A combination of time-resolved optical emission spectroscopy measurements and collisionalradiative modeling is used to investigate the phenomena occurring over multiple time scales in the frequency domain of a low-pressure, axially asymmetric, capacitively coupled radiofrequency (RF) argon plasma with pulsed injection of hexamethyldisiloxane (HMDSO, Si 2 O(CH 3) 6). The collisional-radiative model developed here considers the population of argon 1s and all ten 2p levels (in Paschen's notation). The presence of HMDSO in the plasma is accounted for in the model by quenching of the argon 1s states by species generated by plasma processing of HMDSO, including HMDSO-15 (Si 2 O(CH 3) 5), acetylene (C 2 H 2) and methane (CH 4). Detailed analysis of the relative populations of Ar 2p states reveals cyclic evolutions of the electron temperature, electron density and quenching frequency that are shown to be linked to the kinetics of dust formation in Ar/HMDSO plasmas. Penning ionization of HMDSO and its fragments is found to be an important source of electrons for the plasma maintenance. It is at the origin of the cyclic formation/disappearance of the dust cloud, without attenuation of the phenomenon, as long as the pulsed injection of HMDSO is sustained. The multi-scale approach used in this study further reveals the straightforward relation of the frequency of HMDSO pulsed injection, in particular the HMDSO duty cycle, with the frequency of dust formation/ disappearance cycle.
Laboratory experiments are essential in exploring the mechanisms involved in stardust formation. One key question is how a metal is incorporated into dust for an environment rich in elements involved in stardust formation (C, H, O, Si). To address experimentally this question we have used a radiofrequency cold plasma reactor in which cyclic organosilicon dust formation is observed. Metallic (silver) atoms were injected in the plasma during the dust nucleation phase to study their incorporation in the dust. The experiments show formation of silver nanoparticles (~15 nm) under conditions in which organosilicon dust of size 200 nm or less is grown. The presence of AgSiO bonds, revealed by infrared spectroscopy, suggests the presence of junctions between the metallic nanoparticles and the organosilicon dust. Even after annealing we could not conclude on the formation of silver silicates, emphasizing that most of silver is included in the metallic nanoparticles. The molecular analysis performed by laser mass spectrometry exhibits a complex chemistry leading to a variety of molecules including large hydrocarbons and organometallic species. In order to gain insights into the involved chemical molecular pathways, the reactivity of silver atoms/ions with acetylene was studied in a laser vaporization source. Key organometallic species, AgnC2Hm (n = 1–3; m = 0–2), were identified and their structures and energetic data computed using density functional theory. This allows us to propose that molecular Ag–C seeds promote the formation of Ag clusters but also catalyze hydrocarbon growth. Throughout the article, we show how the developed methodology can be used to characterize the incorporation of metal atoms both in the molecular and dust phases. The presence of silver species in the plasma was motivated by objectives finding their application in other research fields than astrochemistry. Still, the reported methodology is a demonstration laying down the ground for future studies on metals of astrophysical interest, such as iron.
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