Sonoluminescence spectra in relation with sonochemical activity of water sparged with Ar/N2 gas mixtures were systematically studied at two ultrasonic frequencies (20 and 359 kHz). At 20 kHz, solely the molecular emission of OH (A(2)Σ(+)-X(2)Πi) is observed in addition to a broad continuum typical for multibubble sonoluminescence. On the contrary, at high frequency a second emission band is present around 336 nm which is assigned to the NH (A(3)Π-X(3)Σ(-)) system. In addition, the sonolysis of a 0.2 M NH3·H2O solution at 359 kHz in the presence of pure Ar yields the emission bands of NH (A(3)Π - X(3)Σ(-)) (336 nm) and NH (C(1)Π-A(1)Δ) (322 nm) systems confirming the sonochemical production of NH radicals. The N2 (C(3)Πu-B(3)Πg) emission band is absent at both frequencies. This uncommon phenomenon can be explained by the quenching of the N2 (C(3)Πu) excited state with water molecules inside the bubbles. The sonoluminescence of NH radicals at 359 kHz indicates more effective intrabubble dissociation of N2 molecules at high ultrasonic frequency compared to low-frequency (20 kHz) ultrasound. Its absence at 20 kHz may also be related to strong quenching, e.g., by water molecules. The kinetic study of the formation of principal sonochemical products (H2, H2O2, HNO3, HNO2) confirmed the more drastic conditions produced during bubble collapse at higher ultrasonic frequency.
In this work, the sonoluminescence of NH radicals has been evaluated as a new spectroscopic probe for the nonequilibrium plasma produced by multibubble cavitation in liquids. The experiments were performed in aqueous ammonia solutions subjected to power ultrasound at low and high frequencies and under two different rare gases (Ar and Xe). Sonoluminescence (SL) spectroscopy focuses on the emission of the two present systems: NH (AΠ-XΣ) and OH (AΣ-XΠ). Both spectroscopic systems indicate the absence of thermal equilibrium during bubble collapse (T > T) irrespective of the saturating gas. When Ar is used as the saturating gas, these emissions can be fitted using Specair software and the corresponding rovibronic temperatures are derived. Both species indicate a net increase in vibrational temperatures with the US frequency. In Xe, the SL spectra exhibit OH (CΣ-AΣ) and NH (cΠ-aΔ) emission bands indicating a higher electron temperature compared to Ar. However, in Xe, the SL spectra cannot be satisfactorily fitted because of significant line broadening. The estimation of the intrabubble pressure via SL simulation using Specair software is discussed. Monitoring of the sonochemical activity indicates the formation of H and NH, while no HO accumulates under these conditions. In the presence of Xe, NO is also formed as a sonolysis product. The appearance of new possible reaction pathways under Xe is made possible by the higher plasma electron density and correlates with SL data.
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