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Reviews of Modern Physics

Scattering Theory of Absorption-Line Profiles and Refractivity

Bruce W. Shore

Published Apr 1, 1967• 218 citations
Publisher

Abstract

Attenuation processes are examined from the viewpoint of collision theory, and the optical theorem is used to connect attenuation cross section $\ensuremath{\sigma}$ and refractive index $n$ with diagonal elements of the $T$ matrix. This approach provides resonance profiles (for "natural" lines shapes) of the form $\ensuremath{\sigma}(\ensuremath{\omega})=C+\frac{(\frac{\ensuremath{\Gamma}}{2})B+(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})A}{{(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})}^{2}+{(\frac{\ensuremath{\Gamma}}{2})}^{2}},$ $n(\ensuremath{\omega})\ensuremath{-}1=\frac{\mathrm{Nc}}{2\ensuremath{\omega}}\left[\frac{(\frac{\ensuremath{\Gamma}}{2})A\ensuremath{-}(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})B}{{(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})}^{2}+{(\frac{\ensuremath{\Gamma}}{2})}^{2}}\ensuremath{-}D\right],$ where the profile parameters $A$, $B$, $C$, $D$, $\ensuremath{\Gamma}$, ${\ensuremath{\omega}}_{0}$ are given in terms of atomic matrix elements.Part I reviews the notion of resonances. Part II summarizes the relevant results of collision theory, stressing physical interpretation, and gives a definition for excited (or resonance) states based on a simple partition of basis states into two classes. Part III applies perturbation theory to the calculation of resonance profiles. Part IV applies these results specifically to the attenuation and refraction of photons by tenuous gases, with particular attention paid to the profiles of autoionizing lines. The effects of degeneracy (the extension of the bound-state ${Z}^{\ensuremath{-}1}$ expansion theory) are noted.

