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Detecting Laser-Volatilized Salts with a Miniature 100-GHz Spectrometer

DOI:10.1021/acs.jpca.9b10548 期刊:The Journal of Physical Chemistry A 出版年份:2020 更新时间:2025-09-23 15:19:57
摘要: Rotational transitions are unique identi?ers of molecular species, including isotopologues. This article describes the rotational detections of two laser-volatilized salts, NaCl and KCl, made with a miniature Fourier transform millimeter-wave (FTmmW) cavity spectrometer that could one day be used to measure solid composition in the ?eld or in space. The two salts are relevant targets for icy moons in the outer solar system, and in principle, other molecular solids could be analyzed with the FTmmW instrument. By coupling the spectrometer to a collisionally cooling laser ablation source, (a) we demonstrate that the FTmmW instrument is sensitive enough to detect ablation products, and (b) we use the small size of the FTmmW cavity to measure ablation product signal along the carrier gas beam. We ?nd that for 532 nm nanosecond pulses, ablated molecules are widely dispersed in the carrier-gas jet. In addition to the miniature spectrometer results, we present several complementary measurements intended to characterize the laser ablation process. For pulse energies between 10 and 30 mJ, the ablation product yield increases linearly, reaching approximately 1012 salt molecules per 30 mJ pulse. Using mass spectrometry, we observe Li+, Na+, and K+ in the plumes of ablated NaCl, KCl, and LiCl, which implies dissociation of the volatilized material. We do not observe salt ions (e.g., NaCl+). However, with 800 nm femtosecond laser pulses, the triatomic ion clusters Li2Cl+, Na2Cl+, and K2Cl+ are produced. Finally, we observe incomplete volatilization with the nanosecond pulses: some of the ejecta are liquid droplets. The insights about ablation plume physics gleaned from these experiments should guide future implementations of the laser-volatilization technique.
作者: Alexander W. Raymond,Kin Long Kelvin Lee,Michael C. McCarthy,Brian J. Drouin,Eric Mazur
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Investigating the feasibility of using a miniature Fourier transform millimeter-wave (FTmmW) cavity spectrometer for detecting laser-volatilized salts (NaCl and KCl) in situ, relevant for icy moons in the outer solar system, and characterizing the laser ablation process.

The study demonstrates the feasibility of using a miniature FTmmW spectrometer for in situ detection of laser-volatilized salts, relevant for icy moons exploration. The instrument's specificity in identifying molecular composition complements mass spectrometry. Future work should refine the laser ablation source to improve volatilization yield and explore detection of organic molecules.

The study notes incomplete volatilization with nanosecond pulses, leading to liquid droplets in the ejecta. The ionization fraction for nanosecond pulses is estimated to be low (10?7 to 10?6), and the absence of salt ions in mass spectra complicates interpretation. Future improvements should focus on more complete solid-to-vapor conversion.

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