A new pulsed Laval nozzle apparatus with vacuum ultraviolet (VUV) synchrotron photoionization quadrupole mass spectrometry is constructed to study low-temperature radical-neutral chemical reactions of importance for modeling the atmosphere of Titan and the outer planets. A design for the sampling geometry of a pulsed Laval nozzle expansion has been developed that operates successfully for the determination of rate coefficients by time-resolved mass spectrometry. The new concept employs airfoil sampling of the collimated expansion with excellent sampling throughput. Time-resolved profiles of the high Mach number gas flow obtained by photoionization signals show that perturbation of the collimated expansion by the airfoil is negligible. The reaction of C2H with C2H2 is studied at 70 K as a proof-of-principle result for both low-temperature rate coefficient measurements and product identification based on the photoionization spectrum of the reaction product versus VUV photon energy. This approach can be used to provide new insights into reaction mechanisms occurring at kinetic rates close to the collision-determined limit.
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December 2011
Research Article|
December 15 2011
Airfoil sampling of a pulsed Laval beam with tunable vacuum ultraviolet synchrotron ionization quadrupole mass spectrometry: Application to low-temperature kinetics and product detection
Satchin Soorkia;
1Departments of Chemistry and Physics,
University of California
, Berkeley, California 94720, USA
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Chen-Lin Liu;
1Departments of Chemistry and Physics,
University of California
, Berkeley, California 94720, USA
2Chemical Sciences Division,
Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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John D. Savee;
John D. Savee
3Combustion Research Facility,
Sandia National Laboratories
, Mail Stop 9055, Livermore, California 94551, USA
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Sarah J. Ferrell;
Sarah J. Ferrell
2Chemical Sciences Division,
Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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Stephen R. Leone;
Stephen R. Leone
1Departments of Chemistry and Physics,
University of California
, Berkeley, California 94720, USA
2Chemical Sciences Division,
Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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Kevin R. Wilson
2Chemical Sciences Division,
Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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a)
Present address: Institut des Sciences Moléculaires d’Orsay, Université Paris-Sud 11, CNRS UMR 8214, 91405 Orsay, France.
b)
Present address: National Synchrotron Radiation Research Center (NSRRC), Hsinchu 30076, Taiwan.
c)
Author to whom correspondence should be addressed. Electronic mail: krwilson@lbl.gov.
Rev. Sci. Instrum. 82, 124102 (2011)
Article history
Received:
October 26 2011
Accepted:
November 22 2011
Citation
Satchin Soorkia, Chen-Lin Liu, John D. Savee, Sarah J. Ferrell, Stephen R. Leone, Kevin R. Wilson; Airfoil sampling of a pulsed Laval beam with tunable vacuum ultraviolet synchrotron ionization quadrupole mass spectrometry: Application to low-temperature kinetics and product detection. Rev. Sci. Instrum. 1 December 2011; 82 (12): 124102. https://doi.org/10.1063/1.3669537
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