Atomic Processes Research Articles

Novel Fast-X-Ray Reflectivity Setup for Studying Electrochemical Interfaces

A fundamental understanding of atomic scale processes occurring at electrochemical interfaces is crucial for advancing the development of energy-related electrochemical systems such as ion batteries or fuel cells. For this purpose, operando experiments are imperative. X-ray reflectivity (XRR) is a non-destructive technique that enables operando analysis of buried structures with atomic resolution [1,2]. However, the time-resolution of typical XRR setups of minutes per XRR scan is limited by diffractometer motor motion and detector read-out times; this resolution is in many cases too slow to observe interfacial electrochemical phenomena [1,2].To overcome these limitations, we developed a novel fast-XRR setup, which employs a fast quasi-continuous rotation stage in combination with a stationary, high frame rate area detector. With this setup, the sample can be rotated with a frequency of up to 10 Hz, yielding sub-second time resolution for an individual XRR scan. In contrast to complementary fast-XRR setups [3,4], the presented setup can easily be combined with complex sample environments, as typically required for the investigation of electrochemical interfaces.We present first fast-XRR results obtained at PETRA III beamline P08 at DESY using 18 keV and a Dectris Eiger1M detector. We reached a time resolution below one second for an incident angular range between 0° – 6° (≙ 0 – 2 Å-1, i.e., covering the Fresnel XRR range). We measured several multilayer samples (e.g., 2 nm Ti / 20 nm Au coating on a Si substrate) and benchmarked the results to “standard” XRR measurements, where the measurements took several minutes. We find good agreement and conclude, that our novel setup provides significant XRR data within less than one second, demonstrating its usability for operando XRR measurements.Literature:[1] C. Cao, H.-G. Steinrück, Encyclopedia of Solid-Liquid Interfaces, 391–416, Elsevier, 2024.[2] C. Cao, H.-G. Steinrück et al., Nano Letters, 16, 12, 7394–7401, 2016.[3] M. Lippmann et al. Review of Scientific Instruments, 87, 113904, 2016.[4] H. Jorres et al., Applied Physics Letters, 114, 081904, 2019.

Electron diffraction of foam-like clusters between xenon and helium in superfluid helium droplets.

We report electron diffraction results of xenon clusters formed in superfluid helium droplets, with droplet sizes in the range of 105-106 atoms/droplet and xenon clusters from a few to a few hundred atoms. Under four different experimental conditions, the diffraction profiles can be fitted using four atom pairs of Xe. For the two experiments performed with higher helium contributions, the fittings with one pair of Xe-He and three pairs of Xe-Xe distances are statistically preferred compared with four pairs of Xe-Xe distances, while the other two experiments exhibit the opposite preference. In addition to the shortest pair distances corresponding to the van der Waals distances of Xe-He and Xe-Xe, the longer distances are in the range of the different arrangements of Xe-He-Xe and Xe-He-He-Xe. The number of independent atom pairs is too many for the small xenon clusters and too few for the large clusters. We consider these results evidence of xenon foam structures, with helium atoms stuck between Xe atoms. This possibility is confirmed by helium time-dependent density functional calculations. When the impact parameter of the second xenon atom is a few Angstroms or longer, the second xenon atom fails to penetrate the solvation shell of the first atom, resulting in a dimer with a few He atoms in between the two Xe atoms. In addition, our results for larger droplets point toward a multi-center growth process of dopant atoms or molecules, which is in agreement with previous proposals from theoretical calculations and experimental results.

Atomic Precision Processing of Two-Dimensional Materials for Next-Generation Microelectronics.

