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

Charvat, A. and Stasicki, Boleslaw and 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), pp. 3297-3306. American Chemical Society. doi: 10.1021/jp055165e.

Full text not available from this repository.

Abstract

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.

Item URL in elib:https://elib.dlr.de/21938/
Document Type:Article
Additional Information: Published on Web 02/10/2006
Title:Product screening of fast reactions in IR-laser-heated liquid water filaments in vacuum by mass spectrometry
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iDORCID Put Code
Charvat, A.Universität Göttingen, Institut für Physikalische ChemieUNSPECIFIEDUNSPECIFIED
Stasicki, BoleslawUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Abel, BerndMax-Planck-Institut für biophysikalische Chemie, GöttingenUNSPECIFIEDUNSPECIFIED
Date:2006
Journal or Publication Title:The Journal of Physical Chemistry A
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:No
In ISI Web of Science:Yes
Volume:110
DOI:10.1021/jp055165e
Page Range:pp. 3297-3306
Publisher:American Chemical Society
Status:Published
Keywords:high-speed laser stroboscopy, high-temperature water environments
HGF - Research field:Aeronautics, Space and Transport (old)
HGF - Program:Aeronautics
HGF - Program Themes:Aircraft Research (old)
DLR - Research area:Aeronautics
DLR - Program:L AR - Aircraft Research
DLR - Research theme (Project):L - Flight Physics (old)
Location: Göttingen
Institutes and Institutions:Institute of Aerodynamics and Flow Technology > Experimental Methods
Deposited By: Micknaus, Ilka
Deposited On:21 Jun 2006
Last Modified:27 Apr 2009 04:56

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