A proper account of core-polarization with pseudopotentials: single valence-electron alkali compounds

Publisher Summary This chapter discusses several experimental studies conducted on cluster ions. Cluster ions comprise a nonrigid assembly of components having properties between those of large gas phase molecules and the bulk condensed state. Research on the properties of cluster ions is valuable in obtaining a complete understanding of the forces between ions and neutral atoms or molecules, where, for example, data on energetics provide a direct measure of the depth of the potential well of interaction between the ion and the collection of neutral molecules. There are three types of experimental approaches to produce and study these cluster ions depending on different degrees of physical isolation, that is, clusters moving freely in space (gas phase studies), clusters supported upon a substrate surface, and clusters existing in solids and liquids. Moreover, the use of cluster ions for fuel injection into fusion reactors and cluster ions are also present in other high-temperature systems such as those designed as sources of energy employing magnets and hydrodynamics.

Experimental studies on cluster ions

Picosecond transient absorption measurements from 1000–295 nm are used to monitor the recombination dynamics of iodine after photodissociation in a variety of inert solvents The high time resolution and signal‐to‐noise ratio of these measurements permits the development of a detailed model of this reaction, which should resolve disagreements over the time scales of geminate recombination and vibrational relaxation and over the role of excited electronic state trapping Most of the atoms which undergo geminate recombination do so in ≤15 ps, in agreement with the predictions of existing molecular dynamics simulations The subsequent vibrational and electronic energy relaxation of the recombined molecule is relatively slow and accounts for most of the transient absorption dynamics The relaxing X‐state vibrational population distribution is extracted with an approximate method using calculated spectra of the excited vibrational levels and is compared to recent models Vibrational relaxation times vary from 

Studies of chemical reactivity in the condensed phase. I. The dynamics of iodine photodissociation and recombination on a picosecond time scale and comparison to theories for chemical reactions in solution

Lifetime measurements are reported for high principal quantum number (n=40–125) Rydberg states of the NO molecule, prepared using state‐selective double resonance excitation with a narrow bandwidth laser. The influence of (i) the application of a dc electric field, and (ii) interactions of the Rydberg states with surrounding ions, were investigated. It is demonstrated that the presence of dc electric fields can lead to enhancements in the lifetimes due to l‐mixing, and the conclusion is reached that under the conditions existing in a typical zero‐electron‐kinetic‐energy (ZEKE) photoelectron spectroscopy experiment, the Rydberg states involved are excited in a regime where l‐mixing is expected to be significant. It is observed that l‐ and m‐mixing collisional interactions provide a further mechanism to stabilize the optically prepared Rydberg states, beyond the limits which can be achieved by l‐mixing alone.

Lifetimes of Rydberg states in zero‐electron‐kinetic‐energy experiments. I. Electric field induced and collisional enhancement of NO predissociation lifetimes

Although the diatomic halogens are endowed with a wide range of intravalence-shell electronic states, the number and variety of these states is far from obvious in one-photon absorption from the ground state where only a few regions of structured absorption are present at visible and UV wavelengths. Selection rules on angular momentum and parity are key players in enforcing this sparse structure, but Franck- Condon effects also exercise considerable influence by directing transitions into regions where the transition dipole is small o r into a continuum where much of the detail is lost: further, a simultaneous excitation of two o r more electrons is formally forbidden in single-photon transitions. Some of the obstacles to one-photon absorption are avoided in the sequential absorption of two o r three photons using the conveniently placed, low-lying excited sQtes in the visible region for the initial step, in effect broadening the perspective from the ground state to include that from the lower ex...

Multiphoton Spectra and States of Halogens

Electric-field-hindered vibrational autoionization in molecular Rydberg states.

Extensive study of the 1g(3P2) ion pair state of I2

OODR excitation of the 0g+(3P0) state of I2 up to 53800 cm−1

The 1 g and 0+ g (3 P 2) ionic states of iodine interact via the rotational hamiltonian. The resulting Ω doubling in the 1 g state is studied in detail. A value of 103 is deduced for the ratio of the transition probabilities of the 0+ g ← B and 1 g ← B transitions. A complete interpretation of their relative intensities involves saturation effects which are clearly observed for the 0+ g ← B transition. The results give a complete explanation as to why the 0+ g state was the only one to be excited in this spectral region by former workers.

Ω doubling in 1 g state and electronic transition moments for B0+ u towards 0+ g and 1 g (3 P 2) states of iodine

Determinations of electronic transition moments rely generally on the r-centroid approximation. This method is no longer valid when, in the stationary phase approximation, two transition points occur. A purely quantal treatment is applied here to the determination of electronic transition moments M e(r) from both line intensities and lifetime measurements for the 1 g (3 P 2) → A1 u and 0+ g (3 P 2) → B0+ u transitions of the I2 molecule.

Electronic transitions moments from both fluorescence intensities and lifetime measurements for transitions involving the I2 ionic states

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