The growth of the information era economy is driving the pursuit of advanced materials for microelectronics, spurred by exploration into "Beyond CMOS" and "More than Moore" paradigms. Atomically thin 2D materials, such as transition metal dichalcogenides (TMDCs), show great potential for next-generation microelectronics due to their properties and defect engineering capabilities. This perspective delves into atomic precision processing (APP) techniques like atomic layer deposition (ALD), epitaxy, atomic layer etching (ALE), and atomic precision advanced manufacturing (APAM) for the fabrication and modification of 2D materials, essential for future semiconductor devices. Additive APP methods like ALD and epitaxy provide precise control over composition, crystallinity, and thickness at the atomic scale, facilitating high-performance device integration. Subtractive APP techniques, such as ALE, focus on atomic-scale etching control for 2D material functionality and manufacturing. In APAM, modification techniques aim at atomic-scale defect control, offering tailored device functions and improved performance. Achieving optimal performance and energy efficiency in 2D material-based microelectronics requires a comprehensive approach encompassing fundamental understanding, process modeling, and high-throughput metrology. The outlook for APP in 2D materials is promising, with ongoing developments poised to impact manufacturing and fundamental materials science. Integration with advanced metrology and codesign frameworks will accelerate the realization of next-generation microelectronics enabled by 2D materials.

Simulation of the formation process of nanofluid electrostatic atomization under different voltages

Simulation of the formation process of nanofluid electrostatic atomization under different voltages

The formation process and mechanism of coaxial electrostatic atomization of nanofluid oil film droplets

Abstract In coaxial electrostatic atomization cutting, the atomization effect of nanofluid oil film droplets directly affects the cooling and lubrication performance. To further understand the formation process of tiny oil film water droplets in coaxial electrostatic atomization, this paper takes LB2000/water, LB2000/0.1 vol.% graphite water-based nanofluids, LB2000/0.3 vol.% graphite water-based nanofluids, LB2000/0.5 vol.% graphite water-based nanofluids as the research object. Coaxial electrostatic atomization simulation is carried out based on the determined common voltage of the conical jet (-6.5 kV). The formation process of nanofluid oil film water droplets was analyzed using electric field force, charge concentration, and volume force, and the droplet states under different fluid types were compared. The results show that when nanoparticles are added to the inner fluid, the charge concentration increases, the electric field force and volume increase, and the formation speed of the cone jet increases significantly.

Revisiting the statistical equilibrium of H- in stellar atmospheres

The negative hydrogen ion is, almost without exception, treated in local thermodynamic equilibrium (LTE) in the modelling of F, G, and K stars, where it is the dominant opacity source in the visual spectral region. This assumption rests in practice on a study from the 1960s. Since that work, knowledge of relevant atomic processes and theoretical calculations of stellar atmospheres and their spectra have advanced significantly, but this question has not been reexamined. We present calculations based on a slightly modified analytical model that includes H and together with modern atomic data and a grid of 1D LTE theoretical stellar atmosphere models with stellar parameters ranging from T$_ eff = 4000$ to 7000 K, $ g = 1$ to 5 cm/s$^2$, and Fe/H $=-3$ to 0. We find direct non-LTE effects on populations in spectrum-forming regions, continua, and spectral lines of about 1--2<!PCT!> in stars with higher T$_ eff $ and/or lower $ g$. Effects in models for solar parameters are smaller by a factor of 10, about 0.1--0.2<!PCT!>, and are practically absent in models with lower T$_ eff $ and/or higher $ g$. These departures from LTE found in our calculations originate from the radiative recombination of electrons with hydrogen to form exceeding photodetachment, that is, overrecombination. Modern atomic data are not a source of significant differences compared to the previous work, although detailed data for processes on resolved with vibrational and rotational states provide a more complete and complex picture of the role of in the equilibrium of In the context of modern studies of stellar spectra at the percent level, our results suggest that this question requires further attention, including a more extensive reaction network, and indirect effects due to non-LTE electron populations.

Effect of Bias Frequency on Bottom-Up SiO2 Gap-Filling Using Plasma-Enhanced Atomic Layer Deposition.

