Abstract

In pursuit of efficient high-order harmonic conversion in semiconductor devices, modeling insights into the complex interplay among ultrafast microscopic electron–hole dynamics, nonlinear pulse propagation, and field confinement in nanostructured materials are urgently needed. Here, a self-consistent approach coupling semiconductor Bloch and Maxwell equations is applied to compute transmission and reflection high-order harmonic spectra for finite slab and sub-wavelength nanoparticle geometries. An increase in the generated high harmonics by several orders of magnitude is predicted for gallium arsenide nanoparticles with a size maximizing the magnetic dipole resonance. Serving as a conceptual and predictive tool for ultrafast spatiotemporal nonlinear optical responses of nanostructures with arbitrary geometry, our approach is anticipated to deliver new strategies for optimal harmonic manipulation in semiconductor metadevices.

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