Interplay between high-harmonic generation and photoluminescence in ZnO: Anisotropic spectral properties of harmonic emission and the role of excitons

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Abstract
We investigate the nonlinear optical response of bulk ZnO under intense short-wave infrared excitation, focusing on the interplay between high-harmonic generation (HHG) and photoluminescence (PL). While HHG exhibits nonperturbative intensity scaling and a spectral blueshift consistent with plasma-induced refractive index changes, the PL signal shows a pronounced superlinear increase and a redshift, attributed to a combination of exciton-exciton scattering and phonon-assisted exciton recombination emission. A similar PL response under above-bandgap excitation supports its intrinsic origin. Spectral analysis of the HHG emission reveals an intensity-driven transition in the characteristics of the fifth harmonic, indicating a change in the underlying generation mechanism. These findings establish PL and spectral HHG analysis as complementary probes of strong-field and many-body effects in wide-bandgap semiconductors.
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