Abstract
Pulsed laser ablation of molecular solids is important for identification and quantification in (bio-)organic mass spectrometry, for example using matrix-assisted laser desorption/ionization (MALDI). Recently, there has been a major shift to using MALDI and related laser ablation/post-ionization methods at atmospheric pressure. However, the underlying laser ablation processes, in particular early plume formation and expansion, are still poorly understood. Here, we present a study of the early ablation processes on the ns-time scale in atmospheric pressure UV-laser ablation of anthracene as well as of different common MALDI matrices such as 2,5-dihydroxybenzoic acid (2,5-DHB), α-cyano-4-hydroxycinnamic acid and sinapinic acid. Material release as well as the formation and expansion of hemi-spherical shock waves were studied by shadowgraphy with high temporal resolution (∼5 ns). The applicability of the classical Taylor-Sedov model for expansion of strong shock waves (“point-blast model”), as well as the drag force model, were evaluated to mathematically describe the observed shock wave propagation. The time- and energy-dependent expansion of the shock waves could be described using a Taylor-Sedov scaling law of the form R ∝ tq, when a q-exponent of ∼0.5 instead of the theoretical value of q = 0.4 was found, indicating a faster expansion than expected. The deviations from the ideal value of q were attributed to the non-negligible influence of ambient pressure, a weak versus strong shock regime, and additional acceleration processes present in laser ablation that surpass the limit of the point-blast model. The onset of shock wave formation at a fluence of ∼15–30 mJ/cm2 for the compounds investigated coincides with the onset of bulk material release, whereas, pure desorption below this fluence threshold did not lead to features visible in shadowgraphy.
Published Version
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