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arXiv:1210.7285

Nonlinear optical anisotropy due to freed electrons

Jonathan Andreasen, Ewan M. Wright, Miroslav Kolesik

Published Oct 27, 2012• 0 citations
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Abstract

We present a computational study of the pump-probe response of a single atom to assess any microscopic nonlinear optical anisotropy due to freed electrons for non-resonant optical excitation. Using simulations of the Schrödinger equation for an atom exposed to a strong, short-duration linearly polarized pump, we calculate the induced dipole moment along probe directions parallel and perpendicular to the pump polarization. Our simulations show birefringence ratios of approximately 0.78-0.9 on the timescale of tens of femtoseconds following the excitation pulse.

DOI
10.48550/arxiv.1210.7285

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We present a computational study of the pump-probe response of a single atom to assess any microscopic nonlinear optical anisotropy due to freed electrons for non-resonant optical excitation. Using simulations of the Schrödinger equation for an atom exposed to a strong, short-duration linearly polarized pump, we calculate the induced dipole moment along probe directions parallel and perpendicular to the pump polarization. Our simulations show birefringence ratios of approximately 0.78-0.9 on the timescale of tens of femtoseconds following the excitation pulse.
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Polarization response that appears in silver vapors in the field of a high-intensity femtosecond Ti:sapphire laser has been studied by the direct numerical integration of the time-dependent Schrödinger equation. The regions of applicability have been determined for perturbation theory and the power series expansion of the polarization in the field. The contribution of free electrons to the response at the frequency of the interacting field has been calculated, which is due to the photoionization process and limits the Kerr effect. An important contribution of laser-excited atomic states to nonlinear atomic responses of neutral atoms has been demonstrated.
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We present a theoretical study of the induced transient birefringence of a low density homogeneous molecular gas in a resonant pump–probe experiment. The molecular coherent state induced by the resonant pump field is described by second-order perturbation theory. The induced birefringence can be detected by a delayed probe pulse propagating through the molecular medium after illumination by the pump pulse. In the case of a nonresonant probe, the birefringence is linearly proportional to the mean value of the electronic polarizability of the molecular gas. The birefringence signal is composed of distinct components due to population change and those of rotational, vibrational, and mixed vibrational–rotational origins. This is demonstrated by numerical simulations on Li2 gas. Moreover, the quantum beats contained in the birefringence, as a function of the time delay between the pump and probe pulses, is dominated by the pure rotational motion. Finally, the birefringence is sensitive to the shape of the applied pump pulse and dependent on the spectral phase of the pump pulse.