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The electric field of an intense laser pulse can directly modify the electronic properties of materials via electromodulation up to the petahertz regime. In this regime, the energy of the quiver motion of the electron-hole pair is comparable with the photon energy, which results in complex nonadiabatic dynamics. This regime opens opportunities to probe the electronic structure of materials on the attosecond timescale. Here, we show how the quasistatic electromodulation spectroscopy based on the Franz-Keldysh effect (FKE) connects with its nonadiabatic limit, which we find to be determined by resonant transitions between Floquet-Bloch states. This insight can be applied to measure the effective mass, ponderomotive and binding energies of the electron-hole pair on a few-femtosecond timescale. We demonstrate this by experimentally investigating laser-field-driven fused silica, a prototypical material for light-wave electronics, with extreme-ultraviolet attosecond pulse trains. We reproduce the experimental transient absorption spectra with an effective band structure and a dynamical Franz-Keldysh model, offering a simple parametrization for a theoretically challenging but technologically abundant material. Ab initio calculations in α-quartz highlight the contributions of specific bands, symmetry, and crystal orientation that are hidden in the experimental data due to randomized crystallographic orientation and finite temporal and spatial coherence. We show that the dynamical FKE can be explained as a third-order nonlinear process in the weak-field regime. The delay-dependent position of the absorption maxima and minima has a minimum tilt angle, determined by transitions between the underlying Floquet-Bloch states. In our analysis, we discuss the main experimental observables and show their connection to the parameters of the solid, providing the basis for nonadiabatic electromodulation spectroscopy. ISSN:1098-0121 ISSN:0163-1829 ISSN:1550-235X ISSN:0556-2805 ISSN:2469-9969 ISSN:1095-3795 ISSN:2469-9950

Transition metals with their densely confined and strongly coupled valence electrons are key constituents of many materials with unconventional properties, such as high-Tc superconductors, Mott insulators and transition-metal dichalcogenides. Strong electron interaction offers a fast and efficient lever to manipulate their properties with light, creating promising potential for next-generation electronics. However, the underlying dynamics is a fast and intricate interplay of polarization and screening effects, which is poorly understood. It is hidden below the femtosecond timescale of electronic thermalization, which follows the light-induced excitation. Here, we investigate the many-body electron dynamics in transition metals before thermalization sets in. We combine the sensitivity of intra-shell transitions to screening effects with attosecond time resolution to uncover the interplay of photo-absorption and screening. First-principles time-dependent calculations allow us to assign our experimental observations to ultrafast electronic localization on d-orbitals. The latter modifies the whole electronic structure as well as the collective dynamic response of the system on a timescale much faster than the light-field cycle. Our results demonstrate a possibility for steering the electronic properties of solids prior to electron thermalization, suggesting that the ultimate speed of electronic phase transitions is limited only by the duration of the controlling laser pulse. Furthermore, external control of the local electronic density serves as a fine tool for testing state-of-the art models of electron-electron interactions. We anticipate our study to facilitate further investigations of electronic phase transitions, laser-metal interactions and photo-absorption in correlated electron systems on its natural timescale.

High Harmonic generation can be used as a probe of the emitting medium with attosecond and Angstrom resolutions. We show that polarization-resolved pump-probe spectroscopy with high harmonics improves the detection sensitivity of rotationally excited molecules.

We investigate the influence of microscopic and macroscopic ionization effects on the intensity-dependent quantum-path interferences in high-harmonic generation. The resulting interference structures were analyzed in different gases and in spatially resolved harmonic spectra. © 2009 Optical Society of America.

The interference between the emission originating from the short and long electron quantum paths is intrinsic to the high harmonic generation process. We investigate the universal properties of these quantum-path interferences in various generation media and discuss how ionization effects influence the observed interference structures. Our comparison of quantum-path interferences observed in xenon, argon, and neon demonstrates that our experimental tools are generally applicable and should also allow investigating more complex systems such as molecules or clusters.