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Physical Review Letters

Time Domain Investigation on Vibrational Dephasing and Spectral Diffusion in CO-Doped Solid N2

Claudine Crépin, Michel Broquier, Henri Dubost, Jean‐Pierre Galaup, J.-L. Le Gouët, J.M. Ortéga

Published Jul 31, 2000• 20 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.85.964

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Infrared picosecond accumulated photon echo experiments have been performed for the first time, using the Orsay Free Electron Laser, on the v=0\ensuremath→v=1v\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0\ensuremath{\rightarrow}v\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1v=0\ensuremath→v=1 transition of CO in solid nitrogen. The vibrational dephasing time is found to be exceptionally long ( T2\ensuremath≥120{T}_{2}\ensuremath{\ge}120T2​\ensuremath≥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 dynamics in the ground electronic state of the two intramolecular D-Cl stretching modes of (DCl)2 in nitrogen solid has been probed by degenerate four wave mixing experiments. Accumulated photon echoes on the "free" nu1 and "bonded" nu2 modes have been performed by means of the free electron laser of Orsay (CLIO). The analysis of the time-resolved signals provides information on the various processes responsible for the loss of vibrational coherence, in particular intra- and intermolecular vibrational energy transfer and pure dephasing. The influence of the weak hydrogen bond is clearly observed on the coherence times of the two stretching modes. Whatever the temperature, the homogeneous width of nu2 lines is almost twice that of nu1 lines. Contrary to the case of isolated DCl trapped in solid nitrogen, no obvious effect of the nitrogen lattice can be extracted from the temperature dependence of the coherence times.
The first infrared vibrational photon echo experiments conducted in a liquid and a glass are reported. The experiments were performed on the CO stretching mode of tungsten hexacarbonyl at 5.1 \ensuremath{\mu}m (1960 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) in 2-methyltetrahydrofuran over the temperature range 300 to 16 K using picosecond pulses from the free electron laser at Stanford University. In addition, the first vibrational population relaxation measurements spanning a temperature range that takes a system from a liquid to a supercooled liquid to a glass are reported.
The first infrared vibrational photon echo experiments conducted in a liquid and a glass are reported. The experiments were performed on the CO stretching mode of tungsten hexacarbonyl at 5.1 micrometers (1960 cm-1) in 2-methyltetrahydrofuran over the temperature range 300 K to 16 K using picosecond pulses from the free electron laser at Stanford University. In addition, the first vibrational population relaxation measurements spanning a temperature range that takes a system from a liquid to a supercooled liquid to a glass are reported.
Vibrational photon echo experiments were performed on the asymmetric CO stretching mode of tungsten hexacarbonyl in glassy dibutylphthalate as a function of temperature using sub-picosecond infrared pulses (1976 cm−1) from a free electron laser. The echo decays display pronounced beats and are bi-exponential. The beats and bi-exponential decays arise because the bandwith of the pulses exceed the vibrational anharmonicity, leading to the excitation and dephasing of a multilevel coherence. From the beat frequency, the anharmonicity is determined to be 14.7 cm−1. From the bi-exponential decay components, the temperature-dependent vibrational dephasing of both the v = 0 → 1 and v = 1 → 2 transitions are determined.