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We use molecular dynamics (MD) simulation with numerical characterisation and statistical analysis to study the mechanisms of damage evolution and p-type doping efficiency by aluminum (Al) ion implantation into 3C silicon carbide (SiC) with subsequent annealing. By incorporating the electronic stopping power for implantation, a more accurate description of the atomic-scale mechanisms of damage evolution and distribution in SiC can be obtained. The simulation results show a novel observation that the recrystallization process occurs in the region below the subsurface layer, and develops from amorphous-crystalline interface to the damage center region, which is a new insight into previously published studies. During surface recrystallization, significant compressive stress concentration occurs, and more structural phase transition atoms and dislocations formed at the damage-rich-crystalline interface. Another point of interest is that for low-dose implantation, more implantation-induced defects hamper the doping efficiency. Correspondingly, the correlation between lattice damage and doping efficiency becomes weaker as the implant dose increases under the same annealing conditions. Our simulation also predicts that annealing after high temperature (HT) implantation is more likely to lead to the formation of carbon vacancies (V-C).

As a promising material for quantum technology, silicon carbide (SiC) has attracted great interest in materials science. Carbon vacancy is a dominant defect in 4H-SiC. Thus, understanding the properties of this defect is critical to its application, and the atomic and electronic structures of the defects needs to be identified. In this study, density functional theory was used to characterize the carbon vacancy defects in hexagonal (h) and cubic (k) lattice sites. The zero-phonon line energies, hyperfine tensors, and formation energies of carbon vacancies with different charge states (2−, −, 0,+ and 2+) in different supercells (72, 128, 400 and 576 atoms) were calculated using standard Perdew-Burke-Ernzerhof and Heyd-Scuseria-Ernzerhof methods. Results show that the zero-phonon line energies of carbon vacancy defects are much lower than those of divacancy defects, indicating that the former is more likely to reach the excited state than the latter. The hyperfine tensors of VC+(h) and VC+(k) were calculated. Comparison of the calculated hyperfine tensor with the experimental results indicates the existence of carbon vacancies in SiC lattice. The calculation of formation energy shows that the most stable carbon vacancy defects in the material are VC2+(k), VC+(k), VC(k), VC−(k) and VC2−(k) as the electronic chemical potential increases.

We present evidence of homogenization of atomic diffusion properties caused by C and N interstitials in an equiatomic single-phase high entropy alloy (FeMnNiCoCr). This phenomenon is manifested by an unexpected interstitial-induced reduction and narrowing of the directly experimentally determined migration barrier distribution of mono-vacancy defects introduced by particle irradiation. Our observation by positron annihilation spectroscopy is explained by state-of-the-art theoretical calculations that predict preferential localization of C/N interstitials in regions rich in Mn and Cr, leading to a narrowing and reduction of the mono-vacancy size distribution in the random alloy. This phenomenon is likely to have a significant impact on the mechanical behavior under irradiation, as the local variations in elemental motion have a profound effect on the solute strengthening in high entropy alloys. (C) 2021 The Authors. Published by Elsevier Ltd on behalf of Acta Materialia Inc.

${\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ is a wide-band-gap semiconductor of great interest for applications in electronics and optoelectronics. Two-dimensional (2D) ${\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ synthesized from top-down or bottom-up processes can reveal new heterogeneous structures and promising applications. In this paper, we study phase transitions among three low-energy stable ${\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ monolayer configurations using density functional theory and a machine learning Gaussian approximation potential, together with solid-state nudged elastic band calculations. Kinetic minimum energy paths involving direct atomic jump as well as concerted layer motion are investigated. The low phase transition barriers indicate feasible tunability of the phase transition and orientation via strain engineering and external electric fields. Large-scale calculations using the trained machine learning potential on the thermally activated single-atom jumps reveal the clear nucleation and growth processes of different domains. The results provide useful insights into future experimental synthesis and characterization of 2D ${\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ monolayers.

The matrix assembly cluster source (MACS) represents a bridge between conventional instruments for cluster beam deposition (CBD) and the level of industrial production. The method is based on Ar+ ion sputtering of a pre-condensed Ar-M matrix (where M, is typically a metal such as Ag). Each Ar+ ion produces a collision cascade and thus the formation of metal clusters is in the matrix, which are then sputtered out. Here we present an experimental and computational investigation of the cluster emission process, specifically its dependence on the Ar+ ion angle of incidence and the cluster emission angle. We find the incidence angle strongly influences the emerging cluster flux, which is assigned to the spatial location of the deposited primary ion energy relative to the cluster into the matrix. We also found an approximately constant angle between the incident ion beam and the peak in the emitted cluster distribution, with value between 99° and 109°.

