arXiv subjects

Jacobus M. Sturm

Publications and source records attributed to Jacobus M. Sturm.

7 recordsLinked to original sources

arXiv2025

Unveiling the effect of adding B4C at the W-on-Si interface

In this study, we investigate the W-on-Si interface and the effect of adding a B4C interlayer at such interface, using low-energy ion scattering (LEIS) spectroscopy, X-ray reflectivity, X-ray diffraction, and transmission electron microscopy with energy dispersive X-ray spectroscopy. We extract the effective width of the interface in three different structures having: no-B4C, 0.24 nm, and 1.2 nm of B4C deposited in between the W and the Si films. The analysis reveals that the W distribution does not get significantly sharper when B4C atoms are deposited at the W-on-Si interface, showing that B4C does not act as a physical barrier against the diffusion of atoms during the deposition of these structures. W/Si thin-film structures are used in various applications, including X-ray optics. While many studies reported that adding a sub-nm thick B4C film at the W/Si interfaces is beneficial for the overall reflectivity of the structures, the physical mechanisms involved were not yet fully understood. In this context, being able to characterize the width of the interfaces with sub-nm resolution is key. In this study, we show how the analysis of the sub-surface signal of the LEIS spectra enables the characterization of the interface W-on-(B4C-)Si, highlighting the importance of systematically extracting the values of the effective interface width for the analysis and understanding of thin-film growth.

cond-mat.mtrl-sci↗

arXiv2024

Engineering Work Function to Stabilize Metal Oxides in Reactive Hydrogen

Hydrogen, crucial for the green energy transition, poses a challenge due to its tendency to degrade surrounding wall materials. To harness hydrogen's potential, it is essential to identify materials' parameter(s) that modulate hydrogen-material interaction. In a recent publication, we have shown that the reduction (de-nitridation) of transition metal (TM)-nitrides in hydrogen radicals (H*) stops when their work function drops below a threshold limit. In this work, we tailor the work function of a complex TM-oxide by tuning the relative content of its constituent TM-atoms. We show that increasing the fraction of a low work function TM decreases the work function of the complex oxide, thereby decreasing its reducibility (de-oxidation) in H*. This leads to the stabilization of the higher oxidation states of a high work function TM, which otherwise readily reduce in H*. We propose that the work function serves as a tuneable parameter, modulating the interaction of hydrogen with TM compounds.

cond-mat.mtrl-sci↗

arXiv2024

Chemically Stable Group IV-V Transition Metal Carbide Thin Films in Hydrogen Radical Environments

Hydrogen is playing a crucial role in the green energy transition. Yet, its tendency to react with and diffuse into surrounding materials poses a challenge. Therefore, it is critical to develop coatings that protect hydrogen-sensitive system components in reactive-hydrogen environments. In this work, we report group IV-V transition metal carbide (TMC) thin films as potential candidates for hydrogen-protective coatings in hydrogen radical (H*) environments at elevated temperatures. We identify three classes of TMCs based on the reduction of carbides and surface oxides (TMOx). HfC, ZrC, TiC, TaC, NbC, and VC (class A) are found to have a stable carbidic-C (TM-C) content, with a further sub-division into partial (class A1: HfC, ZrC, and TiC) and strong (class A2: TaC, NbC, and VC) surface TMOx reduction. In contrast to class A, a strong carbide reduction is observed in Co2C (class B), along with a strong surface TMOx reduction. The H*-TMC/TMOx interaction is hypothesized to entail three processes: (i) hydrogenation of surface C/O-atoms, (ii) formation of CHx/OHx species, and (iii) subsurface C/O-atoms diffusion to the surface vacancies. The number of adsorbed H-atoms required to form CHx/OHx species (i), and the corresponding energy barriers (ii) are estimated based on the change in the Gibbs free energy (DeltaG) for the reduction reactions of TMCs and TMOx. Hydrogenation of surface carbidic-C-atoms is proposed to limit the reduction of TMCs, whereas the reduction of surface TMOx is governed by the thermodynamic barrier for forming H2O.

cond-mat.mtrl-sci↗

arXiv2024

Work-Function-Dependent Reduction of Transition Metal Nitrides in Hydrogen Environments

