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The Aufbau Principle and Hund's Rule03:02

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Updated: Jun 28, 2026

Infrared Degenerate Four-wave Mixing with Upconversion Detection for Quantitative Gas Sensing
10:42

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Published on: March 22, 2019

High harmonic generation from multiple orbitals in N2.

Brian K McFarland1, Joseph P Farrell, Philip H Bucksbaum

  • 1PULSE Institute, SLAC, Menlo Park, CA 94025, USA, and Departments of Physics and Applied Physics, Stanford University, Stanford, CA 94305, USA.

Science (New York, N.Y.)
|November 1, 2008
PubMed
Summary
This summary is machine-generated.

Researchers observed lower-lying molecular orbitals influencing high harmonic generation (HHG) in N2 molecules. This finding is crucial for understanding ultrafast electron dynamics in laser-excited molecules.

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Harmonic Nanoparticles for Regenerative Research
09:23

Harmonic Nanoparticles for Regenerative Research

Published on: May 1, 2014

Area of Science:

  • Quantum Chemistry
  • Molecular Spectroscopy
  • Attosecond Science

Background:

  • High harmonic generation (HHG) is a key process for generating ultrashort light pulses.
  • Theoretical models predict that molecular orbitals below the highest occupied molecular orbital (HOMO) should influence HHG.
  • Experimental evidence for the contribution of these lower-lying orbitals has been lacking.

Purpose of the Study:

  • To experimentally investigate the influence of molecular electronic states below the HOMO on laser-driven HHG.
  • To explore the role of the HOMO-1 orbital in the HHG process of N2 molecules.
  • To advance the understanding of ultrafast electron dynamics in molecules.

Main Methods:

  • High harmonic generation (HHG) spectroscopy was performed on N2 molecules.
  • Molecular alignment was controlled, with N2 molecules oriented perpendicular to the laser polarization.
  • The resulting HHG spectrum was analyzed for characteristic features.

Main Results:

  • A distinct maximum was observed in the HHG spectrum at the rotational half-revival.
  • This spectral feature provides evidence for the contribution of the HOMO-1 orbital.
  • The results demonstrate the influence of electronic states below the HOMO on HHG.

Conclusions:

  • The study provides the first experimental observation of lower-lying molecular orbitals influencing HHG.
  • The findings are essential for a comprehensive understanding of electron motion on subfemtosecond and subangstrom scales.
  • This work opens new avenues for controlling and probing molecular electronic dynamics.