Be. Newnam et al., INFRARED FEL PHOTOCHEMISTRY - MULTIPLE-PHOTON DISSOCIATION OF FREON GAS, Nuclear instruments & methods in physics research. Section A, Accelerators, spectrometers, detectors and associated equipment, 341(1-3), 1994, pp. 142-145
Wavelength tunability, synchrotron sidebands, and picosecond pulse str
ucture are inherent characteristics of free-electron lasers (FELs) tha
t should be advantageous for photochemistry involving multiple-photon
photodissociation. Tuned to absorption resonance, the FEL sideband str
ucture will overlap the broad, red-shifted, quasi-continuous excited-s
tate absorption spectra and should lead to enhanced dissociation. The
Los Alamos APEX FEL was operated with and without sidebands to test th
is hypothesis on CFCl3 (Freon 11), one of the gases implicated as depl
eting the ozone in the Earth's stratospheric layer. The FEL wavelength
was set at the C-Cl stretch absorption resonance at 11.8 mum, the osc
illator cavity length was detuned first to minimize and then to maximi
ze the spectral bandwidth, and the beam was focused through a pair of
test cells. Comparison of final and initial absorbance spectra indicat
ed the CFCl3 photodissociation yield was 1.2% for the cell exposed wit
h sideband spectra (3% FWHM) and 9-ns micropulse separation. Negligibl
e effect was seen without sidebands, albeit at lower total beam fluenc
e.