High-aspect-ratio patterns are required for next-generation three-dimensional (3D) semiconductor devices. However, it is challenging to eliminate voids and seams during gap-filling of these high-aspect-ratio patterns, such as deep trenches, especially for nanoscale high-aspect-ratio patterns. In this study, a SiO2 plasma-enhanced atomic layer deposition process incorporated with ion collision using bias power to the substrate was used for bottom-up trench gap-filling. The effect of bias power frequency on SiO2 trench gap-filling was then investigated. Results showed that changes in bias power frequency did not significantly change the process rate, such as SiO2 growth per cycle. At relatively low bias power frequencies, high-energy ions formed an overhang at the entrance of the high-aspect-ratio trench pattern through sputter etching and redeposition, blocking the pattern entrance. However, at relatively high-frequency bias power, overhang formation due to sputtering did not occur. In the trench interior, due to a scattering effect of ions, deposition was thicker at the bottom of the trench than that at the top, achieving bottom-up gap-filling and void-free gap-filling.

The Consequences of Random Sequential Adsorption for the Precursor Packing and Growth-Per-Cycle of Atomic Layer Deposition Processes.

Atomic layer deposition (ALD) processes are known to deposit submonolayers of material per cycle, primarily attributed to steric hindrance and a limited number of surface sites. However, an often-overlooked factor is the random sequential adsorption (RSA) mechanism, where precursor molecules arrive one-by-one and adsorb at random surface sites. Consequently, the saturation coverage of precursors significantly deviates from ideal closed packing. In this study, we investigated the influence of RSA on precursor adsorption saturation and, consequently, on the growth per cycle (GPC) of the ALD processes. Our simulations revealed that the RSA model leads to a 22% to 40% lower surface density compared to the reference case of ordered packing. Furthermore, based on the precursor shape and size, we estimated GPC values with an average accuracy of 0.05 Å relative to experimental literature data. This work shows the critical role of RSA in ALD, emphasizing the need to consider this mechanism for a more accurate process design and optimization.

Revealing the controlling mechanisms of atomic layer etching for high-k dielectrics in conventional inductively coupled plasma etching tool

The possibilities of optimization of the two-step atomic layer etching process for HfO2 in conventional plasma etching tools were studied. The surface modification step was realized in Ar/CF4/H2 plasma, and the reaction between the modified layer and the surface was activated by Ar ion bombardment from the plasma in the second step. Investigation of the effects of activation step duration, DC bias during activation, and Ar plasma density was carried out. The mechanism of the etching process has been shown to involve fluorination of oxide during the modification step and subsequent removal of fluorine-containing particles at the activation step. An increase in parasitic sputtering rate and lower process saturation with the growth of DC bias during activation was demonstrated. The advantage of the ALE process in lower surface roughness over the conventional etching process was shown. Similar etching characteristics of HfO2 and ZrO2 suggest a similarity in the etching process for the mixed hafnium-zirconium oxide material.

Application of KH-RT model in lifting flame of methanol jet atomization

Abstract For the methanol jet atomization in a co-flow gas lifting flame, the self-developed WAVE model and KH-RT model were employed using the Saturne program to simulate the primary breakup of the jet column and the atomization of spray particles. Additionally, the unsteady flamelet model was utilized to simulate the combustion process. Comparing the calculated flame lifting height, droplet diameter distribution, and velocity distribution with experimental results demonstrates the atomization model’s ability to accurately capture the methanol fuel atomization process. This comparison verifies the reliability of both the atomization and combustion models, indicating their high accuracy. The study shows that upon injection from the nozzle, methanol fuel rapidly diffused, creating a cone-shaped spray structure. The high concentration of OH radicals is located close to the boundary between the regions of OH radical distribution and methanol distribution, gradually spreading downstream of the methanol jet. Furthermore, an increase in fuel flow rate resulted in a reduction in the flame’s lift height.

