Real-time ab initio description of the photon-echo mechanisms in extended systems: the case study of bulk GaAs

Abstract

In this paper we present an ab initio real-time analysis of free polarization decay and photon echo in extended systems. As a prototype material, we study bulk GaAs driven by ultra-short laser pulses of 10 fs (energy spread of 0.4 eV), with frequency tuned in the continuum of the optical spectrum. We compute the electronic polarization P(t), and define a computational procedure to extract the echo signal in the dipole approximation. Results are obtained in both the low and high field regime, and compared with a two-levels system (TLS) model, with parameters extracted from the ab initio simulations. ab initio results are in optimal agreement with the TLS in the low-field case, whereas some differences are observed in the high-field regime where the multi-band nature of GaAs becomes relevant. In the high field regime we compute the pulse area, and look for fluences with pulse area close to π. We highlight that such fluences are well below the damage threshold of GaAs. However a unique value of the area cannot be defined, due to the strong dependence of the transition dipoles in the energy window excited by the laser pulse.

arXiv comment12 pages, 7 figures

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