A two-dimensional (2D) Ga2O3 monolayer with an asymmetric quintuple-layer configuration was reported as a novel 2D material with excellent stability and strain tunability. This unusual asymmetrical structure opens up new possibilities for improving the selectivity and sensitivity of gas sensors by using selected surface orientations. In this study, the surface adsorptions of nine molecular gases, namely, O2, CO2, CO, SO2, NO2, H2S, NO, NH3, and H2O, on the 2D Ga2O3 monolayer are systematically investigated through first-principles calculations. The intrinsic dipole of the system leads to different adsorption energies and changes in the electronic structures between the top- and bottom-surface adsorptions. Analyses of electronic structures and charge transport calculations indicate a potential application of the 2D Ga2O3 monolayer as a room-temperature NO gas-sensing device with high sensitivity and tunable adsorption energy using plenary strain-induced lattice distortion.

Atomic and close-to-atomic scale fabrication with high yield for the color centers in silicon carbide is critical in developing its applications. Combined with Wigner-Seitz method and identify diamond structure method to consider the structure around the silicon vacancy (VSi), it is found that He ion implantation is more likely to fabricate a small number of silicon vacancies with complete structure but locating deep, while Si ion implantation is more likely to introduce more silicon vacancies with incomplete structure but a large number and closer to the near surface. Therefore, a method of dual ion implantation is proposed in this paper. By adjusting the ratio of He to Si ion concentration for dual ion implantation, the fabrication yield of color centers with depth below 5 nm can be increased compared with that of He implantation after high temperature annealing. Molecular dynamics (MD) simulation is employed to discover the underlying mechanism of VSi color center and damage evolution by helium ion and dual ion implantation into four-hexagonal silicon carbide (4H–SiC) with subsequent annealing. Density-functional theory (DFT) calculation proves that magnetic-spin polarization enhances the stability of carbon anti-vacancy pair (CSiVC) defect, which indicates CSiVC defects are more stable than VSi defects. The evolution of the VSi color centers of different defect models are also calculated at various temperatures by MD, and the dynamic process of VSi defects to CSiVC defects is demonstrated. It is revealed that the decrease of the VSi color center at high temperature annealing is partly due to the transformation of some silicon vacancies to CSiVC defects.

Nanomaterials undergoing cyclic swelling-deswelling benefit from inner void spaces that help accommodate significant volumetric changes. Such flexibility, however, typically comes at a price of reduced mechanical stability, which leads to component deterioration and, eventually, failure. Here, we identify an optimised building block for silicon-based lithium-ion battery (LIB) anodes, fabricate it with a ligand- and effluent-free cluster beam deposition method, and investigate its robustness by atomistic computer simulations. A columnar amorphous-silicon film was grown on a tantalum-nanoparticle scaffold due to its shadowing effect. PeakForce quantitative nanomechanical mapping revealed a critical change in mechanical behaviour when columns touched forming a vaulted structure. The resulting maximisation of measured elastic modulus (similar to 120GPa) is ascribed to arch action, a well-known civil engineering concept. The vaulted nanostructure displays a sealed surface resistant to deformation that results in reduced electrode-electrolyte interface and increased Coulombic efficiency. More importantly, its vertical repetition in a double-layered aqueduct-like structure improves both the capacity retention and Coulombic efficiency of the LIB. Lithiation of anodes during cycling of lithium-ion batteries generates stresses that reduce operation lifetime. Here, a composite silicon-based anode with a nanoscale vaulted architecture shows high mechanical stability and electrochemical performance in a lithium-ion battery., Communications Materials, 2 (1), ISSN:2662-4443

Nanoparticles (NPs), as the most prototypical functional building blocks in nanoscience, exhibit size-, shape-, composition-, and structure-dependent behavior which is different from the corresponding bulk materials. Arguably, the structures and properties of NPs cannot be understood purely from experimental data. Deeper insights can be gained by complementary theoretical or computational modeling. This chapter presents an introduction to simulations of metallic and semiconductor NPs in inert environment using multiscale computational modeling techniques, including density functional theory, classical molecular dynamics, and Monte Carlo methods. We review relevant results obtained with such simulations in the field of cluster beam deposition and comment on several challenges that need to be addressed in future.

