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

MPS-Authors
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Neufeld,  O.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Zhang,  J.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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de Giovannini,  U.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Dipartimento di Fisica e Chimica—Emilio Segrè, Università degli Studi di Palermo;

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Hübener,  H.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Rubio,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Nano-Bio Spectroscopy Group, Universidad del País Vasco UPV/EHU;
Center for Computational Quantum Physics (CCQ), The Flatiron Institute;

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Fulltext (public)

pnas.2204219119.pdf
(Publisher version), 2MB

Supplementary Material (public)

pnas.2204219119.sapp.pdf
(Supplementary material), 479KB

Citation

Neufeld, O., Zhang, J., de Giovannini, U., Hübener, H., & Rubio, A. (2022). Probing phonon dynamics with multidimensional high harmonic carrier-envelope-phase spectroscopy. Proceedings of the National Academy of Sciences of the United States of America, 119(25): e2204219119. doi:10.1073/pnas.2204219119.


Cite as: http://hdl.handle.net/21.11116/0000-000A-17C4-F
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.