Excitons play a key role in the linear optical response of two-dimensional (2D) materials. However, their role in the nonlinear response to intense, nonresonant, low-frequency light is often overlooked as strong fields are expected to tear the electron-hole pair apart. Using high-harmonic generation as a spectroscopic tool, we theoretically study their formation and role in the nonlinear optical response. We show that the excitonic contribution is prominent and that excitons remain stable even when the driving laser field surpasses the strength of the Coulomb field binding the electron-hole pair. We demonstrate a parallel between the behavior of strongly laser-driven excitons in 2D solids and strongly driven Rydberg states in atoms, including the mechanisms of their formation and stability. Last, we show how the excitonic contribution can be singled out by encapsulating the 2D material in a dielectric, tuning the excitonic energy and its contribution to the high-harmonic spectrum.
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| http://dx.doi.org/10.1126/sciadv.adn6985 | DOI Listing |
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