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Proceedings of the Physical Society

The polarization of sensitized fluorescence

W Gough

Published Jan 1, 1967• 29 citations
Publisher

Abstract

By means of the selection rule Σ m J = constant along the axis of a collision between two atoms, it is shown that sensitized fluorescence should in some cases be partially polarized. The degree of polarization of the fluorescence of cadmium vapour sensitized by the presence of mercury vapour is calculated for certain states of polarization of the incident radiation. In the case studied experimentally the degree of polarization varies over a range of 2-5%. The theoretical value is 3/11, which is reduced in practice by various depolarizing effects. The possibility of transfer coherence between eigenstates from mercury to cadmium during a collision is considered.

DOI
10.1088/0370-1328/90/1/335

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Collisional Transfer of Coherence: Polarization of Sensitized Fluorescence

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Energy transfer and coherence transfer between two atoms of different species are studied theoretically. The electric dipole-dipole interaction is the mechanism considered for the excitation transfer. A generalized perturbation method for a damping system is used. A general formula is derived for the polarization of the sensitized fluorescence resulting from the excitation transfer. This polarization is shown to be dependent on the angular momenta of the two atoms, and to be independent of their relative velocity as well as of their difference in the energy of excitation. The polarizations are found to be nonzero in many cases which demonstrate the transfer of coherence through collision processes. A general and compact formula is also derived for the polarization of pure fluorescence where excitation exchange has not taken place. The polarization of the sensitized fluorescence is in general smaller than that of the pure fluorescence. This means that the coherence is transferred only partially. Finally, the magnetic field effect has been included. This field depolarization depends on the ${g}_{j}$ values and the lifetimes of the excited states of both atoms. The general feature of the field dependence also differs considerably from that of the Hanle effect for resonance fluorescence.

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It is pointed out that a recent observation by Gough on the polarization of sensitized fluorescence constitutes an experimental demonstration of the transfer of coherence from mercury to cadmium atoms in collisions of the second kind. The implications of this are discussed.

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Secondary Radiation and Polarization of Resonance Radiation in Cadmium

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Secondary radiation in cadmium vapor containing mercury as an impurity.---Attention is called to the points of difference between the conditions under which the two types of optically excited spectra of mercury vapor appear, namely resonance radiation and fluorescence. In the present experiments it is noted that when a bulb containing cadmium with a slight impurity of mercury is illuminated by light of 2288A wave-length the secondary radiation contains the mercury line 2536.7A in addition to the cadmium lines 2288A and 3261A provided the metal is distilling. As soon as the vapor is stagnant, however, only the cadmium 2288A line appears. The suggestion is made that the phenomenon is due to the presence in the distilling vapor of unstable HgCd molecules. In such a molecule the Cd atom may absorb the 2288A radiation and subsequently in the breakdown of the molecule may excite the Hg atom by a collision of the second kind.Polarization of the cadmium resonance, radiation in zero magnetic field.---The polarization of the cadmium resonance radiation (3261A) in zero magnetic field under certain conditions was found to be 35 percent. In order to explain this value by the kinetic theory, one must assign effective radii to the colliding atoms which are thirty times the radii effective in ordinary collisions.

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The Journal of Chemical Physics•Jan 1, 1970•4 citations

Observation of modulation of mercury-cadmium sensitized fluorescence under the influence of a rotating magnetic field

R S Baker, W Gough

Modulation has been observed in mercury-cadmium sensitized fluorescence under the simultaneous application of a static and a rotating magnetic field. The dependence of the depth of modulation at various frequencies on the static field has been investigated. There are discrepancies between theory and experiment which indicate an anisotropy in the observation of the various collisions. An attempt is made to explain the discrepancies for one particular case on a simple model of the collision, but this attempt is unsuccessful.

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On the influence of magnetic fields on the polarisation of resonance radiation

Robert Williams Wood, A. Ellett

Abstract The emission of polarised light by fluorescent sodium and iodine vapours was discovered by one of the present writers many years ago, and a similar phenomenon was looked for repeatedly, but without success, in the case of the much simpler (presumably) type of emission which occurs when a gas or vapour re-emits without change of wave-length the energy which it abstracts from the incident beam, as when the monochromatic radiation 2536 from a mercury arc traverse as exhausted quartz bulb containing a drop of mercury at room temperature, or the light of a sodium flame falls upon a glass bulb containing highly rarefied sodium vapour. Lord Rayleigh has recently discovered, however, that the resonance radiation of mercury vapour shows fairly strong polarisation, and reported results which apparently indicated that the polarisation becomes stronger as the exciting radiation penetrates to greater and greater depths of the vapour, being practically absent at the point where the radiation enters the bulb or tube. This would mean that polarisation of the light results only when the excitation is, by frequencies, a little out of tune with the natural frequency of the mercury atom, a matter of great theoretical interest. In a report of some work done last year by one of us this last observation of Lord Rayleigh was not confirmed, the polarisation appearing of full strength right up to the entrance window of the exciting beam. A possible explanation of Lord Rayleigh's results will be offered in the present paper in which it will be shown that a very weak magnetic field, properly oriented, destroys completely all traces of polarisation.

