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Low-temperature plasma-processing technologies are essential for material synthesis and device fabrication. Not only the utilization but also the development of plasma-related products and services requires an understanding of the multiscale hierarchies of complex behaviors of plasma-related phenomena, including plasma generation in physics and chemistry, transport of energy and mass through the sheath region, and morphology- and geometry-dependent surface reactions. Low-temperature plasma science and technology play a pivotal role in the exploration of new applications and in the development and control of plasma-processing methods. Presently, science-based and data-driven approaches to control systems are progressing with the state-of-the-art deep learning, machine learning, and artificial intelligence. In this review, researchers in material science and plasma processing, review and discuss the requirements and challenges of research and development in these fields. In particular, the prediction of plasma parameters and the discovery of processing recipes are asserted by outlining the emerging science-based, data-driven approaches, which are called plasma informatics.

Low-temperature plasma plays various roles in industrial material processing as well as provides a number of scientific targets, both from theoretical and experimental points of view. Such rich features in variety are based on its complexities, arising from diverse parameters in constituent gas-phase species, working gas pressure, input energy density, and spatial boundaries. When we consider causalities in these complexities, direct application of machine-learning methods is not always possible since levels of complexities are so high in comparison with other scientific research targets. To overcome this difficulty, progresses in plasma diagnostics and data acquisition systems are inevitable, and the handling of a large number of data elements is one of the key issues for this purpose. In this topical review, we summarize previous and current achievements of visualization, acquisition, and analysis methods for complex plasma datasets which may open a scientific and technological category mixed with rapid machine-learning advancements and their relevant outcomes. Although these research trends are ongoing, many reports published so far have already convinced us of various expanding aspects of low-temperature plasma leading to the potential for scientific progress as well as developments of intellectual design in industrial plasma processes.

Reactions for dissociative ionization and neutral dissociation collisions between an electron and a tetraethoxysilane [Si(OC2H5)4, TEOS] molecule are reported, and neutral dissociation cross sections are calculated by applying the classical Rice–Ramsperger–Kassel theory. Detailed electron collision cross section set of TEOS vapor, including 18 neutral dissociation cross sections and 20 ionization cross sections, is constructed. Electron transport coefficients, such as the mean-arrival-time drift velocity, bulk drift velocity, longitudinal bulk diffusion coefficient, and ionization coefficient, and rate coefficients for both elastic and inelastic collisions in TEOS vapor are calculated from the present cross section set using a Monte Carlo method. The validity of the present cross section set is demonstrated by comparing the calculated electron transport coefficients with measured data. Furthermore, fragmentation of TEOS molecules by electron impact is simulated, and then the number of fragments produced in the simulation is compared with the measured mass spectra.

Plasma enhanced chemical vapor deposition (PECVD) of silicon oxide (SiO2) using tetraethoxysilane (TEOS) was investigated theoretically by developing an unprecedented plasma chemistry model in TEOS/O2/Ar/He gas mixture. In the gas phase reactions, a TEOS molecule is decomposed by the electron impact reaction and/or chemically oxidative reaction, forming intermediate TEOS fragments, i.e., silicon complexes. In this study, we assume that SiO is the main precursor that contributes to SiO2 film growth under a particular process or simulation condition. The surface reaction was also investigated using quantum mechanical simulations with density functional theory. Based on the gas and surface reaction models, we constructed a computational plasma model for SiO2 film deposition in a PECVD process. The simulation results using CHEMKIN pro and CFD-ACE + have shown that the neutral atomic O and SiO as well as the charged O2 + are the dominant species to obtain a high deposition rate and uniformity. The spatial distributions of various species in the TEOS/O2/Ar/He gas mixture plasma were shown in the study. The uniformity of deposited film due to the change in the plasma bulk property was also discussed.

The concentration variations of reactive oxygen/nitrogen species in water, such as H2O2, NO2−, and NO3−generated by pulsed-discharge plasma exposure, are calculated using reaction rates of chemical reactions and acid-base equilibrium in water. The calculated concentrations and pH values are in good agreement with measured data within the range where the significant changes of the measured data are observed. The rate constant for ONOOH generation is estimated to be 7.8×103M−2s−1, and this value is in good agreement with previously reported values. The generation rates of H2O2, NO2−, and NO3−are estimated to be 7.70×10−7, 4.10×10−7, and 1.10×10−7M s−1, respectively.

A reliable set of electron collision cross sections for water vapor, including elastic, rotational, vibrational, and electronic excitation, electron attachment, and ionization cross sections, is estimated by the electron swarm method. In addition, anisotropic electron scattering for elastic and rotational excitation collisions is considered in the cross section set. Electron transport coefficients such as electron drift velocity, longitudinal diffusion coefficient, and effective ionization coefficient are calculated from the cross section set by Monte Carlo simulation in a wide range of E/N values, where E and N are the applied electric field and the number density of H2O molecules, respectively. The calculated transport coefficients are in good agreement with those measured. The obtained results confirm that the anisotropic electron scattering is important for the calculation at low E/N values. Furthermore, the cross section set assuming the isotropic electron scattering is proposed for practical use.

A set of electron collision cross sections for trifluoromethane (CHF3) is estimated by the electron swarm method. Electron transport coefficients in CHF3, such as the electron drift velocity, longitudinal diffusion coefficient, and effective ionisation coefficient, are calculated from the estimated cross section set by the Monte Carlo method, and the values are compared with the measured data. In the case of the transport coefficients, good agreement is obtained between the calculated and measured values in a wide range of reduced electric fields. Furthermore, the transport coefficients described above and the characteristic energy in CHF3–Ar mixtures are calculated, and the values are found to agree well with the measured data. This confirms the validity of the cross section set for CHF3 estimated here.

Metastable crystals are often found in the recovery process of vacuum co-deposited alloy films. In order to explore this possibility in the Mn-Al system, the films with various compositions were prepared and investigated in a hot stage of an electron microscope. Change of their electric resistance was also measured. The films with 100–35 at.%Mn showed only grain growth of the crystals which were found at the corresponding compositions in the equilibrium phase diagram. The films with 30–25 at.%Mn showed discrete nucleation of leaf-formed crystals which were not found in the phase diagram. Further raising up of the temperature gave a transformation of the crystals into the one-dimensionally disordered δ(Mn-Al) phase, which also did not exist in the phase diagram. The films with 15–8 at.%Mn showed discrete nucleation of circular crystals, which were mainly identified as MnAl6. Resistance of the last films showed anomalous oscillation which started just before the nucleation.