Infrared FEL photochemistry: Multiple-photon dissociation of Freon gas

摘要

Wavelength tunability, synchrotron sidebands, and picosecond pulse structure are inherent FEL characteristics that should be advantageous for photochemistry involving infrared multiple-photon photodissociation. Tuned to an absorption resonance, the FEL sideband structure will overlap the broad, excited-state spectral absorption and should lead to enhanced dissociation. The Los Alamos APEX FEL was operated with and without sidebands to test this hypothesis on CFCl(sub 3) (Freon 11), an inert chlorofluorocarbon widely used in refrigeration systems and one of the gases implicated as depleting the ozone in the Earth's stratospheric layer. The FEL wavelength was set at the C-Cl stretch absorption resonance at 11.8-(mu)m, the oscillator cavity length was detuned first to minimize and then to maximize the spectral bandwidth, and the beam was focused through a pair of test cells (1.0 Torr Freon+1.7 Torr air). Comparison of final and initial absorbance spectra indicated the CFCl(sub 3) photodissociation yield was 1.2% for the cell exposed with sideband spectra (3% FWHM) and 9-ns micropulse separation. Negligible effect was seen without sidebands, albeit at lower total beam fluence. Although the result of this single experiment is not large enough to be conclusive, it does provide a basis for optimizing the FEL temporal and spectral parameters to attain higher photodissociation yield in future tests.