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Il Nuovo cimento della Società italiana di fisica. B/Il Nuovo cimento B

Radiative and relaxation effects on line shape

ADRIANO DI GIACOMO, F. Feo

Published Feb 1, 1975• 2 citations
Publisher
DOI
10.1007/bf02724748

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In the limit of a dipole-dipole interaction between neutral atoms and the binary-collision approximation, we present a theory of pressure broadening in which the multiplet structure of the atomic levels is considered. The appropriate Schr\"odinger equations for the collision problem are numerically integrated to obtain solutions for both resonant and foreign gas broadening. The presence of radiation fields is neglected in the first half of the paper, where the collisional time rate of change of the density matrix is found. The pertinent collisional decay parameters are extracted from these equations. The ratios of the parameters of the average magnetic dipole to electric quadrupole moment obtained were 1.21\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the entire ensemble in resonant broadening, 0.966\ifmmode\pm\else\textpm\fi{}0.012 for the relaxation of the initially excited atoms in resonant broadening, and 1.12\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the initially excited atoms in foreign gas broadening. In the second half of the paper, the collisional broadening results are incorporated in a systematic evaluation of (i) spectral profiels (effects arising from the velocity and recoil of the emitting atom are neglected), (ii) Hanle-effect line shapes, and (iii) laser phenomena. For the case of resonant broadening, the radiation trapping process is reviewed and its influence on line shapes discussed. Finally, a detailed comparison of the theory with experimental findings as well as with previous theoretical results is made. We conclude that the dipole-dipole interaction is sufficient to explain most cases of resonant and some cases of foreign gas broadening.

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It has been postulated that the state function can be expressed as a linear superposition of eigenstates of Hermitian operators. When a system is subjected to an external impulse in the form of radiation, the probability of finding the system in different eigenstates of the state function changes. The total probability is always unity, which means the change in probabilities for different states occurs at the expense of each other. This change in probability of finding the system in different eigenstates brought about by system-radiation interaction is called the spectroscopic transition. Here, we use a two-level system to develop the details of a general spectroscopic transition, and work further to examine the effects of interruption in the coherent evolution of the state function. The physical meaning of absorption coefficient is discussed in detail. We derive the general forms of relaxation of the excited state, spectral line shape, and line broadening. The origin and the meaning of homogeneous and inhomogeneous line broadening are discussed. We describe the Doppler effect and its use in the interpretation of inhomogeneous line shape.

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Radiative transitions

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In the limit of a dipole-dipole interaction between neutral atoms and the binary-collision approximation, we present a theory of pressure broadening in which the multiplet structure of the atomic levels is considered. The appropriate Schr\"odinger equations for the collision problem are numerically integrated to obtain solutions for both resonant and foreign gas broadening. The presence of radiation fields is neglected in the first half of the paper, where the collisional time rate of change of the density matrix is found. The pertinent collisional decay parameters are extracted from these equations. The ratios of the parameters of the average magnetic dipole to electric quadrupole moment obtained were 1.21\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the entire ensemble in resonant broadening, 0.966\ifmmode\pm\else\textpm\fi{}0.012 for the relaxation of the initially excited atoms in resonant broadening, and 1.12\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the initially excited atoms in foreign gas broadening. In the second half of the paper, the collisional broadening results are incorporated in a systematic evaluation of (i) spectral profiels (effects arising from the velocity and recoil of the emitting atom are neglected), (ii) Hanle-effect line shapes, and (iii) laser phenomena. For the case of resonant broadening, the radiation trapping process is reviewed and its influence on line shapes discussed. Finally, a detailed comparison of the theory with experimental findings as well as with previous theoretical results is made. We conclude that the dipole-dipole interaction is sufficient to explain most cases of resonant and some cases of foreign gas broadening.
It has been postulated that the state function can be expressed as a linear superposition of eigenstates of Hermitian operators. When a system is subjected to an external impulse in the form of radiation, the probability of finding the system in different eigenstates of the state function changes. The total probability is always unity, which means the change in probabilities for different states occurs at the expense of each other. This change in probability of finding the system in different eigenstates brought about by system-radiation interaction is called the spectroscopic transition. Here, we use a two-level system to develop the details of a general spectroscopic transition, and work further to examine the effects of interruption in the coherent evolution of the state function. The physical meaning of absorption coefficient is discussed in detail. We derive the general forms of relaxation of the excited state, spectral line shape, and line broadening. The origin and the meaning of homogeneous and inhomogeneous line broadening are discussed. We describe the Doppler effect and its use in the interpretation of inhomogeneous line shape.