Existing theories of optical pumping do not take into account the relative phase of the optical field which monitors the resonances. In experiments on excited atoms the optical phase relations have a profound effect on magnetic resonance curves. Signals in the forward-scattered light show Doppler broadening, modified by strong coherence narrowing; a result quite different from that for the laterally scattered light. The question is raised as to whether similar effects are to be expected for resonances in the ground states. The problem is analysed in terms of the classical theory of the propagation of light in polarizable media. The (complex) polarizability of the sample under conditions of optical pumping and magnetic resonance is calculated to first order in perturbation theory. An expression is obtained similar to that found for resonance in the excited states, but different in so far as the factor which describes the magnetic resonance (the density matrix for the ground states) is independent of the factor which describes the Doppler effect (the plasma dispersion function). Since the intensity of the transmitted light is a function of the imaginary part of the polarizability, the conclusion is that the ground-state resonance curves should not be Doppler-broadened, which is in agreement with the known facts.
Existing theories of optical pumping do not take into account the relative phase of the optical field which monitors the resonances. In experiments on excited atoms the optical phase relations have a profound effect on magnetic resonance curves. Signals in the forward-scattered light show Doppler broadening, modified by strong coherence narrowing; a result quite different from that for the laterally scattered light. The question is raised as to whether similar effects are to be expected for resonances in the ground states. The problem is analysed in terms of the classical theory of the propagation of light in polarizable media. The (complex) polarizability of the sample under conditions of optical pumping and magnetic resonance is calculated to first order in perturbation theory. An expression is obtained similar to that found for resonance in the excited states, but different in so far as the factor which describes the magnetic resonance (the density matrix for the ground states) is independent of the factor which describes the Doppler effect (the plasma dispersion function). Since the intensity of the transmitted light is a function of the imaginary part of the polarizability, the conclusion is that the ground-state resonance curves should not be Doppler-broadened, which is in agreement with the known facts.
Abstract A theoretical and experimental study has been made of the intensity of forward scattered light in conditions of radio-frequency double resonance and level-crossing. The main conclusions are (i) that the magnetic resonance and level-crossing effects which are familiar in the laterally scattered light are to be found also in the forward scattered light, but (ii) that the resonance curves are Doppler-broadened, and the strength of the oscillatory field necessary to generate them is correspondingly increased, and (iii) that coherence narrowing is much more pronounced in forward than in lateral scattering. The differences derive from the coherence between the radiation from different atoms which is present in forward, but not in lateral scattering, and which is implicitly recognized in the classical theory of the propagation of light in polarizable media. The equations of electromagnetism form the basis of the present analysis. In the presence of the oscillatory magnetic field the polarization tensor is complex and time-dependent. The time dependence leads to the result that the number of eigenwaves necessary to describe propagated waves in the medium is four, as against the usual two. An arbitrary wave is resolved into a superposition of the four eigenwaves, all of which have different propagation constants. The analysis is very general, and is applicable to experiments with lasers. The components of the polarization tensor are derived by finding first the polarizability of individual atoms from a semi-classical theory of their interaction with light and magnetic fields. The macroscopic polarization, obtained by summing over individual atoms, is then given by folding the individual polarizabilities with the Doppler distribution of resonance frequencies. In the particular case studied in detail (the inter-combination resonance line, 2537 A, in mercury), the Doppler width is much greater than the radiation width, and the imaginary (absorptive) part of the polarizability is Gaussian. Expressions are derived in a ‘weak scattering’ approximation for the intensity of the forward scattered light. They are magnetic resonance functions which are found to be the Doppler-broadened equivalents of the familiar functions, based on Lorentzians, characteristic of scattering by a single atom. In the case of double resonance the forward scattered light is strongly modulated, as is the laterally scattered light. To investigate coherence narrowing, the zero-field level-crossing has been studied with the restriction of ‘weak scattering’ removed. The result is obtained that the width of levelcrossing curves is inversely proportional to the vapour density for magnetic fields such that the Zeeman splitting is small in relation to the Doppler width. This analytical result has been verified experimentally.
