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Optics and Spectroscopy

Radiative properties of Zeeman components of atomic multiplets: Magnetically induced decay of metastable 3 P 2 and 3 P 0 states of inert gases

V. D. Ovsyannikov, Evgenii V Chaplygin

Published Feb 1, 2001• 2 citations
Publisher

Abstract

It is shown that the magnetic field induces the radiative decay of metastable states of inert gases by mixing them with resonant sublevels of the lowest multiplet. The polarization and frequency structures of the “forbidden” lines induced by the magnetic field are determined, and the dependence of the intensity of π and σ components of these lines on the magnetic field is calculated. The effect is totally governed by the paramagnetic atom-field interaction, and the influence of the diamagnetic interaction is insignificant.

DOI
10.1134/1.1351568

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It is shown that the magnetic field induces the radiative decay of metastable states of inert gases by mixing them with resonant sublevels of the lowest multiplet. The polarization and frequency structures of the “forbidden” lines induced by the magnetic field are determined, and the dependence of the intensity of π and σ components of these lines on the magnetic field is calculated. The effect is totally governed by the paramagnetic atom-field interaction, and the influence of the diamagnetic interaction is insignificant.
Analytical expressions for the dependence of the intensity of Zeeman components of doublet lines on the magnetic field are obtained. Sharp changes of these function on passing from the anomalous Zeeman effect to the Paschen-Back effect lead to the disappearance of marginal lines and the equalization of intensities of remaining lines. In the region of the complete Paschen-Back effect, a strong influence on these dependences is produced by the dynamic atom-field interaction, which weakens the paramagnetic effect in the states with a positive magnetic quantum number m and enhances the effect in the states with a negative m . Simple analytical expressions are obtained that take into account the effect of the diamagnetic interaction on line intensities. The role of the diamagnetic interaction increases in Rydberg atomic states with a large spin-orbit splitting. For the states with m > 0, it can lead to the “diamagnetic reversal” of the Paschen-Back effect, i.e., the recovery of the anomalous Zeeman effect.
Under the conditions of the total Paschen-Back effect the diamagnetic interaction determines the dependence of the intensity of the Zeeman components of atomic radiation lines on a magnetic field. The change in the matrix elements of the radiative transitions is due to the magnetically induced corrections to the wavefunctions of the initial and final states, whose contributions are of the same order of magnitude for the head lines of the optical series. For the high-frequency lines the positive corrections to the matrix element from the wavefunction of the upper level dominate. A magnetic field also induces dipole radiative transitions with selection rules for the orbital angular momentum | Δ l | ≥ 3. The matrix elements of such transitions increase rapidly with the energy of the upper level, making possible efficient single-photon population of the dipole-inaccessible Rydberg states in moderate magnetic fields.
We study the effect of diamagnetic interaction on the probability of radiative transitions of an atom from states split by a field. We write the analytic expressions for the diamagnetic corrections to the matrix elements of transitions belonging to the Lyman and Balmer series and of transitions between arbitrary nondegenerate states in hydrogen. We also discuss the perturbation theory for transitions from degenerate diamagnetic states. The theory is based on expanding in powers of the field strength the eigenfunctions and eigenvalues of the matrix of diamagnetic interaction in the subspace of states with given principal and magnetic quantum numbers. The field changes the coefficients in both the superposition and the degenerate basis. To derive the analytic expressions for the higher-order matrix elements, we use the Sturm expansion of the reduced Coulomb Green’s function. We also elaborate on the features of the frequency dependence of the corrections to the radiative matrix elements, which correlate with the structure of the diamagnetic spectrum of excited levels. Finally, we establish that the magnetic field acts selectively on the diamagnetic components of emission lines: as the field strength increases, an increase in the intensity of certain lines is accompanied by a decrease in the intensity of the other lines.
An investigation is made of the change in the magnetic properties of a diamagnetic molecule (atom) induced by a resonance optical radiation field. Calculations are made for the 0→1 molecular transition in the presence of an external magnetostatic field. Expressions are derived for the magnetization and the magnetic susceptibility of the molecule, which depend nonlinearly on the light wave intensity, in the case of longitudinal and transverse directions of the external magnetic field with respect to the direction of propagation of the radiation. It is shown that the field-induced nonlinear magnetic susceptibility of a diamagnetic substance can change sign and increase considerably (by several orders of magnitude compared with the linear diamagnetic susceptibility). The field-induced nonlinear magnetization of the substance does not depend on its magnetic properties and is the same for diamagnetic and paramagnetic substances.
In the intense radiation fields with power density from 104W/cm2 to 109W/cm2 the essential modification of electronic states of atoms occurs displaying, in particular, in modifications of resonant fluorescence (rf) spectra. We use 'Fermi golden rule' for calculations of relative intensities and frequencies for rf multiplet for real multilevel initially unexcited atoms in two monochromatic laser fields of arbitrary intensity resonant to adjacent transitions of (Xi) or (Lambda) types and magnetic field, giving the level splittings of different values from Zeeman to Paschen-Back effect. The dependence of quasienergies on parameters obtained with the help of a sorting program permits us to define the values of parameters for which the states of the system are mixed and so to receive the correct probability amplitudes for instantaneous or adiabatic regimes of switching the perturbation. The analysis of the quasienergies and form of rf spectra permits us to get relations between the form of the spectra and modifications of electronic structure of the atom due to radiation fields and external magnetic field.
By applying an external magnetic field, we have determined the population of the magnetic sublevels of photodissociated atoms from the intensities of atomic fluorescence lines split by the Zeeman effect. A preferential population of the magnetic sublevels of the atomic fragment Na(3 2P3/2), which arises from the direct photodissociation through the D1Π(continuum) state of the NaK molecule, has been observed. The results are explained by assuming the separability of electronic and nuclear motion during the dissociation. The observed results could be rationalized by the sum of the photodissociation amplitudes caused by excitation of the P, Q and R branches. The population of the magnetic sublevels of Rb(5 2P3/2) atoms produced by predissociation of the C1Πu state of the Rb2 molecule by the repulsive molecular state c3Σ+u has been determined from the Zeeman spectra of the emission Rb(5 2P3/2→ 5 2Sm′1/2). The observed results are interpreted by including the spin-orbit coupling between an excited level of the C1Πu state and levels of the c3Σ+u state and the effect of the external magnetic field.