Abstract :
[en] We develop a general, fully quantum mechanical theory of Raman scattering from first principles in terms of many-body correlation functions. In order to arrive at expressions that are practically useful in the context of condensed matter physics, we adopt the Lehmann-Symanzik-Zimmermann reduction formula from high-energy physics and formulate it in the language of many-body perturbation theory. This enables us to derive a general and practically useful expression for the Raman scattering rate in terms of quantities that can be computed ab initio. Our work paves the way toward a comprehensive computational approach to the calculation of Raman spectra that goes beyond the current state of the art by capturing both excitonic and nonadiabatic effects.
Commentary :
The authors would like to thank A. Marini for initial inspiring discussions as well as M. Sadhukhan and Y. Al-Hamdani for helpful discussions during the revision of the manuscript. S.R. and L.W. acknowledge financial support by the National Research Fund (FNR) Luxembourg (Projects RAMGRASEA and INTER/ANR/13/20/NANOTMD). S. R. also acknowledges financial support by the Leverhulme Trust (Grant No. RL-2012-001).
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