Tuning atomic-scale mixing of nanoparticles produced by atmospheric-pressure spark ablation.

Nanoparticles (NPs) mixed at the atomic scale have been synthesized by atmospheric-pressure spark ablation using pairs of Pd and Hf electrodes. Gravimetric analysis of the electrodes showed that the fraction of each material in the resulting mixed NPs can be varied from ca. 15-85 at% to 85-15 at% by employing different combinations of electrode polarities and thicknesses. These results were also qualitatively corroborated by microscopy and elemental analysis of the produced NPs. When using pairs of electrodes having the same diameter, the material from the one at negative polarity was represented at a substantially higher fraction in the mixed NPs regardless of whether a pair of thin or thick electrodes were employed. This can be attributed to the higher ablation rate of the electrodes at the negative polarity, as already known from earlier experiments. When using electrodes of different diameters, the fraction of the element from the thinner electrode was always higher. This is because thinner electrodes are ablated more effectively due to, at least in part, the increased importance of the associated heat losses compared to its thicker counterpart. In those cases, the polarity of the electrodes had a significantly smaller effect. Overall, our results demonstrate, for the first time, that spark ablation can be used to control atomic scale mixing and thus produce alloyed NPs with compositions that can be tuned to a good extent by simply using different combinations of electrode diameters and polarities. This expands the capabilities of the technique for producing mixed nanoparticle building blocks of well-defined composition that are highly desired for a wide range of applications.

Compositional tuning of gas-phase synthesized Pd-Cu nanoparticles.

Bimetallic nanoparticles have gained significant attention in catalysis as potential alternatives to expensive catalysts based on noble metals. In this study, we investigate the compositional tuning of Pd-Cu bimetallic nanoparticles using a physical synthesis method called spark ablation. By utilizing pure and alloyed electrodes in different configurations, we demonstrate the ability to tailor the chemical composition of nanoparticles within the range of approximately 80 : 20 at% to 40 : 60 at% (Pd : Cu), measured using X-ray fluorescence (XRF) and transmission electron microscopy energy dispersive X-ray spectroscopy (TEM-EDXS). Time-resolved XRF measurements revealed a shift in composition throughout the ablation process, potentially influenced by material transfer between electrodes. Powder X-ray diffraction confirmed the predominantly fcc phase of the nanoparticles while high-resolution TEM and scanning TEM-EDXS confirmed the mixing of Pd and Cu within individual nanoparticles. X-ray photoelectron and absorption spectroscopy were used to analyze the outermost atomic layers of the nanoparticles, which is highly important for catalytic applications. Such comprehensive analyses offer insights into the formation and structure of bimetallic nanoparticles and pave the way for the development of efficient and affordable catalysts for various applications.

Template-free generation and integration of functional 1D magnetic nanostructures.

The direct integration of 1D magnetic nanostructures into electronic circuits is crucial for realizing their great potential as components in magnetic storage, logical devices, and spintronic applications. Here, we present a novel template-free technique for producing magnetic nanochains and nanowires using directed self-assembly of gas-phase-generated metallic nanoparticles. The 1D nanostructures can be self-assembled along most substrate surfaces and can be freely suspended over micrometer distances, allowing for direct incorporation into different device architectures. The latter is demonstrated by a one-step integration of nanochains onto a pre-patterned Si chip and the fabrication of devices exhibiting magnetoresistance. Moreover, fusing the nanochains into nanowires by post-annealing significantly enhances the magnetic properties, with a 35% increase in the coercivity. Using magnetometry, X-ray microscopy, and micromagnetic simulations, we demonstrate how variations in the orientation of the magnetocrystalline anisotropy and the presence of larger multi-domain particles along the nanochains play a key role in the domain formation and magnetization reversal. Furthermore, it is shown that the increased coercivity in the nanowires can be attributed to the formation of a uniform magnetocrystalline anisotropy along the wires and the onset of exchange interactions.

Mo3Ni2N Nanoparticle Generation by Spark Discharge.

Spark ablation is an advantageous method for the generation of metallic nanoparticles with defined particle sizes and compositions. The reaction of the metal particles with the carrier gas during the synthesis and, therefore, the incorporation of those light elements into structural voids or even compound formation was confirmed for hydrides and oxides but has only been suspected to occur for nitrides. In this study, dispersed nanoparticles of Mo3Ni2N and Mo with Janus morphology, and defined particle sizes were obtained by spark discharge generation as a result of carrier gas ionization and characterized using transmission electron microscopy and powder X-ray diffraction. Metal nitrides possess beneficial catalytic and thermoelectric properties, as well as high hardness and wear resistance. Therefore, this method offers the possibility of controlled synthesis of materials which are interesting for numerous applications.