Multibubble Sonochemistry and Sonoluminescence at 100 kHz: The Missing Link between Low- and High-Frequency...

Ultrasonic frequency is one of the most important parameters that decides the characteristics of acoustic cavitation. Low- (16-50 kHz) and high- (≥200 kHz) frequency ultrasounds present opposite physical and chemical behaviors and have been extensively studied, yet frequencies in between are poorly characterized. In this study, acoustic cavitation at the intermediate ultrasonic frequency of 100 kHz is compared with that at 20 kHz and at 362 kHz by different experimental investigations: sonochemical yield (H₂O₂), images of sonochemiluminescence and sonoluminescence, as well as sonoluminescence spectra in aqueous media saturated with Ar or Ar/(20 vol %)O₂. The chemical activity (H₂O₂ yield) of cavitation bubbles at 100 kHz presents a transitional behavior between low and high frequencies. The active cavitation zone distributes in the whole sonicated volume, similarly to high-frequency ultrasound and much further than at 20 kHz. The spectral shape of 100 kHz spectra is similar to that at 20 kHz. On the contrary, 100 kHz ultrasound provides the dissociation of O₂ and N₂ molecules inside the bubble, which is more typical for high-frequency ultrasound. This faculty is explained by the more extreme conditions reached at collapse compared with 20 kHz. Rovibronic temperatures of OH (A²Σ⁺) excited radicals derived from spectroscopic simulations confirm this interpretation.