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

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Main Authors: Jessen, Simon P. S., Mero, Mark, Vrakking, Marc J. J., Turtos, Rosana M., Balling, Peter, Jürgens, Peter
Format: Preprint
Published: 2025
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author Jessen, Simon P. S.
Mero, Mark
Vrakking, Marc J. J.
Turtos, Rosana M.
Balling, Peter
Jürgens, Peter
author_facet Jessen, Simon P. S.
Mero, Mark
Vrakking, Marc J. J.
Turtos, Rosana M.
Balling, Peter
Jürgens, Peter
contents 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 non-perturbative 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.
format Preprint
id arxiv_https___arxiv_org_abs_2508_09364
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle The interplay between high-harmonic generation and photoluminescence in ZnO: Anisotropic spectral properties of harmonic emission and the role of excitons
Jessen, Simon P. S.
Mero, Mark
Vrakking, Marc J. J.
Turtos, Rosana M.
Balling, Peter
Jürgens, Peter
Optics
Atomic Physics
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 non-perturbative 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.
title The interplay between high-harmonic generation and photoluminescence in ZnO: Anisotropic spectral properties of harmonic emission and the role of excitons
topic Optics
Atomic Physics
url https://arxiv.org/abs/2508.09364