Spontaneous growth of complexes consisted of a number of individual nanoparticles in a controlled manner, particularly in demanding environments of gas-phase synthesis, is a fascinating opportunity for numerous potential applications. Here, we report the formation of such core-satellite gold nanoparticle structures grown by magnetron sputtering inert gas condensation. Combining high-resolution scanning transmission electron microscopy and computational simulations, we reveal the adhesive and screening role of H2O molecules in formation of stable complexes consisted of one nanoparticle surrounded by smaller satellites. A single layer of H2O molecules, condensed between large and small gold nanoparticles, stabilizes positioning of nanoparticles with respect to one another during milliseconds of the synthesis time. The lack of isolated small gold nanoparticles on the substrate is explained by Brownian motion that is significantly broader for small-size particles. It is inferred that H2O as an admixture in the inert gas condensation opens up possibilities of controlling the final configuration of the different noble metal nanoparticles.

Atomistic rigid lattice Kinetic Monte Carlo (KMC) is an efficient method for simulating nano-objects and surfaces at timescales much longer than those accessible by molecular dynamics. A laborious and non-trivial part of constructing any KMC model is, however, to calculate all migration barriers that are needed to give the probabilities for any atom jump event to occur in the simulations. We calculated three data sets of migration barriers for Fe self-diffusion: barriers of first nearest neighbour jumps, second nearest neighbours hop-on jumps on the Fe {100} surface and a set of barriers of the diagonal exchange processes for various cases of the local atomic environments within the 2nn coordination shell. Keywords: Copper, Iron, Kinetic Monte Carlo, Surface diffusion, Rigid lattice, Migration barriers, Atomic jumps

We present a numerical study on swift ion induced effects in crystalline 3C silicon carbide (SiC) by the two-temperature model, which considering the electronic stopping and electronic-phonon coupling effects simultaneously. Given the results of overlapping radiation, there is only a minority of defects formed in the system during the ionization dominance stage. When the incident energy is braked from 20 MeV to 500 keV by ionization after the first 0.91 ps, the system enters the nuclear stopping stage, the incident energy decreases to 50 keV in 0.44 ps, accomplished with a dramatic increase of damage. In addition, for the low-energy ion implantation process, the sparse atomic arrangement perpendicular to the implantation direction will reduce the response of the atomic subsystem. Insights into the complex correlations between electronic and atomic response may pave the way to elucidate the mechanism behind the experimentally observed defect formation and evolution under extreme energy deposition.

Ion doping technology with precise control of doping concentration and configuration can optimize the performance of β-phase gallium oxide (β-Ga2O3) high-power electronic and optoelectronic devices. In this work, shallow-donor Si and deep-acceptor Mg impurities are doped in β-Ga2O3 separately using edge-defined film-fed growth (EFG) method. Laser scanning confocal microscopy and X-ray diffraction analyses show that the as-grown un/Si/Mg-doped β-Ga2O3 substrates have superior qualities such as smooth surface, homogenous phase, and high crystallinity. Raman spectroscopy analysis indicate that the Raman shift and full width at half-maximum (FWHM) has a linear relationship with temperature in the range of 77–297 K. The temperature-variable photoluminescence (PL) spectroscopy suggests that the Si doping introduces less damage to the β-Ga2O3 lattice structure and the Si-doped sample has higher stability at different temperatures, however, the local atomic configurations of Mg impurities can be more easily/significantly affected by temperature. The work can offer an insightful reference to applications of ion-doped β-Ga2O3 optoelectronic devices.

Volume: 406 Host publication title: Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms The results of molecular dynamics simulations of the bombardment of the Cu (100) and Mo (100) single-crystals by 10 keV Ar cluster ions of different sizes are presented in this paper. Spatial distributions of sputtered material were calculated. The anisotropy of the angular distributions of sputtered atoms was revealed. It was found that the character of the anisotropy is different for Cu and Mo targets. The reasons leading to this anisotropy are discussed according to the dependences of the angular distributions on the cluster size and on the target material.

