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Product screening of fast reactions in IR-laser-heated liquid water filaments in vacuum by mass spectrometry

Charvat, A. und Stasicki, Boleslaw und Abel, Bernd (2006) Product screening of fast reactions in IR-laser-heated liquid water filaments in vacuum by mass spectrometry. The Journal of Physical Chemistry A, 110 (9), Seiten 3297-3306. American Chemical Society. DOI: 10.1021/jp055165e.

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In the present article a novel approach for rapid product screening of fast reactions in IR-laser-heated liquid microbeams in a vacuum is highlighted. From absorbed energies, a shock wave analysis, high-speed laser stroboscopy, and thermodynamic data of high-temperature water the enthalpy, temperature, density, pressure, and the reaction time window for the hot water filament could be characterized. The experimental conditions (30 kbar, 1750 K, density ∼1 g/cm3) present during the lifetime of the filament (20-30 ns) were extreme and provided a unique environment for high-temperature water chemistry. For the probe of the reaction products liquid beam desorption mass spectrometry was employed. A decisive feature of the technique is that ionic species, as well as neutral products and intermediates may be detected (neutrals as protonated aggregates) via time-of-flight mass spectrometry without any additional ionization laser. After the explosive disintegration of the superheated beam, high-temperature water reactions are efficiently quenched via expansion and evaporative cooling. For first exploratory experiments for chemistry in ultrahigh-temperature, -pressure and -density water, we have chosen resorcinol as a benchmark system, simple enough and well studied in high-temperature water environments much below 1000 K. Contrary to oxidation reactions usually present under less extreme and dense supercritical conditions, we have observed hydration and little H-atom abstraction during the narrow time window of the experiment. Small amounts of radicals but no ionic intermediates other than simple proton adducts were detected. The experimental findings are discussed in terms of the energetic and dense environment and the small time window for reaction, and they provide firm evidence for additional thermal reaction channels in extreme molecular environments.

Zusätzliche Informationen: Published on Web 02/10/2006
Titel:Product screening of fast reactions in IR-laser-heated liquid water filaments in vacuum by mass spectrometry
AutorenInstitution oder E-Mail-Adresse der Autoren
Charvat, A.Universität Göttingen, Institut für Physikalische Chemie
Abel, BerndMax-Planck-Institut für biophysikalische Chemie, Göttingen
Erschienen in:The Journal of Physical Chemistry A
Referierte Publikation:Ja
In ISI Web of Science:Ja
DOI :10.1021/jp055165e
Seitenbereich:Seiten 3297-3306
Verlag:American Chemical Society
Stichwörter:high-speed laser stroboscopy, high-temperature water environments
HGF - Forschungsbereich:Verkehr und Weltraum (alt)
HGF - Programm:Luftfahrt
HGF - Programmthema:Starrflügler
DLR - Schwerpunkt:Luftfahrt
DLR - Forschungsgebiet:L AR - Starrflüglerforschung
DLR - Teilgebiet (Projekt, Vorhaben):L - Flugphysik
Standort: Göttingen
Institute & Einrichtungen:Institut für Aerodynamik und Strömungstechnik > Experimentelle Verfahren
Hinterlegt von: Ilka Micknaus
Hinterlegt am:21 Jun 2006
Letzte Änderung:27 Apr 2009 04:56

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