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A commercially available airbrush gun as a new source for spray ionization is presented. It is best operated employing moderate stagnation pressures, resulting in a sonic gas flow. A mass spectrometric investigation on the amino acid lysine and several peptides reveals that this inexpensive approach results in reproducible mass spectra. The ion patterns strongly resemble the results from other studies obtained with custom made sonic spray vaporizers. The patterns as well resemble the mass spectra recorded with electrospray devices. For a better understanding of the vaporization process, the mass spectrometry experiments are accompanied by laser induced fluorescence experiments. Inverse Abel transform of the obtained fluorescence maps allows the determination of the full 3D distribution of the spray cone. Furthermore, via exploitation of the solvatochromism of the used dye the solvation state distribution can be visualized. In addition, expansion parameters like droplet size and velocity are obtained by laser stroboscopy. The experiments demonstrate that the analyte is hardly desolvated throughout the expansion. This indicates a subsequent vaporization of the residual solvent in the intermediate pressure region of the mass spectrometer.
Raman spectroscopy is becoming a commonly used, powerful tool for structural elucidation and species identification of small liquid samples, e.g. in droplet-based digital microfluidic devices. Due to the low scattering cross sections and the temporal restrictions dictated by the droplet flow, however, it depends on amplification strategies which often come at a cost. In the case of surface-enhanced Raman scattering (SERS), this can be an enhanced susceptibility towards memory effects and cross talk, whereas resonant and/or stimulated Raman techniques require higher instrumental sophistication, such as tunable lasers or the high electromagnetic field strengths which are typically provided by femtosecond lasers. Here, an alternative instrumental approach is discussed, in which stimulated Raman scattering (SRS) is achieved using the single fixed wavelength output of an inexpensive diode-pumped solid-state (DPSS) nanosecond laser. The required field strengths are realized by an effective light trapping in a resonator mode inside the interrogated droplets, while the resonant light required for the stimulation is provided by the fluorescence signal of an admixed laser dye. To elucidate the underlying optical processes, proof-of-concept experiments are conducted on acoustically levitated droplets, mimicking a highly reproducible and stable digital fluidic system. By using isotope-labeled compounds, the assignment of the emitted radiation as Raman scattering is firmly corroborated. A direct comparison reveals an amplification of the usually weak spontaneous Stokes emission by up to five orders of magnitude. Further investigation of the optical power dependence reveals the resulting gain to depend on the intensity of both, the input laser fluence and the concentration of the admixed fluorophore, leaving SRS as the only feasible amplification mechanism. While in this study stable large droplets have been studied, the underlying principles also hold true for smaller droplets, in which case significantly lower laser pulse energy is required. Since DPSS lasers are readily available with high repetition rates, the presented detection strategy bears a huge potential for fast online identification and characterization routines in digital microfluidic devices.
Coulomb fission of charged droplets (The terms drop and droplet are often used synonymous. Throughout this manuscript, to avoid confusion, the terms drop and droplet will be used for liquid spheres with radii in the millimeter range and the micrometer range, respectively. In our experiments, the first correspond to the parent drop while the latter describes the ejected progeny droplets.) is a wellstudied natural phenomenon. Controlled droplet fission is already successfully employed in several technological applications. Still, since the occurring surface rupture relies on the exact understanding and description of the liquid gas boundary, some details are still under debate. Most empirical systematic studies observe falling micrometer droplets passing through the electric field inside a plate capacitor. This approach, although easily applicable and reliable, limits the experimental degrees of freedom regarding the observable time and the maximum size of the drops and can only be performed in consecutive individual observations of different subsequent drops. Here we present a novel setup to study the field induced breakup of acoustically levitated drops. The design does not bear any restrictions towards the temporal window of observation, and allows handling of drops of a tunable radius ranging from 10 µm to several millimeters and a real-time monitoring of one single drop. Our comprehensive study includes a time resolved visual inspection, laser shadowgraphy, laser induced fluorescence imaging, and ambient mass spectrometric interrogation of the nascent Taylor cone. The results shown for a millimeter sized drop, previously inaccessible for Coulomb fission experiments, are mostly comparable with previous results for smaller drops. The major difference is the time scale and the threshold potential of the drop rupture. Both values, however, resemble theoretically extrapolations to the larger radius. The technique allows for a systematic study of breakup behavior of drops of different charge, material, and size.