The structure of heterogeneous nanocatalysts supported on metal oxide materials and their morphological changes during oxidation/reduction processes play a crucial role in determining the resulting catalytic activity. Herein, we study the thermal oxidation mechanism of Pd nanoparticles supported on CuO nanowires by combining in situ environmental transmission electron microscopy (TEM), ex situ experiments, and ab initio density functional theory (DFT) calculations. High-resolution TEM imaging assisted by geometric phase analysis enabled the analysis of partially oxidized, fully oxidized, and distinct onion-like Pd nanoparticles with subsurface dislocations. Furthermore, preferential crystalline orientations between PdO nanoparticles and the CuO nanowire support have been found. Hence, the CuO–Pd interface is crucial for the thermal oxidation of Pd nanoparticles, as corroborated by electron energy loss spectroscopy and DFT calculations. The latter revealed a considerably lower energy barrier for penetratio...

In this paper, a model of helium ion implanted monocrystalline Si was constructed by using molecular dynamics (MD) simulation method to study the interaction mechanism of helium ion with monocrystalline Si and helium ion migration. In order to study the damage effect of helium ion implantation on monocrystalline Si, identify diamond structure (IDS), radial distribution function, temperature analysis were calculated and analyzed. The effects of ion doses, beam currents and energies on the damage were studied. Helium ion implanted Si with ion doses of 1 x 10(14)/cm(2) was subsequently heated to 300 K. MD simulation results indicated that IDS damage induced by ion implantation was positively correlated with ion doses as the ion implantation increased to 1 x 10(14)/cm(2). The mean-square displacement of helium atoms was calculated during the temperature rising to 300 K. It was found that the high permeability of helium atoms in Si and the acceleration of atomic thermal motion owing to elevated temperature as well as the existence of larger stress would be helpful to the migration of implant helium atoms.

To this day, engineering nanoalloys beyond bimetallic compositions has scarcely been within the scope of physical deposition methods due to the complex, nonequilibrium processes they entail. Here, we report a gas-phase synthesis strategy for the growth of multimetallic nanoparticles: magnetron-sputtering inert-gas condensation from neighboring monoelemental targets provides the necessary compositional flexibility, whereas in-depth atomistic computer simulations elucidate the fast kinetics of nucleation and growth that determines the resultant structures. We fabricated consistently trimetallic Au–Pt–Pd nanoparticles, a system of major importance for heterogeneous catalysis applications. Using high-resolution transmission electron microscopy, we established their physical and chemical ordering: Au/Pt-rich core@Pd-shell atomic arrangements were identified for particles containing substantial amounts of all elements. Decomposing the growth process into basic steps by molecular dynamics simulations, we identified a fundamental difference between Au/Pt and Pd growth dynamics: Au/Pt electronic arrangements favor the formation of dimer nuclei instead of larger-size clusters, thus significantly slowing down their growth rate. Consequently, larger Pd particles formed considerably faster and incorporated small Au and Pt clusters by means of in-flight decoration and coalescence. A broad range of icosahedral, truncated-octahedral, and spheroidal face-centered cubic trimetallic nanoparticles were reproduced in simulations, in good agreement with experimental particles. Comparing them with their expected equilibrium structures obtained by Monte Carlo simulations, we identified the particles as metastable, due to out-of-equilibrium growth conditions. We aspire that our in-depth study will constitute a significant advance toward establishing gas-phase aggregation as a standard method for the fabrication of complex nanoparticles by design.

Atomistic rigid lattice Kinetic Monte Carlo (KMC) is an efficient method for simulating nano-objects and surfaces at timescales much longer than those accessible by molecular dynamics. A laborious and non-trivial part of constructing any KMC model is, however, to calculate all migration barriers that are needed to give the probabilities for any atom jump event to occur in the simulations. We have calculated three data sets of migration barriers for Cu self-diffusion with two different methods. The data sets were specifically calculated for rigid lattice KMC simulations of copper self-diffusion on arbitrarily rough surfaces, but can be used for KMC simulations of bulk diffusion as well.

In this paper, we study the mechanisms of growth of Ag nanoclusters in a solid Ar matrix and the emission of these nanoclusters from the matrix by a combination of experimental and theoretical methods. The molecular dynamics simulations show that the cluster growth mechanism can be described as "thermal spike-enhanced clustering" in multiple sequential ion impact events. We further show that experimentally observed large sputtered metal clusters cannot be formed by direct sputtering of Ag mixed in the Ar. Instead, we describe the mechanism of emission of the metal nanocluster that, at first, is formed in the cryogenic matrix due to multiple ion impacts, and then is emitted as a result of the simultaneous effects of interface boiling and spring force. We also develop an analytical model describing this size-dependent cluster emission. The model bridges the atomistic simulations and experimental time and length scales, and allows increasing the controllability of fast generation of nanoclusters in experiments with a high production rate.