Amidst the growing importance of hydrogen in a sustainable future, it is crucial to develop coatings that can protect hydrogen-sensitive system components in reactive hydrogen environments. However, the prediction of the chemical stability of materials in hydrogen is not fully understood. In this study, we show that the work function is a key parameter determining the reducibility (i.e., de-nitridation) of transition metal nitrides (TMNs) in hydrogen radicals (H*) at elevated temperatures. We demonstrate that when the work function of a TMN system drops below a threshold limit, its reduction effectively stops. We propose that this is due to the preferential binding of H* to TM-atoms rather than N-atoms, which makes the formation of volatile species (NHx) unfavourable. This finding provides a novel perspective for comprehending the interaction of hydrogen with transition metal compounds and allows predicting the chemical stability of hydrogen-protective coatings.

cond-mat.mtrl-sci↗

arXiv2023

Resolving buried interfaces with Low Energy Ion Scattering

We investigate the use of Low Energy Ion Scattering (LEIS) to characterize buried interfaces of ultra-thin films. LEIS spectra contain depth-resolved information in the so-called sub-surface signal. However, the exact correlation between the sub-surface signal and the depth composition is still unknown. For this reason, LEIS spectra so far only provided qualitative information about buried interfaces. In this study, we investigate nm-thin films of Si-on-W and Si-on-Mo, where we compare simulated data to LEIS spectra. We present a method to extract depth-sensitive compositional changes -- resolving buried interfaces -- from LEIS spectra for the first few nanometers of a thin film sample. In the case of Si-on-Mo, the simulation of the LEIS sub-surface signal allows obtaining a quantitative measurement of the interface profile that matches the value determined using the LEIS layer growth profile method with an accuracy of 0.1 nm. These results pave the way to further extend the use of LEIS for the characterization of features buried inside the first few nanometers of a sample.

cond-mat.mtrl-sci↗

arXiv2022

Laser-induced electron dynamics and surface modification in ruthenium thin films

We performed the experimental and theoretical study of the heating and damaging of ruthenium thin films induced by femtosecond laser irradiation. Results of an optical pump-probe thermoreflectance experiment with rotating sample allowing to significantly reduce heat accumulation in irradiated spot are presented. We show the evolution of surface morphology from growth of a heat-induced oxide layer at low and intermediate laser fluences to cracking and grooving at high fluences. Theoretical analysis of pump-probe signal allows us to relate behavior of hot electrons in ruthenium to the Fermi smearing mechanism. The analysis of heating is performed with the two-temperature modeling and molecular dynamics simulation, results of which demonstrate that the calculated melting threshold is higher than experimental damage threshold. We attribute it to heat-induced surface stresses leading to cracking which accumulates to more severe damage morphology. Our results provide an upper limit for operational conditions for ruthenium optics and also direct to further studies of the Fermi smearing mechanism in other transition metals.

cond-mat.mtrl-sci↗

arXiv2018

Limits of surface analysis of thin film compounds using LEIS

Low Energy Ion Scattering (LEIS) was employed to study the surface composition of thin films of Ru on B, C and B4C films at different stages of growth. Effects of surface segregation of C were observed. Previously unknown matrix effects were observed in these samples, expressed in the decrease of LEIS signals of Ru, B and C at low Ru concentrations. The effect disappears for Ru-rich surfaces. Measurements with different He+ ion energies prove that the characteristic velocities of the elements involved change with surface composition. We suggest that these matrix effects appear due to the changes in neutralization efficiency in quasiresonant neutralization from the valence band (VB-qRN). This neutralization channel is present in elemental C and B due to a wide valence band with energy states as low as -20 eV, which are in a (quasi-)resonance with the He 1s level. This mechanism was earlier reported for graphitic carbon. We suggest that it can be applied to a much wider range of materials, leading to potential matrix effects in LEIS from a variety of surfaces, containing B, C and potentially O and N atoms, e.g. borides, carbides, oxides and nitrides, as well as alloys with B and C. This hypothesis is supported by additional LEIS measurements on oxidized Ru which show matrix effect in Ru-O LEIS signals as well. We argue that it is possible to avoid the matrix effects from compounded surfaces within certain ranges of composition by a proper choice of reference samples, while for other compositions knowledge of characteristic velocities is required for reliable quantification.

cond-mat.mtrl-sci↗