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Schmidt, M. ; Hakkim, H. ; Anders, L. ; Kalamašņikovs, A. ; Kröger-Badge, T. ; Irsig, R.* ; Graf, N.* ; Kelnberger, R.* ; Passig, J. ; Zimmermann, R.

A solid-state infrared laser for two-step desorption–ionization processes in single-particle mass spectrometry.

Atmos. Meas. Tech. 18, 2425-2437 (2025)

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Recent advancements in single-particle mass spectrometry (SPMS) have enabled the detection of aromatic hydrocarbons at the individual particle level in conjunction with inorganic/refractory particle components. However, the laser desorption (LD) of organic material from particles prior to their ionization in a two-step process necessitates pulsed infrared lasers with adequate pulse energy that can be irregularly triggered on detected particles. Pulsed CO2 lasers with a 10.6 µm wavelength have been traditionally utilized, yet these lasers are bulky and costly and require regular maintenance, including gas exchange or a continuous laser gas supply. In this study, we present the application of a prototype solid-state laser based on an erbium-doped yttrium aluminum garnet (Er:YAG) crystal, emitting long pulses of 200 µs at 3 µm wavelength as a compact, cost-effective, and user-friendly alternative for LD. We directly compared the new laser with a commonly used CO2 laser and found similar performance in LD for both laboratory particles and ambient air experiments. With the exception of slightly increased fragmentation observed with the CO2 laser due to its beam profile, no qualitative differences were noted in the resulting mass spectra. Additionally, we compared a novel two-step ionization (LD-REMPI–LDI) with the conventional single-step LDI regarding the potential to detect polycyclic aromatic hydrocarbons (PAHs) and inorganics in laboratory and field experiments. The combined methods demonstrated superior performance in the detection of PAHs, for both the CO2 and the new Er:YAG laser. In addition to its higher sensitivity and lower fragmentation for PAHs when compared to single-step LDI, it is less dependent on the particle matrix, sharing the benefits of traditional two-step methods but extending its capability to combine PAH measurements with the LDI-based detection of inorganic particle compounds.

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