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Journal of Luminescence

Infrared time resolved saturation spectroscopy of CO in solid N2 : A study of vibrational dephasing and spectral diffusion mechanisms

M. Harig, Renée Charneau, Henri Dubost

Published Nov 1, 1981• 10 citations
Publisher
DOI
10.1016/0022-2313(81)90061-2

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Physical Review Letters•Sep 6, 1982•21 citations
Infrared picosecond accumulated photon echo experiments have been performed for the first time, using the Orsay Free Electron Laser, on the $v\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0\ensuremath{\rightarrow}v\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1$ transition of CO in solid nitrogen. The vibrational dephasing time is found to be exceptionally long ( ${T}_{2}\ensuremath{\ge}120$ ns) at low temperature. The analysis of the observed spectral diffusion leads one to assume different energy transfer mechanisms depending on the CO concentration.
The influence of the environment on vibrational dynamics, and especially on the vibrational dephasing time, is investigated for a simple system : DCl in a van der Waals solid (N2 lattice). Photon echo experiments are performed using the infrared free electron laser CLIO. In solid nitrogen, decay times of the third order polarization are in the picosecond range. In the case of the isolated DCl monomers in van der Waals interaction with the host, the observed signals are interpreted in term of a rapid spectral diffusion. The two different stretching modes of DCl dimers, perturbed in a different way by the weak hydrogen bond, exhibit different coherence times, reflecting the influence of the interaction strength between the molecules.
The population hole burned within the inhomogeneously broadened ir fundamental absorption band of 12C^{12}\mathrm{C}12C17O^{17}\mathrm{O}17O in solid N2{\mathrm{N}}_{2}N2​ by a narrow-band pulsed laser is detected as an antihole in the transient absorption of a tunable cw probe beam whose frequency is swept through the $v=1\ensuremath{\rightarrow}v=2$ resonance. The time development of the transient profile demonstrates that spectral diffusion is governed by an energy-dependent process, contrary to what has been observed in many disordered systems.