Evolution of level population in Ar interacting with XFEL pulses: impact of resonant absorptions

Theoretical exploration of the population dynamics at fine-structure levels of Ar atoms interacting with ultrafast ultraintense x-ray free electron laser (XFEL) pulses is conducted. A time-dependent rate equation based on a detailed-level accounting approach is applied for tracking population levels, encompassing microscopic atomic processes such as photoexcitation, radiative decay, photoionization and Auger decay. A Monte Carlo algorithm is implemented to solve large-scale rate equations efficiently. The primary investigation centers on generating Ar17+ through resonant absorption by the second-harmonic radiation of the x-ray pulse. The calculated population ratios of Ar17+ to Ar16+ align well with the experimental measurements (LaForge et al 2021 Phys. Rev. Lett. 127 213202). In comparison to the transition energy of the strongest line, (1s2)0→(1s1/22p3/2)1 of Ar16+, there is a distinct ∼25 eV red shift in the peak ratio, which is attributed to the presence of intricate resonant channels in the lower ionization stages. The results demonstrate the sensitivity of the population ratio Ar17+/Ar16+ to the laser pulse parameters such as x-ray pulse duration, bandwidth and the contribution of second-harmonic radiation, indicating their potential as diagnostic tools in future experiments.

Design and experimental research of air-assisted nozzle for pesticide application in orchard.

This article reports the design and experiment of a novel air-assisted nozzle for pesticide application in orchard. A novel air-assisted nozzle was designed based on the transverse jet atomization pattern. This article conducted the performance and deposition experiments and established the mathematical model of volume median diameter (D50) and liquid flow rate with the nozzle design parameters. The D50 of this air-assisted nozzle ranged from 52.45 μm to 113.67 μm, and the liquid flow rate ranged from 142.6 ml/min to 1,607.8 ml/min within the designed conditions. These performances meet the low-volume and ultra-low-volume pesticide application in orchard. The droplet deposition experiment results demonstrated that the droplet coverage distribution in different layers and columns is relatively uniform, and the predicted value of spray penetration (SP) numbers SPiA , SPiB , and SPiC (i = 1, 2, and 3) are approximately 70%, 60%, and 70%, respectively. The droplet deposits on the foliage of the canopy (inside and outside) uniformly bring benefit for plant protection and pesticide saving. Compared with the traditional air-assisted nozzle that adopts a coaxial flow atomization pattern, the atomization efficiency of this air-assisted nozzle is higher. Moreover, the nozzle air pressure and liquid flow rate are considerably lower and greater than the traditional air-assisted nozzle, and these results proved that this air-assisted nozzle has great potential in orchard pesticide application. The relationship between the D50 and nozzle liquid pressure of this air-assisted nozzle differs from that of traditional air-assisted nozzles due to the atomization pattern and process. While this article provides an explanation for this relationship, further study about the atomization process and mechanism is needed so as to improve the performance.

Prospective life cycle assessment of titanium powder atomization

The environmental sustainability of titanium powders production mainly depends by atomization that is the most diffused technology in this field, ensuring the environmental advantages of high mass flow rate, energetical efficiency and reduced waste which have greatly encouraged its diffusion on an industrial scale. However, few quantitative assessment studies have been proposed on atomization sustainability and none of them consider the many technological evolutions of atomization that the industries are working on. This study proposes a prospective life cycle assessment (LCA), of the ex-ante type, of future new Electrode Induction Gas Atomization (EIGA) and Plasma Rotating Electrode Process (PREP) that will produce Ti6Al4V powders in 2035. This time point, referring to a medium-term view is considered to ensure the relevance and the reliability of technology forecasts based on quantitative estimates. Both the systems have been modelled through data retrieved from patents to assess their future impacts. The prospective LCA shows that in the future EIGA the average impact, in each indicator, will be 50% lower for electrical consumption and 98% lower for argon consumption compared to future PREP. The future EIGA and future PREP are more sustainable than the mature EIGA (of the crucible and crucible-free type) and mature PREP (of the traditional and supreme-speed plasma type) currently on the market. The average impact reductions, respectively passing from future to mature EIGA and PREP, are 65% and 23% for electricity consumption and 11% and 28% for argon consumption. The variabilities in technological solutions, scalability and future scenarios about electricity and argon production scale all the impacts without reverse the ranking. At a structural level, the most sustainable solutions are the optimization of the geometries of the titanium bar in the future EIGA and the optimization of the disposition of the plasma gun in the future PREP. This study shows which technological advancement increase the sustainability of EIGA and PREP atomization process in the future and to what extent in the two cases.

