High harmonic generation (HHG) in solids has been identified as a promising mechanism for light source generation and for spectroscopy of materials. HHG from bulk solids, however, often suffers from nonlinear propagation effects, resulting in a loss of spectral coherence and the skewing of spectroscopic measurements. Here, we study HHG in epitaxial ZnO thin films grown on Al2O3substrates using atomic layer deposition. We find that the HHG emission consists of narrow spectral peaks, in contrast to those seen in bulk, and that the dependence of the harmonic yield on the film thickness differs for above-gap and below-gap harmonics, which can be understood from analytical models based on the linear and nonlinear response of the medium. The measured harmonic spectra depend qualitatively on the preparation of the films, with as-grown films generating even harmonic orders, which are absent in annealed films. The results are interpreted using transmission electron microscopy measurements, which indicate different morphologies for the as-grown and annealed films.
- Award ID(s):
- 1719875
- PAR ID:
- 10325367
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Many-body effects play an important role in enhancing and modifying optical absorption and other excited-state properties of solids in the perturbative regime, but their role in high harmonic generation (HHG) and other nonlinear response beyond the perturbative regime is not well-understood. We develop here an ab initio many-body method to study nonperturbative HHG based on the real-time propagation of the non-equilibrium Green’s function with the GW self energy. We calculate the HHG of monolayer MoS2and obtain good agreement with experiment, including the reproduction of characteristic patterns of monotonic and nonmonotonic harmonic yield in the parallel and perpendicular responses, respectively. Here, we show that many-body effects are especially important to accurately reproduce the spectral features in the perpendicular response, which reflect a complex interplay of electron-hole interactions (or exciton effects) in tandem with the many-body renormalization and Berry curvature of the independent quasiparticle bandstructure.
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High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8
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Vigorous efforts to harness the topological properties of light have enabled a multitude of novel applications. Translating the applications of structured light to higher spatial and temporal resolutions mandates their controlled generation, manipulation, and thorough characterization in the short-wavelength regime. Here, we resort to high-order harmonic generation (HHG) in a noble gas to upconvert near-infrared (IR) vector, vortex, and vector-vortex driving beams that are tailored, respectively, in their spin angular momentum (SAM), orbital angular momentum (OAM), and simultaneously in their SAM and OAM. We show that HHG enables the controlled generation of extreme-ultraviolet (EUV) vector beams exhibiting various spatially dependent polarization distributions, or EUV vortex beams with a highly twisted phase. Moreover, we demonstrate the generation of EUV vector-vortex beams (VVB) bearing combined characteristics of vector and vortex beams. We rely on EUV wavefront sensing to unambiguously affirm the topological charge scaling of the HHG beams with the harmonic order. Interestingly, our work shows that HHG allows for a synchronous controlled manipulation of SAM and OAM. These EUV structured beams bring in the promising scenario of their applications at nanometric spatial and sub-femtosecond temporal resolutions using a table-top harmonic source.more » « less
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41467-021-24450-9
