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Zsolt Czigány

Publications and source records attributed to Zsolt Czigány.

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Materials and Spin Characteristics of Nanodiamonds Partially Covered with Amino Groups and Embedded with Nitrogen-Vacancy Color Centers

Fluorescent nanodiamonds (FNDs) with optically read qubits hold great potential for detecting electric and magnetic fields, temperature, and other nanoscale physicochemical quantities relevant to chemistry and biology. Proper surface functionalization is essential for their application as probes, but surface modifications can impact qubit sensor properties. We systematically study nitrogen-vacancy (NV) color centers in FNDs as a function of size and surface termination. FNDs were produced from high-pressure, high-temperature diamonds, with NV centers introduced via electron irradiation and annealing. The initial oxygen-covered FNDs were homogenized with hydroxyl (-OH) groups as reference samples, while the noninvasive Hofmann degradation introduced amino (-NH2) groups for potential direct biomolecule attachment. Amino groups may not cover the nanodiamonds homogeneously, but we label them as -NH2 terminated throughout. We monitored charge state stability and the zero-field splitting parameters of the embedded NV centers. First, we resolve the size dependence of the NV(-) zero-field splitting parameters across the 10-140 nm range and show that the symmetry-breaking E parameter decreases monotonically from about 8 to about 5 MHz with increasing size while the axial D parameter is shifted only in the smallest (<= 30 nm) particles, thereby disentangling the static-strain and fluctuating electric-field contributions to the spin levels. Second, while NV charge state stabilization was observed in both -OH- and -NH2-terminated FNDs above a certain size, we demonstrate that a remarkably high and laser-power-independent NV(-) content (f_NV(-) of about 0.8) is achieved by wet-chemical Hofmann amino termination only in 140 nm particles, an effect we link through electron spin resonance to the degradation of surface paramagnetic defects rather than to the introduction of new ones.

quant-ph

Impact of O concentration on the thermal stability and decomposition mechanism of (Cr,Al)N compared to (Ti,Al)N thin films

The composition-dependent thermal stability of (Cr$_{0.47 \mp 0.03}$Al$_{0.53 \mp 0.03}$)$_{z}$(O$_{y}$N$_{1-y}$)$_{1-z}$ thin films with O concentrations of y = 0, 0.15, and 0.40 is investigated up to 1200 °C and then compared to (Ti$_{0.56}$Al$_{0.44}$)$_{z}$(O$_{y}$N$_{1-y}$)$_{1-z}$. X-ray diffraction reveals a thermal stability limit of 1150 °C independent of the O concentration, as witnessed by the formation of decomposition products, namely h-Cr$_{2}$N for (Cr$_{0.50}$Al$_{0.50}$)$_{0.49}$N$_{0.51}$ and c-Cr for both (Cr$_{0.48}$Al$_{0.52}$)$_{0.48}$(O$_{0.15}$N$_{0.85}$)$_{0.52}$ and (Cr$_{0.44}$Al$_{0.56}$)$_{0.46}$(O$_{0.40}$N$_{0.60}$)$_{0.54}$. Based on TEM and ERDA data, the thermal stability limit is extended to 1100 - 1150 °C. DFT calculations indicate that bond breaking limits the thermal stability. In (Cr,Al)N, N has the lowest activation energy for migration. Furthermore, the O vacancy formation energy is highest in (Cr,Al)(O,N). It has to be overcome to enable diffusion on the non-metal sublattice, which is necessary for forming decomposition products like w-AlN or c-Cr. However, once Cr-N bonds break, decomposition into h-Cr$_{2}$N and subsequent c-Cr together with N$_{2}$ is triggered. This results in N evaporation, generating sufficient non-metal vacancies that greatly enhance diffusion and render the extensive vacancy formation energies for non-metals irrelevant. This reduction of the activation energy for mass transport on the non-metal sublattice to the migration barrier causes the similar thermal stability in (Cr$_{0.47 \mp 0.03}$Al$_{0.53 \mp 0.03}$)$_{z}$(O$_{y}$N$_{1-y}$)$_{1-z}$. In contrast, Al bonds break first without creating non-metal vacancies in (Ti,Al)(O,N). Thus, the high O vacancy formation energy in (Ti,Al)(O,N) significantly increases the thermal stability compared to (Ti,Al)N as well as the here investigated films.

cond-mat.mtrl-sci

High- and medium-entropy nitride coatings from the Cr-Hf-Mo-Ta-W-N system: properties and high-temperature stability

High- and medium-entropy nitride coatings from the Cr-Hf-Mo-Ta-W-N system were studied using ab initio calculations and experiments to clarify the role of entropy and individual elements in phase stability, microstructure, and high-temperature behaviour. Formation energy calculations indicated that nitrogen vacancies stabilise the cubic (fcc) phase, with hafnium and tantalum acting as strong stabilisers, while tungsten destabilises the lattice. Coatings were deposited by reactive magnetron sputtering at approx. 50C (AT) and approx. 580C (HT). All exhibited columnar fcc structures; high-temperature deposition produced denser coatings, lower nitrogen content, and larger crystallites, resulting in higher hardness and elastic modulus. Thermal stability was tested up to 1200C on Si and oxidation at 1400C on sapphire. AT coatings failed early, while most HT coatings endured. Nitrogen loss less than 10 at.% at 1000C was critical for survival. TEM revealed tungsten segregation and HfO2 formation, while fcc nitride remained dominant. Ta enrichment proved essential for superior thermal and oxidation stability.

cond-mat.mtrl-sci

Thiolation and PEGylation of silicon carbide nanoparticle

In this study, we implement thiol termination on the surface of few-nanometer-sized silicon carbide (SiC) nanoparticles (NPs) to enable further applications, such as fluorescent biomarkers. Various spectroscopic techniques are employed to monitor the effectiveness of the surface treatment. A thiol-Michael addition reaction is performed by conjugating 4-arm PEGmaleimide molecules to the thiol groups of SiC NPs, further demonstrating the reactivity of thiol-terminated SiC NPs, which also acts as a protection layer against oxidation. These fluorescent thiolated SiC NPs, both with and without conjugated molecules, are directly applicable as bioinert probes. Since SiC NPs can potentially host room-temperature fluorescent defect quantum bits, our results are an important step to realize a bioinert, ultrasmall quantum sensor bioagents, which may open new avenues in biotechnology.

cond-mat.mtrl-sci

Characterization of Defect Structure in Electrodeposited Nanocrystalline Ni Films

The microstructure of electrodeposited Ni films produced without and with organic additives (saccharin and formic acid) was investigated by X-ray diffraction (XRD) line profile analysis and cross-sectional transmission electron microscopy (TEM). Whereas the general effect of these additives on the microstructure (elimination of columnar growth as well as grain refinement) was reproduced, the pronounced intention of this study was to compare the results of various seldom-used high-performance structural characterization methods on identical electrodeposited specimens in order to reveal fine details of structural changes qualitatively not very common in this field. In the film deposited without additives, a columnar structure was observed showing similarities to the T-zone of structure zone models. Both formic acid and saccharin additives resulted in equiaxed grains with reduced size, as well as increased dislocation and twin fault densities in the nanocrystalline films. Moreover, the structure became homogeneous and free of texture within the total film thickness due to the additives. Saccharin yielded smaller grain size and larger defect density than formic acid. A detailed analysis of the grain size and twin boundary spacing distributions was carried out with the complementary application of TEM and XRD, by carefully distinguishing between the TEM and XRD grain sizes.

cond-mat.mtrl-sci