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Journal of Physics B Atomic and Molecular Physics

A method for the direct determination of the decay rate γ0for the population of an excited state

Harry Gunn, Weston J. Sandle

Published Jan 1, 1971• 6 citations
Publisher

Abstract

The method involves the application of a depolarizing magnetic field at the 'no-polarization' angle of 54.7 degrees to the electric vector of the optical resonance excitation. The decay of fluorescence following a pulse of excitation then gives gamma 0 directly. Application is made to the 5 3 P 1 state of cadmium.
DOI
10.1088/0022-3700/4/1/001

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Following (i) a sharp step or (ii) a pulse of applied magnetic field, the resonance fluorescence of an atomic vapour exposed to steady linearly polarized resonance radiation undergoes transient behaviour until a new steady state is reached; the form of the transient will be (i) modulation of the intensity with an exponential envelope, or (ii) simple exponential decay. From the modulation period the gJ value of the excited state is obtained. From the exponential decay the lifetime for the relaxation of atomic alignment is obtained directly. The technique, applied to the 63P1 state of mercury, gives 117.4+or-1.0 ns for the natural mean life.
The polarization of the resonance fluorescence of interacting atoms and the transfer of coherence, due to the exchange of excitation, are studied theoretically. The treatment is for the general case where both the excited and the ground states can have arbitrary angular momenta, except that they can be connected to each other by an allowed transition. Electrostatic dipole–dipole interaction and electromagnetic radiative interaction are considered simultaneously as the perturbations on the system. Heitler and Ma's generalized time-dependent perturbation method is used. The system is quantized with respect to the space-fixed z axis and a static magnetic field along the z axis may be present, so that the magnetic sublevels (m, m′, etc., for the excited state J, and α, β, etc., for the ground state J′) are not necessarily degenerate. The intensity of the scattered light of a given polarization, in a given direction, is expressed as a function of kR (where ℏck is the energy of excitation and R is the internuclear distance), and of the orientation of R with respect to z axis. The matrix elements (ℏ / 2)γmβ,αm′ and Vmβ,αm′, which cause resonant transfer of excitation between two atoms through radiative and electrostatic interaction, respectively, are also expressed as a function of kR, and of the orientation of R. For randomly oriented atoms, the polarization after being averaged over the random orientation of R becomes a function of kR. Numerical calculations have been carried out for S01 → 1P1 transition. The coherence is shown to be conserved upon resonant transfer of excitation when R is parallel to the quantization axis.
The theory of how excited-state hyperfine structure can be determined using a magnetic field to decouple the nuclear and electronic angular momentum is presented. The initial excited state is assumed to have an anisotropic Zeeman sublevel population distribution, which can be conveniently created by a laser-induced multiphoton excitation of an unpolarized atom. The Zeeman sublevel populations are subsequently mixed by the hyperfine interaction. The degree of mixing is controlled by a magnetic field applied along the quantization axis. The relative Zeeman sublevel populations can be monitored by detecting the polarization of fluorescence emitted when the excited state radiatively decays. It is convenient to take the ratio of two time-integrated fluorescent signals measured for orthogonal linear polarizations, since this is independent of the excited-state number density. The plot of this ratio versus magnetic field is very well approximated by a Lorentzian curve whose half-width is proportional to the magnetic dipole hyperfine coupling constant. This method was used to determine the magnitude of the magnetic dipole constant of the cesium 8D3/2{\mathit{D}}_{3/2}D3/2​ state to be 3.92\ifmmode\pm\else\textpm\fi{}0.10 MHz, which is in excellent agreement with previous results.
Excitation of atoms in a vapor by polarized light produces unequal population of the magnetic sublevels of the excited state. The emitted optical resonance radiation is therefore partly polarized. The application of radiofrequency or microwave fields at a magnetic resonance frequency will induce transitions between sublevels of the excited state. The degree of polarization of the emitted optical resonance radiation is altered when the magnetic resonance condition is fulfilled. As suggested by Brossel and Kastler, this effect may be used to reveal the structure of the energy level. A detailed theory applicable to, and experiments on the 3P1^{3}P_{1}3P1​ state of all the isotopes of mercury are reported. The results obtained indicate that double resonance phenomena constitute a valuable new tool for investigating the structure of atomic energy levels. The mean life of the 3P1^{3}P_{1}3P1​ state is shown by observations on the resonance line widths to be 1.55\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}7}$ sec for all the isotopes. The ggg-factor of the 3P1^{3}P_{1}3P1​ state for isotopes with zero spin, measured in terms of the proton ggg-factor, is 1.4838\ifmmode\pm\else\textpm\fi{}0.0004.