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Radiation Physics and Chemistry

Photon absorption and photon scattering—What we do not know and why it matters

Richard H. Pratt

Published Oct 31, 2013• 18 citations
Publisher
DOI
10.1016/j.radphyschem.2013.10.018

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Introduction Engineers who design transistors, lasers and other semiconductor components want to understand and control the cause of resistance to current flow so that they may better optimize device performance. A detailed microscopic understanding of electron motion from one part of a semiconductor to another requires the explicit calculation of electron scattering probability. One would like to know how to predict electron scattering from one state to another. In this chapter we will see how to do this using powerful quantummechanical techniques. In addition to understanding electron motion in a semiconductor we also want to understand how to make devices that emit or absorb light. In Chapter 6 it was shown that a superposition of two harmonic oscillator eigenstates could give rise to dipole radiation and emission of a photon. The creation of a photon was only possible if a superposition state existed between a correct pair of eigenstates. This leads directly to the concept of rules determining pairs of eigenstates which can give rise to photon emission. Such selection rules are a useful tool to help us understand the emission and absorption of light by matter. However, the real challenge is to use what we know to make practical devices which operate using emission and absorption of photons. This usually requires imposing some control over atomic-scale physical processes which, of course, can only be understood using quantum mechanics.
This chapter focuses on absorption. Absorption has been called the “death of photons.” While the energy of a photon is never truly lost, most people find the conversion of photons into heat and chemical reactions less appealing than their original emission. However, without absorption, the earth would be a far less colorful place, with no paintings, flowers, leopard spots, or stained-glass windows. There would still be some colors due to interference and scattering, but people would be blind to them because human vision is based on absorption. More importantly, if nothing on earth absorbed light, the planet would be lifeless and cold. Understanding absorption helps one understand all the interactions of light with matter.
The frequency-domain pump-probe signal of a material system interacting with two quantum modes of the radiation field is recast in terms of products of scattering amplitudes (T matrix elements) rather than the third-order susceptibility Im chi((3)). The resulting expression offers a more intuitive physical picture for the optical process compared with the semiclassical approach which treats the radiation field as classical. It can be derived and interpreted using closed-time-path-loop diagrams which represent the joint state of the matter and the field for each contribution to the signal. The signal has two components representing stimulated Raman scattering omega(1) - omega(2) and two-photon absorption omega(1) + omega(2) two-photon resonances. Both are expressed as nonequi-librium steady-state photon and matter fluxes, as is common in the description of dissipative processes in open quantum systems.