DOI
10.1103/revmodphys.39.439

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American Journal of Physics•Feb 1, 1983•1 citation
Attenuation processes are examined from the viewpoint of collision theory, and the optical theorem is used to connect attenuation cross section \ensuremathσ\ensuremath{\sigma}\ensuremathσ and refractive index nnn with diagonal elements of the TTT matrix. This approach provides resonance profiles (for "natural" lines shapes) of the form \ensuremathσ(\ensuremathω)=C+(\ensuremathΓ2)B+(\ensuremathω\ensuremath−\ensuremathω0)A(\ensuremathω\ensuremath−\ensuremathω0)2+(\ensuremathΓ2)2,\ensuremath{\sigma}(\ensuremath{\omega})=C+\frac{(\frac{\ensuremath{\Gamma}}{2})B+(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})A}{{(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})}^{2}+{(\frac{\ensuremath{\Gamma}}{2})}^{2}},\ensuremathσ(\ensuremathω)=C+(\ensuremathω\ensuremath−\ensuremathω0​)2+(2\ensuremathΓ​)2(2\ensuremathΓ​)B+(\ensuremathω\ensuremath−\ensuremathω0​)A​, n(\ensuremathω)\ensuremath−1=Nc2\ensuremathω[(\ensuremathΓ2)A\ensuremath−(\ensuremathω\ensuremath−\ensuremathω0)B(\ensuremathω\ensuremath−\ensuremathω0)2+(\ensuremathΓ2)2\ensuremath−D],n(\ensuremath{\omega})\ensuremath{-}1=\frac{\mathrm{Nc}}{2\ensuremath{\omega}}\left[\frac{(\frac{\ensuremath{\Gamma}}{2})A\ensuremath{-}(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})B}{{(\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{0})}^{2}+{(\frac{\ensuremath{\Gamma}}{2})}^{2}}\ensuremath{-}D\right],n(\ensuremathω)\ensuremath−1=2\ensuremathωNc​[(\ensuremathω\ensuremath−\ensuremathω0​)2+(2\ensuremathΓ​)2(2\ensuremathΓ​)A\ensuremath−(\ensuremathω\ensuremath−\ensuremathω0​)B​\ensuremath−D], where the profile parameters AAA, BBB, CCC, DDD, \ensuremathΓ\ensuremath{\Gamma}\ensuremathΓ, \ensuremathω0{\ensuremath{\omega}}_{0}\ensuremathω0​ are given in terms of atomic matrix elements.Part I reviews the notion of resonances. Part II summarizes the relevant results of collision theory, stressing physical interpretation, and gives a definition for excited (or resonance) states based on a simple partition of basis states into two classes. Part III applies perturbation theory to the calculation of resonance profiles. Part IV applies these results specifically to the attenuation and refraction of photons by tenuous gases, with particular attention paid to the profiles of autoionizing lines. The effects of degeneracy (the extension of the bound-state Z\ensuremath−1{Z}^{\ensuremath{-}1}Z\ensuremath−1 expansion theory) are noted.
This paper examines attenuation processes from t h e view- point of c o l l i s i o n theory, using the o p t i c a l theorem t o connect c a t t e n u a t i o n cross-section CJ and r e f r a c t i v i t y n with diagonal elements of the T matrix.This approach provides resonance prof i l e s (for '*natural*' l i n e s shapes) of the form where t h e p r o f i l e parameters A, B, C , D, r, w 0 are given i n t e r m s of atomic matrix elements.P a r t I reviews the notion of resonances.Part I1 summarizes the r e l e v a n t r e s u l t s of c o l l i s i o n theory, s t r e s s i n g physical ' 1
A general theory of line broadening is used to study the effects of collisions on absorption line shapes when self-broadening is important. Special attention is focused on the role of processes in which an excited atom transfers its electronic excitation to an unexcited atom; it is this process which distinguishes self-broadening from foreign-gas broadening. Several forms for the absorption rate are presented corresponding to particular assumptions about the amplitudes associated with this phenomenon. For example, one approximation leads to a generalized Lorentz-Lorenz law in which the one-atom polarizability is replaced by one that accounts for line broadening. Finally, the importance of many-body effects in the calculation of the linewidth is briefly discussed to determine when simple impact theories are applicable.
The work of two previous papers is extended and a theory of pressure broadening is developed which treats the perturbers quantum mechanically and allows for inelastic collisions, degeneracy, and overlapping lines. The impact approximation is used. It consists in assuming that it takes, on the average, many collisions to produce an appreciable disturbance in the wave function of the atom, and it results in an isolated line having a Lorentz shape. Validity criteria are given. When the approximation is valid, it is allowable to replace the exact, fluctuating interaction of the perturbers with the atom by a constant effective interaction. The effective interaction is expressed in terms of the one-perturber quantum mechanical transition amplitudes on and near the energy shell and its close relationship to the scattering matrix is stressed. The calculation of the line shape in terms of the effective interaction is the same as when the perturbers move on classical paths. Results are written explicitly for isolated lines. If the interaction of the perturbers with the final state can be neglected, the shift and width are proportional to the real and imaginary part of the forward elastic scattering amplitude, respectively. By the optical theorem, the width can also be written in terms of the total cross section. When the interaction in the final state cannot be neglected, the shift and width are still given in terms of the elastic scattering amplitudes, in a slightly more complicated fashion. Finally, rules are given for taking into account rotational degeneracy of the radiating states.
I recent years, significant attention has been given to nonlinear optical phenomena, such as nonlinear optical absorption and dispersion, derived from a driven quantum transition of semiconductor nanostructures, such as semiconductor quantum wells, quantum disks and mainly quantum dots. An important issue that is widely studied is the effect of probe electromagnetic field intensity on the total (nonlinear) absorption coefficient and on the total (nonlinear) index of refraction. Some of the phenomena that are commonly found for large electromagnetic field intensities are the creation of a strong dip in the absorption spectrum near or at resonance (the so-called bleaching effect), negative absorption near or at resonance that leads to optical gain and the change of the slope of the total index of refraction near or at resonance from negative to positive that changes the behavior of the system from fast to slow light. Unfortunately, these phenomena do not exist and are artifacts of a common abuse of the theoretical methodology for the study of the total absorption coefficient and the total index of refraction. The main error is that the total absorption coefficient and the total index of refraction was initially derived from density matrix equations using perturbation theory and includes first-order (linear) as well as third-order (nonlinear) terms. This method gives correct results for small electromagnetic field intensities and it leads to saturation of absorption and dispersion in this regime. However, for larger intensities it gives the misleading results mentioned above due to either failure of the order of perturbation theory considered in the derivation of the total absorption coefficient and the total index of refraction or even failure of perturbation theory at all in the treatment of the problem. In this work, we revisit the problem of the total absorption coefficient and the total index of refraction in a symmetric semiconductor quantum dot structure (we choose the example of a core-shell quantum dot) under a strong probe field excitation. We use the two-level model, solve the relevant density matrix equations under the rotating wave approximation and under steady state conditions, and obtain the correct form of the nonlinear optical susceptibility that is then used for the derivation of the formulae of the total absorption coefficient and the total index of refraction under the interaction with a strong probe field. Actually, the commonly used perturbation theory formulae can be obtained by our formulae using a series expansion and keeping terms up to second order in electric field amplitude. We also derive the electronic structure of the quantum dot system by solving numerically the time-independent Schrodinger equation, under the effective mass approximation, using the potential morphing method and obtain the energy difference and the electric dipole matrix element for the relevant transitions of the quantum dot system. Then, for the specific quantum dot system we compare the results of the total absorption coefficient and the total index of refraction for the two methodologies (the perturbation result and our result) for different electromagnetic field intensities.