Tailored pump-probe transient spectroscopy with time-dependent density-functional theory: controlling absorption spectra

Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use of tailored pumps in order to enhance (or reduce) some given features of the probe absorption (for example, absorption in the visible range of otherwise transparent samples). This type of manipulation of the system response could be helpful for its full characterization, since it would allow us to visualize transitions that are dark when using unshaped pulses. In order to investigate these possibilities, we perform first a theoretical analysis of the non-equilibrium response function in this context, aided by one simple numerical model of the hydrogen atom. Then, we proceed to investigate the feasibility of using time-dependent density-functional theory as a means to implement, theoretically, this absorption-optimization idea, for more complex atoms or molecules. We conclude that the proposed idea could in principle be brought to the laboratory: tailored pump pulses can excite systems into light-absorbing states. However, we also highlight the severe numerical and theoretical difficulties posed by the problem: large-scale non-equilibrium quantum dynamics are cumbersome, even with TDDFT, and the shortcomings of state-of-the-art TDDFT functionals may still be serious for these out-of-equilibrium situations.     

Ab initio description of the first stages of laser-induced ultra-fast nonthermal melting of InSb

Using first principles, all-electron calculations and dynamical simulations we study the behavior of solid InSb immediately after intense femtosecond excitation. First, we determine the laser-excited potential energy surfaces with high accuracy for different electronic temperatures (corresponding to different laser fluences). Then, we demonstrate that, although most phonon modes become only slightly softened even for high electron temperatures, the transverse acoustic modes at the boundary of the Brillouin zone undergo dramatic changes and become unstable. This is the origin of nonthermal melting. Based on these results, the dynamics during the first hundreds of femtoseconds after laser excitation can be unambiguously elucidated. Our results are in agreement with recent experiments and support the predictions made by Stampfli and Bennemann for silicon.     

Anharmonic noninertial lattice dynamics during ultrafast nonthermal melting of InSb

We compute the potential energy surface of femtosecond-laser-excited InSb along the directions in which the crystal becomes soft. Using dynamical simulations the time dependence of the atomic coordinates is obtained. We find that at high excitation densities the anharmonicity of the potential energy surface becomes significant after approximately 100 fs. On the basis of our results we explain recent time-resolved x-ray diffraction experiments. We point out that an alternative model for ultrafast melting [A. M. Lindenberg, Science 308, 392 (2005)] is inconsistent with our calculations.