (cryo-)lithography, and focused-electron-beam-induced deposition and becomes, thus, a valuable versatile analysis tool to study both fundamental and process parameters in these nanotechnology fields.

Revealing Localised Mechanochemistry of Biomaterials Using In Situ Multiscale Chemical Analysis.

The study of mechanical and chemical phenomena arising within a material that is being subjected to external stress is termed mechanochemistry (MC). Recent advances in MC have revealed the prospect not only to enable a greener route to chemical transformations but also to offer previously unobtainable opportunities in the production and screening of biomaterials. To date, the field of MC has been constrained by the inability of current characterisation techniques to provide essential localised multiscale chemically mapping information. A potential method to overcome this is secondary electron hyperspectral imaging (SEHI). SEHI is a multiscale material characterisation technique applied within a scanning electron microscope (SEM). Based on the collection of secondary electron (SE) emission spectra at low primary beam energies, SEHI is applicable to the chemical assessment of uncoated polymer surfaces. Here, we demonstrate that SEHI can provide in situ MC information using poly(glycerol sebacate)-methacrylate (PGS-M) as an example biomaterial of interest. This study brings the use of a bespoke in situ SEM holder together with the application of SEHI to provide, for the first time, enhanced biomaterial mechanochemical characterisation.

SECONDARY ELECTRON EMISSION FROM THIN ALUMINIUM FOILS PRODUCED BY HIGH ENERGY ELECTRON BEAMS

The description of the experimental equipment and technique for measuring the secondary emission of elec-trons (SEE) with application of accelerated electrons at the linear accelerator of the IHEPNP NSC KIPT with ener-gies up to 30 MeV and a standard secondary emission monitor [1] are presented. Experimental data of secondary electron emission yields from thin aluminum targets (8 and 50 μm) for primary electron beam energies of 16 and 25 MeV have been experimentally measured. The analysis of the experimental data and their comparison with the theory are carried out. It is shown that the proposed technique for measuring the yields of secondary electron emis-sion is useful and applied for study of low-energy and δ-electrons yields from thin foils, as well as to research the effect of the density effect depending on the energy of the primary electron beam.

Influence of primary beam energy on localized surface plasmon resonances mapping by STEM-EELS

Influence of primary beam energy on localized surface plasmon resonances mapping by STEM-EELS

Effect of the molecular weight on the depth profiling of PMMA thin films using low‐energy Cs+ sputtering

In this work, we investigate the influence of the molecular weight of poly(methyl methacrylate) (PMMA) thin films coated on silicon wafer on the time‐of‐flight secondary ion mass spectrometry (ToF‐SIMS) sputtering mechanisms and kinetics during depth profiling using low‐energy monoatomic caesium ions. The sputtering yield volumes are determined as function of molecular weight, film thickness and beam energy. The results show that the sputtering yield volume decreases with increasing molecular weight Mw down to a threshold value below which it becomes nearly constant, as previously observed with argon cluster ions. The relevance of physical parameters such as the glass transition temperature Tg—determined here from ellipsometry measurements—and the entanglement of the polymer chains to account for this behaviour is discussed. The variation of the sputtering yield was also found to vary logarithmically with the primary beam energy. In addition, preliminary experiments carried out using a low molecular weight PMMA (4 kg/mol) evidenced a nanoconfinement effect similar to that observed with argon cluster sputtering but of lower magnitude.

Resistivity contrast imaging in semiconductor structures using ultra-low energy scanning electron microscopy

The damage-induced voltage alteration (DIVA) contrast mechanism in scanning electron microscope (SEM) has been studied in broad range of the primary electron beam energies, with a special emphasis on the ultra-low energy range. The SEM imaging contrast related to resistivity changes in the In(0.55)Al(0.45)P irradiated with He2+ ions of 600 keV was subjected to an analysis in a range of 10 keV down to 10 eV of primary electron energies. The problem of specimen charging in ultra-low energy range and its effect on the contrast in SEM images has been tackled for the first time. Contrary to expectations based on the classical total emission yield approach, the potentials formed at the highly resistive part of irradiated area led to dramatic increase in the intensity of registered signal for primary electron energies below E1, which can be explained as signal saturation due to potential on the specimen surface acting as repeller for primary electrons. Nevertheless, the experimental data presenting the influence of the beam energy on the potential formation on the surface of an insulating material under electron irradiation have been presented for the first time in ultra-low energy regime.

