Enhanced high harmonic efficiency through phonon-assisted photodoping effect

High-harmonic generation (HHG) has emerged as a central technique in attosecond science and strong-field physics, providing a tool for investigating ultrafast dynamics. However, the microscopic mechanism of HHG in solids is still under debate, and it is unclear how it is modified in the ubiquitous p...

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Bibliographic Details
Published in:npj computational materials 2024-09, Vol.10 (1), p.202-7, Article 202
Main Authors: Zhang, Jin, Neufeld, Ofer, Tancogne-Dejean, Nicolas, Lu, I-Te, Hübener, Hannes, De Giovannini, Umberto, Rubio, Angel
Format: Article
Language:English
Subjects:
639/166/987
639/301/119/995
639/766/1130
Characterization and Evaluation of Materials
Chemistry and Materials Science
Computational Intelligence
Electrons
Graphite
Harmonic generations
Lasers
Materials Science
Mathematical and Computational Engineering
Mathematical and Computational Physics
Mathematical Modeling and Industrial Mathematics
Molybdenum disulfide
Nanoscience
Nonlinear dynamics
Nonlinear optics
Phonons
Spectrum analysis
Symmetry
Theoretical
Vibration mode
Vibrations
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Summary:High-harmonic generation (HHG) has emerged as a central technique in attosecond science and strong-field physics, providing a tool for investigating ultrafast dynamics. However, the microscopic mechanism of HHG in solids is still under debate, and it is unclear how it is modified in the ubiquitous presence of phonons. Here we theoretically investigate the role of collectively coherent vibrations in HHG in a wide range of solids (e.g., hBN, graphite, 2H-MoS 2 , and diamond). We predict that phonon-assisted high harmonic yields can be significantly enhanced, compared to the phonon-free case – up to a factor of ~20 for a transverse optical phonon in bulk hBN. We also show that the emitted harmonics strongly depend on the character of the pumped vibrational modes. Through state-of-the-art ab initio calculations, we elucidate the physical origin of the HHG yield enhancement – phonon-assisted photoinduced carrier doping, which plays a paramount role in both intraband and interband electron dynamics. Our research illuminates a clear pathway toward comprehending phonon-mediated nonlinear optical processes within materials, offering a powerful tool to deliberately engineer and govern solid-state high harmonics.
ISSN:2057-3960
2057-3960
DOI:10.1038/s41524-024-01399-z