Boiling induced atomization of liquid film produced by oblique jet impingement on superheated wall

For the thermal management of industrial devices, a reduction in the net coolant flow rate by droplet dispersion from a liquid film is important because it can cause unexpected thermal failure. To understand the process of droplet dispersion from a liquid film better, we experimentally and theoretically evaluated the characteristics of boiling-induced atomization in a liquid film formed by oblique jet impingement on a superheated wall. Atomization processes were visualized using magnified high-speed imaging using a backlight technique. In this study, two types of droplets were observed using high-speed-magnification imaging. These were large droplets that disintegrated from the ligament formed on a relatively high-temperature wall, and small droplets from the ligament formed via bubble bursting in the nucleate boiling regime. For the atomization induced by nucleate boiling, larger droplets were produced via bubble bursting further downstream from the impingement point because the bubble size and liquid film thickness increased. Finally, the total volume of the droplets produced by nucleate boiling was estimated from the frequency of bubble bursting and droplet size measured from the visualization results. The estimation results suggest that the ratio of the total volume flow rate of the ejected droplets to the injection flow rate of the liquid was negligible (2%). Thus, most of the injected liquid eventually reached the wetting front of the sheet, separating it from the wall before drying out.

Investigations of atomic and molecular processes of NBI-heated discharges in the MAST Upgrade Super-X divertor with implications for reactors

This experimental study presents an in-depth investigation of the performance of the MAST-U Super-X divertor during NBI-heated operation (up to 2.5 MW) focussing on volumetric ion sources and sinks as well as power losses during detachment. The particle balance and power loss analysis revealed the crucial role of Molecular Activated Recombination and Dissociation (MAR and MAD) ion sinks in divertor particle and power balance, which remain pronounced in the change from ohmic to higher power (NBI heated) L-mode conditions. The importance of MAR and MAD remains with double the absorbed NBI heating. MAD results in significant power dissipation (up to ∼20% of PSOL ), mostly in the cold ( Te<5 eV) detached region. Theoretical and experimental evidence is found for the potential contribution of D− to MAR and MAD, which warrants further study. These results suggest that MAR and MAD can be relevant in higher power conditions than the ohmic conditions studied previously. Post-processing reactor-scale simulations suggests that MAR and MAD can play a significant role in divertor physics and synthetic diagnostic signals of reactor-scale devices, which are currently underestimated in exhaust simulations. This raises implications for the accuracy of reactor-scale divertor simulations of particularly tightly baffled (alternative) divertor configurations.

Atomic transport dynamics in crossed optical dipole trap

Abstract We study the dynamical evolution of cold atoms in crossed optical dipole trap theoretically and experimentally. The atomic transport process is accompanied by two competitive kinds of physical mechanics, atomic loading and atomic loss. The loading process normally is negligible in the evaporative cooling experiment on the ground, while it is significant in preparation of ultra-cold atoms in the space station. Normally, the atomic loading process is much weaker than the atomic loss process, and the atomic number in the central region of the trap decreases monotonically, as reported in previous research. However, when the atomic loading process is comparable to the atomic loss process, the atomic number in the central region of the trap will initially increase to a maximum value and then slowly decrease, and we have observed the phenomenon first. The increase of atomic number in the central region of the trap shows the presence of the loading process, and this will be significant especially under microgravity conditions. We build a theoretical model to analyze the competitive relationship, which coincides with the experimental results well. Furthermore, we have also given the predicted evolutionary behaviors under different conditions. This research provides a solid foundation for further understanding of the atomic transport process in traps. The analysis of loading process is of significant importance for preparation of ultra-cold atoms in a crossed optical dipole trap under microgravity conditions.

