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Related Experiment Videos

Controlling high harmonic generation with molecular wave packets.

J Itatani1, D Zeidler, J Levesque

  • 1National Research Council Canada, Ottawa, Ontario, K1A 0R6 Canada. jitatani@lbl.gov

Physical Review Letters
|May 21, 2005
PubMed
Summary

Controlling molecular alignment influences high harmonic generation. This molecular wave packet method shapes attosecond pulses and reveals molecular orbital symmetry.

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Area of Science:

  • Quantum optics
  • Attosecond science
  • Molecular physics

Background:

  • High harmonic generation (HHG) is a crucial process for producing ultrashort light pulses.
  • Controlling molecular alignment offers a pathway to tailor HHG properties.
  • Understanding molecular orbital symmetry is key to controlling electron dynamics.

Purpose of the Study:

  • To investigate the influence of molecular alignment on high harmonic generation.
  • To demonstrate spectral shaping of high harmonics using rotational wave packets.
  • To correlate molecular orbital symmetry with HHG intensity modulation.

Main Methods:

  • Utilizing rotational wave packets in low-density N2 and O2 gases.
  • Controlling molecular alignment relative to laser polarization.

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  • Analyzing the intensity modulation and spectral characteristics of generated high harmonics.
  • Main Results:

    • Observed strong intensity modulation and spectral shaping of high harmonics.
    • In N2 (sigma(g) HOMO), maximum HHG signal aligns with laser polarization; minimum is perpendicular.
    • In O2 (pi(g) HOMO), harmonics are enhanced at ~45-degree alignment.
    • Demonstrated that molecular orbital symmetry can be deduced from harmonic spectra.

    Conclusions:

    • Molecular alignment is a powerful tool for controlling high harmonic generation.
    • Rotational wave packets enable spectral shaping of attosecond pulses.
    • HHG provides a method to probe and understand molecular orbital symmetries.