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Heteronuclear single-quantum correlation spectroscopy (HSQC) is a 2D NMR technique that reveals one-bond correlations between hydrogen and a heteronucleus. The HSQC experiment is similar to the heteronuclear correlation experiment (HETCOR) but is more sensitive. In the HSQC spectrum, the proton chemical shift is plotted on the horizontal F2 axis, while the 13C chemical shift is plotted on the vertical F1 axis. The corresponding proton and 13C spectra are also shown. The HSQC contour plot does...
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Probing phonon dynamics with multidimensional high harmonic carrier-envelope-phase spectroscopy.

Ofer Neufeld1, Jin Zhang1, Umberto De Giovannini1,2

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Proceedings of the National Academy of Sciences of the United States of America
|June 15, 2022
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Summary

We demonstrate how terahertz-driven coherent phonons in hexagonal boron nitride alter high harmonic generation (HHG) spectra. This method offers femtosecond resolution for probing ultrafast lattice dynamics and controlling HHG emission.

Keywords:
HHGnonlinear opticsphononspump-robe spectroscopyultrafast spectroscopy

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Area of Science:

  • Condensed Matter Physics
  • Attosecond Science
  • Materials Science

Background:

  • High harmonic generation (HHG) is a key process for generating extreme ultraviolet and X-ray light.
  • Coherent optical phonons can significantly influence electronic and optical properties of materials.
  • Hexagonal boron nitride (hBN) is a promising 2D material with unique phononic properties.

Purpose of the Study:

  • To investigate the impact of terahertz-excited coherent optical phonons on pump-probe high harmonic generation (HHG) in monolayer hBN.
  • To explore the potential of HHG as a probe for ultrafast lattice dynamics.
  • To demonstrate control over the HHG spectrum using coherent phonons.

Main Methods:

  • State-of-the-art ab initio calculations.
  • Pump-probe spectroscopy setup using terahertz pump and infrared probe pulses.
  • Analysis of HHG emission spectra and yield oscillations.

Main Results:

  • Coherent phonons attenuate the discrete harmonic orders in the HHG spectrum, leading to continuous emission.
  • HHG yield oscillates with pump-probe delay, reflecting ultrafast lattice dynamics (bond compression/stretching).
  • HHG becomes sensitive to carrier-envelope phase (CEP) when phonon period approaches pulse duration, enabling ultrafast spectroscopy.

Conclusions:

  • Pump-probe HHG in hBN provides a sensitive probe for ultrafast structural changes with ~1 femtosecond temporal resolution.
  • This technique allows for multidimensional HHG spectroscopy and control over HHG spectra.
  • The findings open new avenues for probing phonons and material dynamics with subcycle temporal resolution.