Tabletop Femtosecond VUV Photoionization and PEPICO Detection of Microreactor Pyrolysis Products

Couch, David E.; Buckingham, Grant T.; Baraban, Joshua H.; Porterfield, Jessica P.; Wooldridge, Laura A.; Ellison, G. Barney; Kapteyn, Henry C.; Murnane, Margaret M.; Peters, William K.

doi:10.1021/acs.jpca.7b02821

Title: Tabletop Femtosecond VUV Photoionization and PEPICO Detection of Microreactor Pyrolysis Products

Journal Article · Thu Jun 29 00:00:00 EDT 2017 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.7b02821· OSTI ID:1686161

^[1]; Buckingham, Grant T. ^[2]; Baraban, Joshua H. ^[1]; Porterfield, Jessica P. ^[3]; Wooldridge, Laura A. ^[1];

^[1]; Kapteyn, Henry C. ^[1]; Murnane, Margaret M. ^[1];

^[1]

Univ. of Colorado, Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Colorado, Boulder, CO (United States); Harvard-Smithsonian Center for Astrophysics, Cambridge, MA (United States); Harvard Univ., Cambridge, MA (United States)

Here, we report the combination of tabletop vacuum ultraviolet photoionization with photoion--photoelectron coincidence spectroscopy for sensitive, isomer-specific detection of nascent products from a pyrolysis microreactor. Results on several molecules demonstrate two essential capabilities that are very straightforward to implement: the ability to differentiate isomers, and to distinguish thermal products from dissociative ionization. We derive vacuum ultraviolet light is from a commercial tabletop femtosecond laser system, allowing data to be collected at 10 kHz; this high repetition rate is critical for coincidence techniques. The photoion—photoelectron coincidence spectrometer uses the momentum of the ion to identify dissociative ionization events, and coincidence techniques to provide a photoelectron spectrum specific to each mass, which is used to distinguish different isomers. We also have used this spectrometer to detect the pyrolysis products that result from the thermal cracking of acetaldehyde, cyclohexene, and 2-butanol. The photoion—photoelectron spectrometer can detect and identify organic radicals and reactive intermediates that result from pyrolysis. Direct comparison of laboratory and synchrotron data illustrate the advantages and potential of this approach.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-99ER14982; AC02-05CH11231; CBET-1403979

OSTI ID:: 1686161

Alternate ID(s):: OSTI ID: 1372114

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 121, Issue 28; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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