Optimization of the gas system for gas–water combined atomization technique in FeSiBC amorphous powder production

The gas–water combined atomization is an advanced technology for Fe-based amorphous powder preparation, and its gas/water system parameters have significant impacts on powder properties. In this study, numerical simulations and industrial trials were combined to optimize the gas atomization parameters. The results showed that increasing the atomization pressure promotes the transition of the flow field to the closed wake. Moreover, the median particle size was significantly refined and the cooling rate was improved. Extending the extrusion length facilitated the decrease in suction pressure, while excessively long extrusion lengths led to instability in the atomization process. The decrease in delivery tube diameter enhances droplet breakup and cooling, but increases the risk of clogging. Industrial trials at different atomization pressures showed that low atomization pressure led to the formation of needle-shaped powder, and the FeSiBC amorphous powder prepared at 3.0 MPa exhibited optimal comprehensive properties, with saturation magnetization of 166.1 emu·g−1 and coercivity of 4.5 Oe.

Molecular dynamics simulations and analyzation of Cu deposited on stainless steel substrate surfaces

Copper (Cu) is used in integrated circuits and microdevices and has the potential to replace aluminum alloys due to its low resistivity, strong electromigration properties, and affordability. However, a significant factor that influences the performance of devices at the micro and nano scales is the surface roughness of the deposits. LAMMPS software is employed to simulate the deposition Cu on an ideal state for a stainless-steel substrate. The deposition process and deformation behavior of Cu on the surface and the roughness of the deposition surface are analyzed. Taking the deposition process of Cu atoms as an object, the effects of different atomic numbers, different temperatures, different velocities, and different heights on the surface roughness of the deposits were investigated. The atomic structure composition of the deposition velocity is analyzed, and the radial distribution function is analyzed to reveal the microscopic mechanism of action. The results of the theoretical deposition and analysis show that the surface roughness increases with the number of atoms deposited and decreases with increasing substrate temperature. The surface roughness first decreases and then, after some fluctuation, stays constant at a particular level with increasing velocity. Additionally, as the deposition height increases, the surface roughness reduces. There is a nonlinear relationship between the various components and the deposited surface roughness. The surface quality of deposits can be improved during the deposition process by optimizing the deposition parameters of deposition atoms, substrate temperature, deposition velocity, and deposition height.

Effect of neural firing pattern on NbOx/Al2O3 memristor-based reservoir computing system

The implementation of reservoir computing using resistive random-access memory as a physical reservoir has attracted attention due to its low training cost and high energy efficiency during parallel data processing. In this work, a NbOx/Al2O3-based memristor device was fabricated through a sputter and atomic layer deposition process to realize reservoir computing. The proposed device exhibits favorable resistive switching properties (&amp;gt;103 cycle endurance) and demonstrates short-term memory characteristics with current decay. Utilizing the controllability of the resistance state and its variability during cycle repetition, electrical pulses are applied to investigate the synapse-emulating properties of the device. The results showcase the functions of potentiation and depression, the coexistence of short-term and long-term plasticity, excitatory post-synaptic current, and spike-rate dependent plasticity. Building upon the functionalities of an artificial synapse, pulse spikes are categorized into three distinct neural firing patterns (normal, adapt, and boost) to implement 4-bit reservoir computing, enabling a significant distinction between “0” and “1.”

Shadowgraph tomography of a high-pressure GDI spray

An isooctane spray from a high-pressure multihole GDI injector (Bosch HDEV6) was characterised by means of optical extinction tomography, relying on collimated illumination by a focused shadowgraph setup. The tests were carried out in air under ambient conditions at an injection pressure of 300 bar. Spray images were acquired over a 180-degree angular range in 1-degree increments. The critical issues of optical extinction tomography of sprays, related to the strong light extinction by the dense liquid core of fuel jets, were addressed. To mitigate artefacts arising from the reconstruction process, the extinction data were subjected to spatially-variant filtering steps for both raw and post-log data before being analytically inverted through the inverse Radon transform. This approach made it possible to process extinction data at very large optical depths. A nearly complete three-dimensional reconstruction of the spray was obtained, providing significant details of the spray morphology and the internal structure of the jets throughout spray development. Different phases of the atomization process, from the near-field to the far-field regions of the spray, were observed.