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Observation of laser-induced electronic structure in oriented polyatomic molecules.

P M Kraus1, O I Tolstikhin2, D Baykusheva1

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|May 6, 2015
PubMed
Summary

Strong laser fields significantly alter molecular electronic structures, as revealed by high-harmonic spectroscopy. This finding impacts attosecond spectroscopies and our understanding of light-matter interactions.

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Area of Science:

  • Quantum optics
  • Molecular spectroscopy
  • Strong-field physics

Background:

  • Attosecond time-resolved measurements commonly use intense near-infrared laser pulses.
  • Techniques like attosecond streaking and high-harmonic generation involve non-perturbative light-matter interactions.
  • The influence of strong laser fields on the sample itself has often been overlooked.

Purpose of the Study:

  • To investigate laser-induced modifications of molecular electronic structure using high-harmonic spectroscopy.
  • To study the effect of strong laser fields on polar polyatomic molecules (CH3F and CH3Br).
  • To demonstrate that robust observables can reveal substantial electronic structure changes.

Main Methods:

  • Utilizing high-harmonic spectroscopy to probe molecular electronic properties.
  • Employing spatially oriented CH3F and CH3Br molecules.
  • Measuring intensity ratios of even and odd harmonic orders and emission from aligned vs. unaligned molecules.

Main Results:

  • Accurate measurement of intensity ratios of harmonic orders.
  • Quantification of emission differences between aligned and unaligned molecules.
  • Demonstration of substantial modification of molecular electronic structure by the external laser field.

Conclusions:

  • The strong laser field significantly modifies the electronic structure of molecules.
  • High-harmonic spectroscopy provides robust observables to detect these modifications.
  • These findings present new avenues for strong-field attosecond spectroscopies.