Abstract
Time-resolved coherent anti-Stokes Raman scattering is applied to prepare and interrogate vibrational coherences on the ground electronic surface of molecular iodine isolated in Ar matrices. The coherence decay time shows a linear dependence on vibrational quantum numbers for v=3–15. The temperature dependence of decoherence rates is negligible for v<7 in the experimental range T=18–32 K. For a v=13, 14 superposition, the temperature dependence indicates dephasing by a 66 cm−1 pseudo-local phonon, just outside the Debye edge of the solid. The accuracy of the data is limited due to two-photon induced dissociation of the molecule, a process which is characterized using polarized fields. The T→0 limit of dephasing is discussed.
Highlights
In a recent paper we reported time-resolved coherent anti-Stokes Raman scatteringTRCARSmeasurements on I2 isolated in an Ar matrix.[1]
A detailed analysis of the process was presented, based on data limited to wave packets prepared near vϭ[4], and limited to Tϭ32 K
TRCARS measurements are well suited for the preparation of vibrational coherences and the detailed analysis of their dephasing.[2,3]
Summary
In a recent paper we reported time-resolved coherent anti-Stokes Raman scatteringTRCARSmeasurements on I2 isolated in an Ar matrix.[1] A detailed analysis of the process was presented, based on data limited to wave packets prepared near vϭ[4], and limited to Tϭ32 K. We have since succeeded in making measurements on packets prepared at vibrations as high as vϭ[14], and as a function of temperature, for Tϭ17– 33 K. TRCARS measurements are well suited for the preparation of vibrational coherences and the detailed analysis of their dephasing.[2,3] The characterization of vibrational decoherence in this model system: a diatomic impurity, in an atomic solid, with weak and relatively well understood coupling between molecule and lattice,[4] is our aim. Of particular interest is the understanding of decoherence in the T→0 limit.[5]
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