van der Waals (vdW) magnets are receiving ever-growing attention nowadays due to their significance in both fundamental research on low-dimensional magnetism and potential applications in spintronic devices. The high crystalline quality of vdW magnets is the key to maintaining intrinsic magnetic and electronic properties, especially when exfoliated down to the two-dimensional limit. Here, ultrahigh-quality air-stable vdW CrSBr crystals are synthesized using the direct solid–vapor synthesis method. The high single crystallinity and spatial homogeneity have been thoroughly evidenced at length scales from submm to atomic resolution by X-ray diffraction, second harmonic generation, and scanning transmission electron microscopy. More importantly, specific heat measurements of ultrahigh-quality CrSBr crystals show three thermodynamic anomalies at 185, 156, and 132 K, revealing a stage-by-stage development of the magnetic order upon cooling, which is also corroborated with the magnetization and transport results. Our ultrahigh-quality CrSBr can further be exfoliated down to monolayers and bilayers easily, providing the building blocks of heterostructures for spintronic and magneto-optoelectronic applications.

Correlations between physical properties linking film quality with wet etch rate (WER), one of the leading figures of merit, in plasma-enhanced atomic layer deposition (PEALD) grown silicon nitride (SiN x ) films remain largely unresearched. Achieving a low WER of a SiN x film is especially significant in its use as an etch stopper for technology beyond 7 nm node semiconductor processing. Herein, we explore the correlation between the hydrogen concentration, hydrogen bonding states, bulk film density, residual impurity concentration, and the WERs of PEALD SiN x using Fourier transform infrared spectrometry, X-ray reflectivity, and spectroscopic ellipsometry, etc. PEALD SiN x films for this study were deposited using hexachlorodisilane and hollow cathode plasma source under a range of process temperatures (270–360 °C) and plasma gas compositions (N2/NH3 or Ar/NH3) to understand the influence of hydrogen concentration, hydrogen bonding states, bulk film density, and residual impurity concentration on the WER. Varying hydrogen concentration and differences in the hydrogen bonding states resulted in different bulk film densities and, accordingly, a variation in WER. We observe a linear relationship between hydrogen bonding concentration and WER as well as a reciprocal relationship between bulk film density and WER. Analogous to the PECVD SiN x processes, a reduction in hydrogen bonding concentration arises from either (1) thermal activation or (2) plasma excited species. However, unlike the case with silane (SiH4)-based PECVD SiN x , PEALD SiN x WERs are affected by residual impurities of Si precursors (i.e., chlorine impurity). Thus, possible wet etching mechanisms in HF in which the WER is affected by hydrogen bonding states or residual impurities are proposed. The shifts of amine basicity in SiN x due to different hydrogen bonding states and the changes in Si electrophilicity due to Cl impurity content are suggested as the main mechanisms that influence WER in the PEALD processes.

In this work, effects of NH3/N2 and N2-H2/Ar plasma gases for the growth of PEALD SiNx films using pentachlorodisilane (PCDS, HSi2Cl5) were studied using a hollow cathode PEALD system. At identical process conditions, the combination of PCDS and N2−H2/Ar plasma showed a relatively lower (approximately < 10 %) growth rate as compared to NH3/N2 plasma under a range of process temperatures (240−300 °C) whereas the wet etch resistance to HF acid was improved (> 1.6 nm/min, 500:1 HF). Using XPS and FTIR analysis, it was identified that N2−H2/Ar gas mixture results in a Si-rich SiNx film with less N−Hx bonds when compared to NH3/N2 mixture, thereby resulting in a decreased wet etch rate.

Aluminum nitride (AlN) thin films were grown using thermal atomic layer deposition in the temperature range of 175–350 °C. The thin films were deposited using trimethyl aluminum (TMA) and hydrazine (N2H4) as a metal precursor and nitrogen source, respectively. Highly reactive N2H4, compared to its conventionally used counterpart, ammonia (NH3), provides a higher growth per cycle (GPC), which is approximately 2.3 times higher at a deposition temperature of 300 °C and, also exhibits a low impurity concentration in as-deposited films. Low temperature AlN films deposited at 225 °C with a capping layer had an Al to N composition ratio of 1:1.1, a close to ideal composition ratio, with a low oxygen content (7.5%) while exhibiting a GPC of 0.16 nm/cycle. We suggest that N2H4 as a replacement for NH3 is a good alternative due to its stringent thermal budget.

Cleaning of copper surfaces is required to remove undesired surface oxidation during the interconnect fabrication process. In this work, we examined the vapor-phase cleaning of Cu surfaces using anhydrous N2H4. Gas cluster ion beam (GCIB) depth profiling and elemental analysis using XPS shows that CuxO in the Cu sample, formed after exposure to air, can be effectively reduced to Cu0 at 200 °C. By monitoring the surface chemistry using in-situ reflectance absorption infrared spectroscopy (RAIRS), we found that atomic layer deposition (ALD)-like single exposure of N2H4 at 200 °C can remove the adventitious surface contamination and, most importantly, reduce the Cu2O to metallic Cu.