Abstract
We explore pump-probe high harmonic generation (HHG) from monolayer hexagonal-boron-nitride, where a terahertz pump excites coherent optical phonons that are subsequently probed by an intense infrared pulse that drives HHG. We find, through state-of-the-art ab initio calculations, that the structure of the emission spectrum is attenuated by the presence of coherent phonons and no longer comprises discrete harmonic orders, but rather a continuous emission in the plateau region. The HHG yield strongly oscillates as a function of the pump-probe delay, corresponding to ultrafast changes in the lattice such as specific bond compression or stretching dynamics. We further show that in the regime where the excited phonon period and the pulse duration are of the same order of magnitude, the HHG process becomes sensitive to the carrier-envelope phase (CEP) of the driving field, even though the pulse duration is so long that no such sensitivity is observed in the absence of coherent phonons. The degree of CEP sensitivity versus pump-probe delay is shown to be a highly selective measure for instantaneous structural changes in the lattice, providing an approach for ultrafast multidimensional HHG spectroscopy. Remarkably, the obtained temporal resolution for phonon dynamics is ∼1 femtosecond, which is much shorter than the probe pulse duration because of the inherent subcycle contrast mechanism. Our work paves the way toward routes of probing phonons and ultrafast material structural changes with subcycle temporal resolution and provides a mechanism for controlling the HHG spectrum.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.