Tracking ultrafast solid-state dynamics using high harmonic spectroscopy
Abstract
We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy method for tracking photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal phase transitions in vanadium dioxide. We benchmark the technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency characteristic of a coherent phonon of the equilibrium monoclinic phase over a wide range of excitation fluences. These results demonstrate that tr-HHG is capable of tracking complex dynamics in solids through its sensitivity to the band structure.
- Publication:
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Physical Review Research
- Pub Date:
- June 2021
- DOI:
- 10.1103/PhysRevResearch.3.023250
- arXiv:
- arXiv:2003.10430
- Bibcode:
- 2021PhRvR...3b3250B
- Keywords:
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- Physics - Optics;
- Condensed Matter - Materials Science
- E-Print:
- 20 pages and 4 figures main text, 8 pages and 4 figures supplementary information