The ground electronic state of even such simple atoms as those of alkali elements has the set of sublevels. These sublevels are hyperfine (HF) components and magnetic sublevels. The collisions with particles of nonmagnetic buffer gas or even with walls (when walls have proper coating) do not mix practically the populations of ground state HF sublevels, if the orbital moment of electrons in the ground state is equal to zero. Due to this reason these sublevels may be extremely long lived. Because of this, for instance, the so-called effects of optical orientation and optical pumping are apparent in atoms of alkali metals. The radiation can pump practically all the atoms (with which there is effective interaction) to a single HF component. In a situation in which optical pumping is a minor effect, the monochromatic absorption line consists of separate lines corresponding to intra-atomic transitions. The optical pumping is not significant, for example, if the radiation intensity is so low that now pumping between HF sublevels occurs in the time it takes the atom to traverse the light beam. Under the conditions of optical pumping and when other nonlinear effects are present, the absorption line profile can undergo considerable alteration. Many theoretical and experimental investigations have been done in the laser spectroscopy of resonant transitions of atoms (atoms of alkali metals) under the conditions of optical pumping within ground state HF structure. A characteristic feature of all such investigations is the velocity-selective excitation of absorbing atoms. Also, as a rule, the value of HF splitting is not very big in comparison to Doppler broadening in these experiments. Under such conditions, the absorption spectra consists of Doppler- broadened lines with nonlinear resonances, which emerge when two fields of different frequencies or different propagation directions are employed. When only one monochromatic traveling wave is employed, optical pumping leads to formation of a single smooth absorption line occupying a position between the resonant transitions frequencies associated with HF components. As HF splitting grows, the line profile remains smooth, its width is approximately equal to the size of the HF splitting. The strength of the optical pumping from one ground state HF component to another is greater for greater HF splitting in comparison to the Doppler width. In this regard, Cs and Rb are the most typical of the alkali atoms (the HF splitting exceeds the Doppler width by a factor close to 20). This is the qualitative picture of the absorption line profile (particularly for a monochromatic radiation) under the conditions of optical pumping between the HF sublevels of the electronic ground state, this qualitative picture had formed by now.
Existing theories of level crossing and modulation effects in the light scattered from optically thin vapours are restricted to cases where the light from different atoms is either completely incoherent (lateral scattering) or completely coherent (forward scattering). In the latter case the resonances are Doppler broadened equivalents of the well known Lorentzian forms predicted for lateral scattering. The more general case of partial coherence of the scattered light, which might be expected at small scattering angles, has not previously been considered. In this paper the degree of coherence of the scattered light has been formulated in terms of an autocorrelation function. For scattering from an ideal gas the autocorrelation function may be split into two terms representing complete incoherence and complete coherence. The predicted resonances for scattering into an arbitrary direction are mixtures of the Lorentzian and Doppler broadened forms, but the latter have a strong angular dependence that effectively restricted their observation to the small angular range associated with diffraction from the active volume of the vapour.
Optical pumping experiments have been performed on helium 4 atoms in the metastable level 2 3 S 1 with the object of studying the modulation of light in absorption in the longitudinal and transverse beams. Magnetic resonance curves were obtained similar to those found in emission in double-resonance experiments. With a particular geometrical arrangement employing circular polarizers, the Bloch magnetic resonance curves were obtained. Modulation at four times the applied frequency was obtained with a linear polarizer in the pumping beam. This modulation is ascribed to the circulation of coherence in the optical pumping cycle. From the behaviour of the resonance signals as a function of the frequency and amplitude of the stimulating field, it is inferred that a substantial part of the signal arises from coherence which has survived two complete cycles. The observations are satisfactorily explained by the theory developed in the previous paper.
The optical pumping of Cs atoms with light of the D 1 line under magnetic resonance conditions is numerically calculated. This calculation is done to check the suggestion that an unexpectedly strong influence of the polarization of the pumping light on the resonance signals of transverse alignment, which we observed experimentally, is caused by the coupling between orientation and alignment by means of the magnetic field and/or the pumping light. This suggestion has been confirmed: upon circularly polarized pumping, the shape of the signal line of transverse alignment proved to be similar, as well as in the experiment, to the shape of the signal line of transverse orientation and was sharply different from the shape of the line of alignment observed upon linearly polarized pumping. For metastable 23 S 1 4He atoms, in accordance with the experimental data, the calculated shape of the signal line of transverse alignment is found to be independent of the polarization of the pumping light. The calculations also confirm the possibility of a reverse effect: the influence of alignment on orientation, which manifests itself in the occurrence of orientation upon pumping with unpolarized light under magnetic resonance conditions. For Cs atoms exposed to a field of ∼0.6 Oe, the largest contribution to this effect is yielded by the field coupling of orientation and alignment, whereas, for metastable 23 S 1 4He atoms, the largest contribution is made by the light coupling of these polarization moments.
The D1 line spectrally selective pumping process in Doppler-broadened cesium is analyzed by solving the optical Bloch equations. The process, described by a three-level model with the Λ scheme, shows that the saturation intensity of broadened atoms is three orders of magnitude larger than that of resting atoms. The |Fg = 3〉 → |Fe = 4〉 resonance pumping can result in the ground state |Fg = 4, mF = 4〉 sublevel having a maximum population of 0.157 and the population difference would be about 0.01 in two adjacent magnetic sublevels of the hyperfine (HF) state Fg = 4. To enhance the anisotropy in the ground state, we suggest employing dichromatic optical HF pumping by adding a laser to excite D1 line |Fg = 4〉 → |Fe = 3〉 transition, in which the cesium magnetometer sensitivity increases by half a magnitude and is unaffected by the nonlinear Zeeman effect even in Earth's average magnetic field.