Mapping Light-Dressed Floquet Bands by Highly Nonlinear Optical Excitations and Valley Polarization

J Phys Chem Lett. 2023 Dec 21;14(50):11298-11304. doi: 10.1021/acs.jpclett.3c02936. Epub 2023 Dec 8.

Abstract

Ultrafast nonlinear optical phenomena in solids have been attracting a great deal of interest as novel methodologies for the femtosecond spectroscopy of electron dynamics and control of the properties of materials. Here, we theoretically investigate strong-field nonlinear optical transitions in a prototypical two-dimensional material, hBN, and show that the k-resolved conduction band charge occupation patterns induced by an elliptically polarized laser can be understood in a multiphoton resonant picture, but, remarkably, only if using the Floquet light-dressed states instead of the undressed matter states. Our work demonstrates that Floquet dressing affects ultrafast charge dynamics and photoexcitation even from a single pump pulse and establishes a direct measurable signature for band dressing in nonlinear optical processes in solids, opening new paths for ultrafast spectroscopy and valley manipulation.