The focusing, by means of an electrostatic quadrupole, of polar molecules with first‐ or second‐order Stark effects is discussed. Indications of molecular electronic symmetry may be obtained from quantitative measurements of the intensity of refocusing of beams of diatomic molecules. Such measurements indicate that the ground state of LiO is Π while that of LaO is Σ. It is suggested that the optical spectroscopic data of ScO, YO, and LaO are best explained by assigning the ground states of these three molecules as 2Σ. The observed low‐lying electronic states of these molecules are interpreted in terms of a localized‐orbital picture.

Determination of Electronic Symmetry by Electric Deflection: LiO and LaO

An analysis of the O2+b4Σg−-a4Πu First Negative band system

The perturbation due to spin‐orbit and spin‐spin interactions has been studied for a Hund's Case b diatomic molecule with two outer electrons. The interactions are expressed as scalar products of two irreducible tensors and Racah's method is used to compute the off‐diagonal matrix elements between states differing by ΔΛ=0, ±1, ±2; ΔS=0, ±1; ΔN=0, ±1, ±2. The matrix elements are used to study the ``forbidden predissociation'' of the metastable c 3Πu state of H2 via the repulsive b 3Σu+ state, which was the mechanism assumed by Lichten to account for the differences in the lifetimes of fs levels of c 3Πu state of H2. The relative lifetimes of fs levels thus calculated are in reasonable agreement with Lichten's measurements. The N dependence of the matrix element of spin‐orbit interaction is shown to be similar to that of spin‐spin interaction. The second‐order perturbations via intermediate states are found to have N dependence similar to that of the first order when N is large. The interference among diffe...

Electron Magnetic Perturbation in Diatomic Molecules of Hund's Case b

A formalism for obtaining the effective rotational hamiltonian for any open-shell molecule is described. This effective hamiltonian is shown to be formed of series of irreducible tensors composed of real and fictitious angular momentum operators. The operations of these tensors may in all cases be restricted to a particular electronic state. Application of such a formalism should be particularly valuable in the interpretation of the high resolution spectra (zero-field microwave, gas-phase electron resonance, etc.) of open-shell molecules, for it follows that the experimental data may always be interpreted without explicit reference to electronic states other than that wherein the spectrum originates. Useful rules are given which determine the relevant orders of tensors in the series and the method is illustrated for the case of a 3Σ diatomic molecule.

The effective rotational hamiltonian for open-shell molecules

The heterogeneous perturbation of the a 3Π (υ = 4) state of CO by the nearly degenerate a′ 3Σ+ (υ′ = 0) state is observed in the rf electric–dipole spectrum of the metastable a 3Π (υ = 4) state. Perturbed lambda doublings and Stark effects in states | υ, Ω, J〉 = | 4, 2, 2–6〉 have been measured in molecular‐beam electric resonance from 7–400 MHz. These measurements are combined with existing optical data to obtain the off‐diagonal matrix elements of the fine structure which describe the a–a′ interaction, 〈a 3Π ‖ AL+ / 2 ‖ a′ 3Σ+〉 = − 18.1 ± 0.3 cm−1, 〈a 3Π ‖ BL+ ‖ a′ 3Σ+〉 = 0.16 ± 0.01 cm−1, and the diagonal and off‐diagonal components of the dipole moment, 〈a 3Π ‖ μ ‖ a 3Π〉 = 1.3791 ± 0.0003 D, 〈a 3Π ‖ μ ‖ a′ 3Σ+〉 = 0.62 ± 0.02 D. This last quantity is identically the electronic transition moment of the (a′ 3Σ+−a 3Π) Asundi system.

Molecular‐Beam Electric‐Resonance Spectroscopy of the a 3Π (υ = 4)−a′ 3Σ+ (υ′ = 0) Perturbation in CO

Similarity between the Spin-Spin and Spin-Orbit Interactions in the Diatomic Molecules

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Similarity between the Spin-Spin and Spin-Orbit Interactions in the Diatomic Molecules