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Register a new userPhotoionization and transient Wannier-Stark ladder in silicon: First principle simulations versus Keldysh theory
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Added by
Thibault J.Y. Derrien
Publication date
2021
fields
Physics
and research's language is
English
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Nonlinear photoionization of dielectrics and semiconductors is widely treated in the frames of the Keldysh theory whose validity is limited to small photon energies compared to the band gap and relatively low laser intensities. The time-dependent density functional theory (TDDFT) simulations, which are free of these limitations, enable to gain insight into non-equilibrium dynamics of the electronic structure. Here we apply the TDDFT to investigate photoionization of silicon crystal by ultrashort laser pulses in a wide range of laser wavelengths and intensities and compare the results with predictions of the Keldysh theory. Photoionization rates derived from the simulations considerably exceed the data obtained with the Keldysh theory within the validity range of the latter. Possible reasons of the discrepancy are discussed and we provide fundamental data on the photoionization rates beyond the limits of the Keldysh theory. By investigating the features of the Stark shift as a function of photon energy and laser field strength, a manifestation of the transient Wannier-Stark ladder states have been revealed which become blurred with increasing laser field strength. Finally, it is shown that the TDDFT simulations can potentially provide reliable data on the electron damping time that is of high importance for large-scale modeling.
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We provide a nonperturbative theory for photoionization of transparent solids. By applying a particular steepest-descent method, we derive analytical expressions for the photoionization rate within the two-band structure model, which consistently account for the $selection$ $rules$ related to the parity of the number of absorbed photons ($odd$ or $even$). We demonstrate the crucial role of the interference of the transition amplitudes (saddle-points), which in the semi-classical limit, can be interpreted in terms of interfering quantum trajectories. Keldyshs foundational work of laser physics [Sov. Phys. JETP 20, 1307 (1965)] disregarded this interference, resulting in the violation of $selection$ $rules$. We provide an improved Keldysh photoionization theory and show its excellent agreement with measurements for the frequency dependence of the two-photon absorption and nonlinear refractive index coefficients in dielectrics.
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