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Zeitschrift für angewandte Mathematik und Physik

On the emission spectrum of atomic N in solid N2: Vibrational relaxation rates of N2

O. Oehler, K. Dressler

Published Jul 1, 1971• 0 citations
Publisher
DOI
10.1007/bf01587783

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The behavior of the sensitized fluorescent spectrum of sodium, produced by irradiating Hg–Na–N2 mixtures with Hg 2537 Å resonance radiation, was studied in relation to N2 pressure. In this ternary vapor-gas system, the sodium atoms become excited by collisional transfer from Hg 63P1 atoms and also from Hg 63P0 atoms which are formed in Hg(63P1) + N2 collisions. The spontaneous decay of the collisionally populated S, P, and D sodium states gives rise to the fluorescent spectrum and their radiationless decay (quenching) caused by collisions with N2 molecules, manifests itself in a decrease of the fluorescent intensities as N2 pressure is increased. An analysis of the variation of the fluorescent intensities with N2 pressure, yielded 15 quenching cross sections for various S, P, and D sodium states, which appear to exhibit resonance properties with respect to upward vibrational transitions in N2.
A thermal energy beam of helium atoms in the metastable state is used to coherently excite ions of Sr, Ca, and Ba in a Penning collision. The anisotropic excited state distributions appears as Polarized line emission from the excited ions. The degree of ion alignment may be used to determine the populations of the quasi-molecular states of the ion-atom pair. The coherent emission is also utilized to obtain Hanle signals from which the radiative decay rate of the excited ion is determined. This is the first case in which coherence is produced in a collision process involving Penning ionization. The alignment of the Penning ions is an important new parameter in the description of these reactions. In an effort to extend such observations to molecular systems a nitrogen molecular metastable beam source was demonstrated. The use of metal vapor targets and the excitation rate of the excited states of Cd and Zn in energy transfer collisions with the N2(m) enable us to determine the vibrational distribution of the A 3Sigma state of N2 in the beam. Energy transfer cross sections and some Penning cross sections were measured in the beam system. (Author)
The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.