The advanced materials process by non-thermal plasmas with a high plasma density allows the synthesis of small-to-big sized Si quantum dots by combining low-temperature deposition with superior crystalline quality in the background of an amorphous hydrogenated silicon nitride matrix. Here, we make quantum dot thin films in a reactive mixture of ammonia/silane/hydrogen utilizing dual-frequency capacitively coupled plasmas with high atomic hydrogen and nitrogen radical densities. Systematic data analysis using different film and plasma characterization tools reveals that the quantum dots with different sizes exhibit size dependent film properties, which are sensitively dependent on plasma characteristics. These films exhibit intense photoluminescence in the visible range with violet to orange colors and with narrow to broad widths (∼0.3-0.9 eV). The observed luminescence behavior can come from the quantum confinement effect, quasi-direct band-to-band recombination, and variation of atomic hydrogen and nitrogen radicals in the film growth network. The high luminescence yields in the visible range of the spectrum and size-tunable low-temperature synthesis with plasma and radical control make these quantum dot films good candidates for light emitting applications.

Control of the plasma densities and energies of the principal plasma species is crucial to induce modification of the plasma reactivity, chemistry, and film properties. This work presents a systematic and integrated approach to the low-temperature deposition of hydrogenated amorphous silicon nitride films looking into optimization and control of the plasma processes. Radiofrequency (RF) and ultrahigh frequency (UHF) power are combined to enhance significantly the nitrogen plasma and atomic-radical density to enforce their effect on film properties. This study presents an extensive investigation of the influence of combining radiofrequency (RF) and ultrahigh frequency (UHF) power as a power ratio (PR = RF : UHF), ranging from 4 : 0 to 0 : 4, on the compositional, structural, and optical properties of the synthesized films. The data reveal that DF power with a characteristic bi-Maxwellian electron energy distribution function (EEDF) is effectively useful for enhancing the ionization and dissociation of neutrals, which in turn helps in enabling high rate deposition with better film properties than that of SF operations. Utilizing DF PECVD, a wide-bandgap of ∼3.5 eV with strong photoluminescence features can be achieved only by using a high-density plasma and high nitrogen atom density at room temperature. The present work also proposes the suitability of the DF PECVD approach for industrial applications.

The characterization of plasma and atomic radical parameters along with the energy influx from plasma to the substrate during plasma enhanced chemical vapor deposition (PECVD) of Si quantum dot (QD) films is presented and discussed. In particular, relating to the Si QD process optimization and control of film growth, the necessity to control the deposition environment by inducing the effect of the energy of the key plasma species is realized. In this contribution, we report dual frequency PECVD processes for the low-temperature and high-rate deposition of Si QDs by chemistry and energy control of the key plasma species. The dual frequency plasmas can effectively produce a very high plasma density and atomic H and N densities, which are found to be crucial for the growth and nucleation of QDs. Apart from the study of plasma chemistry, the crucial role of the energy imparted due to these plasma activated species on the substrate is determined in light of QD formation. Various plasma diagnostics and film analysis methods are integrated to correlate the effect of plasma and energy flux on the properties of the deposited films prepared in the reactive mixtures of SiH/NH at various pressures. The present results are highly relevant to the development of the next-generation plasma process for devices that rely on effective control of the QD size and film properties.