Probing phonon dynamics with multidimensional high harmonic carrier-envelope-phase spectroscopy

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Erscheinungsjahr:
2022
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Text
Beschreibung:
  • High harmonic generation (HHG) has recently been established as a powerful method for probing ultrafast electron dynamics in solids. However, it remains unknown if HHG can be similarly applied for probing lattice distortions such as phonons. Specifically, it is unclear if the extreme nonlinearity of HHG can contribute to enhanced temporal resolution or sensitivity for probing lattice dynamics (compared to other, perturbative, methods). Here, we theoretically explore HHG in solids with active phonons. We present a pump-probe and multidimensional spectroscopy approach that relies on carrier-envelope-phase-sensitivity, in which HHG is highly sensitive for phonon dynamics. Strikingly, the predicted temporal resolution is ∼1 femtosecond, much below the probe pulse duration, owing to the subcycle nature of the approach. 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.
Lizenz:
  • info:eu-repo/semantics/openAccess
Quellsystem:
Forschungsinformationssystem der UHH

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oai:www.edit.fis.uni-hamburg.de:publications/78baa240-f79b-44be-adeb-ba7cbed7e2ad