Spectroscopy of Sonoluminescence and Sonochemistry
in Water Saturated with N<sub>2</sub>–Ar Mixtures
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Abstract
Sonoluminescence
spectra in relation with sonochemical activity
of water sparged with Ar/N<sub>2</sub> gas mixtures were systematically
studied at two ultrasonic frequencies (20 and 359 kHz). At 20 kHz,
solely the molecular emission of OH (A<sup>2</sup>Σ<sup>+</sup>–X<sup>2</sup>Π<sub>i</sub>) 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<sup>3</sup>Π–X<sup>3</sup>Σ<sup>–</sup>) system. In addition, the sonolysis
of a 0.2 M NH<sub>3</sub>·H<sub>2</sub>O solution at 359 kHz
in the presence of pure Ar yields the emission bands of NH (A<sup>3</sup>Π – X<sup>3</sup>Σ<sup>–</sup>)
(336 nm) and NH (C<sup>1</sup>Π–A<sup>1</sup>Δ)
(322 nm) systems confirming the sonochemical production of NH radicals.
The N<sub>2</sub> (C<sup>3</sup>Π<sub>u</sub>–B<sup>3</sup>Π<sub>g</sub>) emission band is absent at both frequencies.
This uncommon phenomenon can be explained by the quenching of the
N<sub>2</sub> (C<sup>3</sup>Π<sub>u</sub>) excited state with
water molecules inside the bubbles. The sonoluminescence of NH radicals
at 359 kHz indicates more effective intrabubble dissociation of N<sub>2</sub> 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 (H<sub>2</sub>, H<sub>2</sub>O<sub>2</sub>, HNO<sub>3</sub>, HNO<sub>2</sub>) confirmed
the more drastic conditions produced during bubble collapse at higher
ultrasonic frequency