High harmonic generation (HHG) from solids shows great application prospects in compact short-wavelength light sources and as a tool for imaging the dynamics in crystals with subnanometer spatial and attosecond temporal resolution. However, the underlying collision dynamics behind solid HHG is still intensively debated and no direct mapping relationship between the collision dynamics with band structure has been built. Here, we show that the electron and its associated hole can be elastically scattered by neighboring atoms when their wavelength approaches the atomic size. We reveal that the elastic scattering of electron/hole from neighboring atoms can dramatically influence the electron recombination with its left-behind hole, which turns out to be the fundamental reason for the anisotropic interband HHG observed recently in bulk crystals. Our findings link the electron/hole backward scattering with Van Hove singularities and forward scattering with critical lines in the band structure and thus build a clear mapping between the band structure and the harmonic spectrum. Our work provides a unifying picture for several seemingly unrelated experimental observations and theoretical predictions, including the anisotropic harmonic emission in MgO, the atomic-like recollision mechanism of solid HHG, and the delocalization of HHG in ZnO. This strongly improved understanding will pave the way for controlling the solid-state HHG and visualizing the structure-dependent electron dynamics in solids.
We investigate the transient optical response in high-quality Cd 0.88 Zn 0.12 Te crystals in the regime of slow light propagation on the lower exciton-polariton branch. Femtosecond photoexcitation leads to very substantial transmission changes in a ∼10-meV broad spectral range within the transparency window of the unexcited semiconductor. These nonlinear optical signatures decay on picosecond time scales governed by carrier thermalization and recombination. The temporal and spectral dependence indicate the dynamical optical response as arising from excitation-induced dephasing and perturbed free induction decay. Model simulations for the optical response taking into account the actual exciton-polariton dispersion and excitation-induced dephasing of a nonlinearly driven two-level system support this interpretation.
We report on ultrafast time-resolved pump-probe studies in a CdZnTe/CdMgTe planar guiding structure covered with a metallic grating. The one-dimensional periodic gold structure allows for efficient coupling into the guiding layer for p-polarized 30 fs optical pulses with a large spectral bandwidth of about 60 nm. The resulting spectral width of optical pulses propagating inside the guiding layer corresponds to 20-30 nm. We demonstrate that the excitation of exciton-polariton modes in the guiding layer leads to a modulation of the optical response in the vicinity of the excitonic resonance. Spatially resolved pump-probe measurements show an asymmetric behavior in the optical response when the relative position of the pump and probe spots is varied on the scale of ten micrometers perpendicular to the metal ridges. This is attributed to the excitation of resonant and off-resonant exciton-polariton modes which propagate in opposite directions inside the guiding layer in accordance with their dispersion relations. Two main mechanisms are considered and evaluated, namely, Pauli blocking and excitation-induced dephasing, which are shown to be responsible for the pump-induced changes in the exciton absorption spectrum. While both of these processes lead to the generation of photoexcited carriers in the guiding layer, their impact on the optical properties (transmission and reflection) are different which leads to the asymmetric behavior of the spatially resolved transients.
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