High harmonic generation and molecular orbital tomography in multielectron systems

Area of Science:

• Quantum optics
• Atomic and molecular physics
• Computational chemistry

Background:

• High harmonic generation (HHG) produces radiation containing molecular electronic structure information.
• Previous HHG theories were limited to the single-active-electron approximation.

Purpose of the Study:

• Develop a theory for HHG in multielectron systems.
• Incorporate electron spin statistics and electron-electron correlations.
• Improve theoretical predictions and experimental agreement.

Main Methods:

• Utilized the semisudden approximation for the recombination step.
• Developed a theory for tomographic reconstruction in multielectron systems.
• Accounted for electron spin and electron-electron correlations.

Main Results:

• Theoretical predictions were significantly modified by including electron correlations.
• The new theory shows better agreement with experimental results.
• Exchange contributions to harmonic radiation offer additional electronic wave function information.

Conclusions:

• The developed theory accurately describes HHG in multielectron systems.
• Electron correlations are crucial for accurate HHG predictions.
• HHG can provide deeper insights into molecular electronic properties.