Proceedings of the Royal Society of London Series A Containing Papers of a Mathematical and Physical Character•Jun 1, 1923•48 citations
By means of the selection rule Σ m J = constant along the axis of a collision between two atoms, it is shown that sensitized fluorescence should in some cases be partially polarized. The degree of polarization of the fluorescence of cadmium vapour sensitized by the presence of mercury vapour is calculated for certain states of polarization of the incident radiation. In the case studied experimentally the degree of polarization varies over a range of 2-5%. The theoretical value is 3/11, which is reduced in practice by various depolarizing effects. The possibility of transfer coherence between eigenstates from mercury to cadmium during a collision is considered.
Energy transfer and coherence transfer between two atoms of different species are studied theoretically. The electric dipole-dipole interaction is the mechanism considered for the excitation transfer. A generalized perturbation method for a damping system is used. A general formula is derived for the polarization of the sensitized fluorescence resulting from the excitation transfer. This polarization is shown to be dependent on the angular momenta of the two atoms, and to be independent of their relative velocity as well as of their difference in the energy of excitation. The polarizations are found to be nonzero in many cases which demonstrate the transfer of coherence through collision processes. A general and compact formula is also derived for the polarization of pure fluorescence where excitation exchange has not taken place. The polarization of the sensitized fluorescence is in general smaller than that of the pure fluorescence. This means that the coherence is transferred only partially. Finally, the magnetic field effect has been included. This field depolarization depends on the gj{g}_{j}gj​ values and the lifetimes of the excited states of both atoms. The general feature of the field dependence also differs considerably from that of the Hanle effect for resonance fluorescence.
Secondary radiation in cadmium vapor containing mercury as an impurity.---Attention is called to the points of difference between the conditions under which the two types of optically excited spectra of mercury vapor appear, namely resonance radiation and fluorescence. In the present experiments it is noted that when a bulb containing cadmium with a slight impurity of mercury is illuminated by light of 2288A wave-length the secondary radiation contains the mercury line 2536.7A in addition to the cadmium lines 2288A and 3261A provided the metal is distilling. As soon as the vapor is stagnant, however, only the cadmium 2288A line appears. The suggestion is made that the phenomenon is due to the presence in the distilling vapor of unstable HgCd molecules. In such a molecule the Cd atom may absorb the 2288A radiation and subsequently in the breakdown of the molecule may excite the Hg atom by a collision of the second kind.Polarization of the cadmium resonance, radiation in zero magnetic field.---The polarization of the cadmium resonance radiation (3261A) in zero magnetic field under certain conditions was found to be 35 percent. In order to explain this value by the kinetic theory, one must assign effective radii to the colliding atoms which are thirty times the radii effective in ordinary collisions.
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.
Modulation has been observed in mercury-cadmium sensitized fluorescence under the simultaneous application of a static and a rotating magnetic field. The dependence of the depth of modulation at various frequencies on the static field has been investigated. There are discrepancies between theory and experiment which indicate an anisotropy in the observation of the various collisions. An attempt is made to explain the discrepancies for one particular case on a simple model of the collision, but this attempt is unsuccessful.
Abstract The emission of polarised light by fluorescent sodium and iodine vapours was discovered by one of the present writers many years ago, and a similar phenomenon was looked for repeatedly, but without success, in the case of the much simpler (presumably) type of emission which occurs when a gas or vapour re-emits without change of wave-length the energy which it abstracts from the incident beam, as when the monochromatic radiation 2536 from a mercury arc traverse as exhausted quartz bulb containing a drop of mercury at room temperature, or the light of a sodium flame falls upon a glass bulb containing highly rarefied sodium vapour. Lord Rayleigh has recently discovered, however, that the resonance radiation of mercury vapour shows fairly strong polarisation, and reported results which apparently indicated that the polarisation becomes stronger as the exciting radiation penetrates to greater and greater depths of the vapour, being practically absent at the point where the radiation enters the bulb or tube. This would mean that polarisation of the light results only when the excitation is, by frequencies, a little out of tune with the natural frequency of the mercury atom, a matter of great theoretical interest. In a report of some work done last year by one of us this last observation of Lord Rayleigh was not confirmed, the polarisation appearing of full strength right up to the entrance window of the exciting beam. A possible explanation of Lord Rayleigh's results will be offered in the present paper in which it will be shown that a very weak magnetic field, properly oriented, destroys completely all traces of polarisation.