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Line shape theory for a Doppler-broadened signal in presence of an infrared pump
Published in -
Volume: 83
Issue: 8
Pages: 4015 - 4023
A theory of line shape for a Doppler broadened probe in the presence of a strong infrared pump is presented. The optical analog of Bloch equations has been developed; the T1, T2 relaxations are introduced phenomenologically in these equations. Doppler broadening of both the pump and signal transitions are taken into account to obtain the absorption coefficient for the signal. This leads to a Doppler broadened Gaussian function weighted by a pump induced Lorentzian function whose position and linewidth are controlled by the detuning and power respectively of the pump radiation. The absorption coefficient is further modulated by a Lorentzian function containing the fourth power of the radiation. The off-resonance pumping leads to two symmetrically located "Lamb dips" or "peaks" around the Gaussian pedestal for co- and counter propagating laser radiations. A calculation of the line shape of the central sub-Doppler feature for the on-resonance pumping is in good agreement with the observed variation of linewidth with pressure. Numerical results are presented graphically to demonstrate the pump and signal power dependence of the central hole or peak for the bent and cascade-type double resonances. The results obtained confirm the expected behavior based on level populations. © 1985 American Institute of Physics.
About the journal
JournalThe Journal of Chemical Physics