Atomistic rigid lattice Kinetic Monte Carlo is an efficient method for simulating nano-objects and surfaces at timescales much longer than those accessible by molecular dynamics. A laborious part of constructing any Kinetic Monte Carlo model is, however, to calculate all migration barriers that are needed to give the probabilities for any atom jump event to occur in the simulations. One of the common methods of barrier calculations is Nudged Elastic Band. The number of barriers needed to fully describe simulated systems is typically between hundreds of thousands and millions. Calculations of such a large number of barriers of various processes is far from trivial. In this paper, we will discuss the challenges arising during barriers calculations on a surface and present a systematic and reliable tethering force approach to construct a rigid lattice barrier parameterization of face-centred and body-centred cubic metal lattices. We have produced several different barrier sets for Cu and for Fe that can be used for KMC simulations of processes on arbitrarily rough surfaces. The sets are published as Data in Brief articles and available for the use.

A key challenge in nanotechnology is the rational design of multicomponent materials that beat the properties of their elemental counterparts. At the same time, when considering the material composition of such hybrid nanostructures and the fabrication process to obtain them, one should favor the use of nontoxic, abundant elements in view of the limited availability of critical metals and sustainability. Cluster beam deposition offers a solvent- and, therefore, effluent-free physical synthesis method to achieve nanomaterials with tailored characteristics. However, the simultaneous control of size, shape, and elemental distribution within a single nanoparticle in a small-size regime (sub-10 nm) is still a major challenge, equally limiting physical and chemical approaches. Here, a single-step nanoparticle fabrication method based on magnetron-sputtering inert-gas condensation is reported, which relies on selective wetting of specific surface sites on precondensed iron nanocubes by gold atoms. Using a newly developed Fe-Au interatomic potential, the growth mechanism is decomposed into a multistage model implemented in a molecular dynamics simulation framework. The importance of growth kinetics is emphasized through differences between structures obtained either experimentally or computationally, and thermodynamically favorable configurations determined via global optimization techniques. These results provide a roadmap for engineering complex nanoalloys toward targeted applications.

In this work, we study the formation mechanisms of iron nanoparticles (Fe NPs) grown by magnetron sputtering inert gas condensation and emphasize the decisive kinetics effects that give rise specifically to cubic morphologies. Our experimental results, as well as computer simulations carried out by two different methods, indicate that the cubic shape of Fe NPs is explained by basic differences in the kinetic growth modes of {100} and {110} surfaces rather than surface formation energetics. Both our experimental and theoretical investigations show that the final shape is defined by the combination of the condensation temperature and the rate of atomic deposition onto the growing nanocluster. We, thus, construct a comprehensive deposition rate-temperature diagram of Fe NP shapes and develop an analytical model that predicts the temporal evolution of these properties. Combining the shape diagram and the analytical model, morphological control of Fe NPs during formation is feasible; as such, our method proposes a roadmap for experimentalists to engineer NPs of desired shapes for targeted applications.

In the nanoregime, chemical species can reorganize in ways not predicted by their equilibrium bulk behavior. Here, we engineer Ni-Cr nanoalloys at the magnetic end of their compositional range (i.e., 0–15 at. % Cr), and we investigate the effect of Cr incorporation on their structural stability and resultant magnetic ordering. To ensure their stoichiometric compositions, the nanoalloys are grown by cluster beam deposition, a method that allows one-step, chemical-free fabrication of bimetallic nanoparticles. While full Cr segregation toward nanoparticle surfaces is thermodynamically expected for low Cr concentrations, metastability occurs as the Cr dopant level increases in the form of residual Cr in the core region, yielding desirable magnetic properties in a compensatory manner. Using nudged elastic band calculations, residual Cr in the core is explained based on modifications in the local environment of individual Cr atoms. The resultant competition between ferromagnetic and antiferromagnetic ordering gives rise to a wide assortment of interesting phenomena, such as a cluster-glass ground state at very low temperatures and an increase in Curie temperature values. We emphasize the importance of obtaining the commonly elusive magnetic nanophase diagram for M-Cr (M=Fe, Co, and Ni) nanoalloys, and we propose an efficient single-parameter method of tuning the Curie temperature for various technological applications.