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• W1520341047 abstract "The dynamics of vibrational relaxation in polyatomic van der Waals clusters is investigated theoretically, using as an example a one-dimensional model of I2(Ne) N with excited I2 vibration. The method employed is classical dynamics simplified by the time-dependent self-consistent-field (TDSCF) approximation. The dependence of the relaxation on cluster size is examined, with calculations for N = 4, 8, 16 and with extrapolation to N → ∞ representing I2 in a solid Ne matrix. Also studied is the variation of the relaxation mechanism with initial vibrational state v, in the range v = 25–60. The main results are: (i) Relaxation can be interpreted best as affected by collisions between I2 and neighbouring Ne atoms. Collective modes do not, in most cases, play a significant role in the relaxation. (ii) The I2 centre-of-mass vibration plays a less significant role than the Ne atoms in the redistribution of the released vibrational energy in the cluster. (iii) The initial relaxation rate decreases with cluster size, the lifetime of v = 28 being τ = 3·6 ps for N = 4 and τ = 51 ps for N = 8. This is due to decreasing frequency of impulsive I2-Ne ‘collisions’ in the larger clusters. (iv) Initial relaxation behaviour and rates for the N = 16 cluster appear converged to those of the corresponding solid matrix. (v) relaxation dynamics switches from weak to strong coupling-type behaviour as v increases from 35 to 60." @default.
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• W1520341047 date "1985-09-01" @default.
• W1520341047 modified "2023-09-26" @default.
• W1520341047 title "Relaxation of vibrationally highly excited diatomics in van der Waals clusters" @default.
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• W1520341047 doi "https://doi.org/10.1080/00268978500102151" @default.
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