A polarization-sensitive laser-light-scattering method is developed for simultaneous in situ measurements of properties (size, size dispersion, density, and refractive index) of particulates formed in processing plasmas. The developed system is applied to observe the growth processes of particulates in a range of their size larger than about 10 nm in rf silane plasmas. A size, a size dispersion (logarithm of a standard deviation of size), a density, and a refractive index of particulates in the plasmas are found to be 10–200 nm, about 0.1, 107–109 cm−3 and about 3–5i, respectively. The former three of such values agree fairly well with ones deduced from scanning electron microscopic (SEM) observation. These particulates grow through three phases of nucleation and initial growth, rapid growth, and growth saturation. Coexistence of two size groups of particulates with narrow size dispersions during and after the rapid growth phase verified by the SEM observation may be explained by a model taking into account coagulation between oppositely charged particulates.
Growth processes of particles in high frequency silane plasmas are studied as a parameter of discharge frequency (3.5–28 MHz) or by modulating the amplitude of discharge voltage (125–275 V). Except for the 28 MHz case, particles tend to grow through three phases of nucleation and subsequent initial growth, rapid growth, and growth saturation. A detailed study for 6.5 MHz explains the following features: morphology of particles shows that coagulation of particles plays a crucial role in the rapid growth phase; a coagulation rate of 200 s−1 observed in the rapid growth phase is extremely high compared to a thermal collision rate of 5 s−1 between particles; coagulation almost stops when decreasing the discharge power by about one-fourth at the middle of the rapid growth phase; two size groups of particles with narrow size dispersions coexist during and after the rapid growth phase. For 28 MHz, while, as compared to 6.5 MHz, particles appear early after the initiation of discharge and their density is high by about two orders, their growth rate in the subsequent phase is quite low. To properly explain most rapid growth features, a model, taking into account coagulation between oppositely charged particles, is proposed.
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