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Hyeok Yun1, Kyung-Min Lee1, Jae Hee Sung1,2

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Two-dimensional high-harmonic spectroscopy distinguishes contributions from individual molecular orbitals in high-harmonic generation. This technique advances the study of molecular structure and ultrafast dynamics in complex systems.

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Area of Science:

  • Quantum optics
  • Molecular physics
  • Attosecond science

Background:

  • High-harmonic generation (HHG) in molecules reveals insights into electronic structure and dynamics.
  • Resolving contributions from multiple molecular orbitals is essential for advanced HHG spectroscopy.
  • Current methods struggle to disentangle orbital-specific information in complex molecular systems.

Purpose of the Study:

  • To demonstrate a method for resolving the distinct contributions of the two highest-occupied molecular orbitals (HOMO and HOMO-1) to high-harmonic radiation.
  • To establish two-dimensional high-harmonic spectroscopy as a tool for probing multi-orbital dynamics.

Main Methods:

  • Utilized a two-dimensional high-harmonic spectroscopy technique.
  • Employed an orthogonally polarized two-color laser field (fundamental and second-harmonic).
  • Applied the method to aligned carbon dioxide (CO2) molecules.

Main Results:

  • Successfully resolved high-harmonic radiation originating from both the HOMO and HOMO-1 orbitals.
  • Observed distinct imprints of the two orbitals in odd and even harmonic orders.
  • Demonstrated the capability to differentiate orbital contributions in HHG.

Conclusions:

  • Two-dimensional high-harmonic spectroscopy can effectively separate and identify contributions from different molecular orbitals.
  • This technique offers a new pathway for investigating ultrafast molecular dynamics in chemical processes.
  • The findings pave the way for more detailed studies of complex molecular systems using HHG.