Tuneable in-situ nanoCT workflow using FIB/SEM

Inspired by the standard computed tomography, a new method of 3D X-ray imaging embedded in FIB-SEM microscope is proposed. The unique combination of TEM-like specimen stage enabling in lens STEM detection (referred to as CompuStage), nanomanipulator (referred to as EasyLift) facilitating in-situ sample transfer from bulk sample to TEM-like stage and pixelated in-situ Timepix X-ray detector in Helios G4 FX FIB-SEM system offers an unprecedented workflow. Motivated by common circular CT scan known from microCT world, the object under study is placed on CompuStage rod which enables two possible rotation (in TEM/SEM terminology called tilt) movements – α-tilt – rotation of the CompuStage rod around its axis, and β-tilt – rotation around axis perpendicular to CompuStage rod. β-tilt rotation enables a circular movement of the sample while α-tilt sets the correct position of sample with respect to target and detector. Thin metal lamella of suitable material welded to EasyLift manipulator needle is used as an X-ray target. The final target-sample geometry – position, distance – can be fine-tuned using position control of CompuStage and EasyLift and in-situ monitored by SEM. Both sample and target can also be easily prepared in-situ. Radiographs are recorded by Timepix detector with inherent noise-free operation and energy filtration. For the 3D reconstruction standard microCT reconstruction algorithm is used with the procedure adjusted for the format and quality of nanoCT images.The experiments were carried out on Helios G4 FX DualBeam using titanium and tungsten targets and various semiconductor samples. The ultimate resolution of the proposed method in orders of tens of nanometers was achieved both by the possibility of close target to sample positioning and of adjustment of primary beam energy down to low energies reducing the interaction volume in the target. Since the lower energy radiation is well suited for life-science, the method was also tested on several bio-samples using silver target. The silver target, thanks to its massive low energy Lα line, allowed to distinguish subtle structures in the resin embedded stained mouse brain and also to observe and reconstruct canaliculi in the mouse bone (earlier reported by Dierolf et al. 2010, Nature 467 436).

Low-energy electron transport in gold: mesoscopic potential calculation and its impact on electron emission yields

In a previous work, we extended and benchmarked the MDM Monte Carlo code with available data for gold metallic media irradiated by electron beams. In this paper, we worked with the aim of improving the cross sections on which our Monte Carlo simulation is based, and which are essential for an accurate description of the transport of electrons in gold. The mesoscopic potential of solid gold has been predicted, and its sensitivity toward electron emission has been evaluated. This potential was derived from the calculation of the electrostatic and atomistic potential by density functional theory and used to calculate inelastic inverse mean free path for electron transport. After integrating these results into our Monte Carlo code, we evaluated the impact of these new cross sections on yields of electron emission from solid gold irradiated by monoenergetic electron beams. We obtained a mesoscopic potential value of − 12.77 eV for our model of bulk metal gold, 27% lower than the one commonly estimated from the Fermi energy. This result impacted on the inverse mean free path for plasmon excitations with a 10% decrease for electrons in the range of 6–30 eV. Regarding electron emission yields, there was no impact of the new mesoscopic potential on the primary electron yields, but for secondary electrons, the emission yields were increased by a factor of up to two depending on the primary beam energy and thickness of the gold foil.

On the fate of high-resolution electron energy loss spectroscopy (HREELS), a versatile probe to detect surface excitations: will the Phoenix rise again?

From its advent, high-resolution electron energy loss spectroscopy (HREELS) has emerged as one of the most versatile tools in surface science. In the last few decades, HREELS was widely used for the fundamental study of (i) chemical reactions at the surfaces of model catalysts (mostly single crystals), (ii) lattice dynamics (phonons), (iii) surface plasmons and (iv) magnons. However, HREELS has experienced a continuous decay of the number of daily users worldwide so far, due to several factors. However, the rise of Dirac materials (graphene, topological insulators, Dirac semimetals) offers new perspectives for HREELS, due to its unique features enabling ultrasensitive detection of (i) chemical modifications at their surfaces, (ii) Kohn anomalies arising from electron-phonon coupling and (iii) novel plasmonic excitations associated to Dirac-cone fermions, as well as their eventual mutual interplay with other plasmon resonances related to topologically trivial electronic states. By selected case-study examples, here we show that HREELS can uniquely probe these phenomena in Dirac materials, thus validating its outstanding relevance and its irreplaceability in contemporary solid-state physics, thus paving the way for a renewed interest. In addition, recent technological upgrades enable the combination of HREELS as an add-on to photoemission apparatuses for parallel readout of energy and momentum of surface excitations. Open issues for theoretical modelling of HREELS related to the dependence on primary electron beam energy and scattering geometry are also critically presented.