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Schmidt, M. ; Irsig, R.* ; Duca, D. ; Peltz, C.* ; Passig, J. ; Zimmermann, R.

Laser-pulse-length effects in ultrafast laser desorption.

Anal. Chem. 95, 18776-18782 (2023)
Publ. Version/Full Text DOI PMC
Open Access Gold (Paid Option)
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Shortening the laser pulse length opens up new opportunities for laser desorption (LD) of molecules, with benefits for mass spectrometry (MS) sampling and ionization. The capability to ablate any material without the need for an absorbing matrix and the decrease of thermal damage and molecular fragmentation has promoted various applications with very different parameters and postionization techniques. However, the key issues of the optimum laser pulse length and intensity to achieve efficient and gentle desorption of molecules for postionization in MS are not resolved, although these parameters determine the costs and complexity of the required laser system. Here, we address this research gap with a systematic study on the effect of the pulse length on the LD of molecules. Keeping all other optical and ionization parameters constant, we directly compared the pulses in the femtosecond, picosecond, and nanosecond range with respect to LD-induced fragmentation and desorption efficiency. To represent real-world applications, we investigated the LD of over-the-counter medicaments naproxen and ibuprofen directly from tablets as well as the LD of retene and ship emission aerosols from a quartz filter. With our study design, we excluded interfering effects on fragmentation and LD efficiency from, for example, collisional cooling or postionization by performing the experiments in vacuum with resonance-enhanced multiphoton ionization as the postionization technique. Regarding LD-induced fragmentation, we already found benefits for the picosecond pulses. However, the efficiency of LD was found to continuously increase with decreasing pulse length, pointing to the application potential of ultrashort pulses in trace analytics. Because many interfering effects beyond the LD pulse length could be excluded in the experiment, our results may be directly transferable to the LD applied in other techniques.
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Publication type Article: Journal article
Document type Scientific Article
Corresponding Author
Keywords Mass-spectrometry; Internal Energy; Icp-ms; Femtosecond; Ablation; Vaporization; Ionization; Matrix; Nanosecond; Identification
ISSN (print) / ISBN 0003-2700
e-ISSN 1520-6882
Journal Analytical Chemistry
Quellenangaben Volume: 95, Issue: 51, Pages: 18776-18782 Article Number: , Supplement: ,
Publisher American Chemical Society (ACS)
Publishing Place 1155 16th St, Nw, Washington, Dc 20036 Usa
Non-patent literature Publications
Reviewing status Peer reviewed
Institute(s) Cooperation Group Comprehensive Molecular Analytics (CMA)
Grants German Federal Ministry for Economic Affairs and Climate Action
Deutsche Forschungsgemeinschaft
Helmholtz Association (International Laboratory)
Light-Matter Interactions at Interfaces"
Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
, Deutsche Forschungsgemeinschaft