GIST Scholar
College of Natural Sciences
Department of Physics and Photon Science
1. Journal Articles
Resolving Multiple Molecular Orbitals Using Two-Dimensional High-Harmonic Spectroscopy
- Type
- Article
- Citation
- Physical Review Letters, v.114, no.15
- Issued Date
- 2015-04
- Abstract
- High-harmonic radiation emitted from molecules in a strong laser field contains information on molecular structure and dynamics. When multiple molecular orbitals participate in high-harmonic generation, resolving the contribution of each orbital is crucial for understanding molecular dynamics and for extending high-harmonic spectroscopy to more complicated molecules. We show that two-dimensional high-harmonic spectroscopy can resolve high-harmonic radiation emitted from the two highest-occupied molecular orbitals, HOMO and HOMO-1, of aligned molecules. By the application of an orthogonally polarized two-color laser field that consists of the fundamental and its second-harmonic fields to aligned CO2 molecules, the characteristics attributed to the two orbitals are found to be separately imprinted in odd and even harmonics. Two-dimensional high-harmonic spectroscopy may open a new route to investigate ultrafast molecular dynamics during chemical processes.
- Publisher
- American Physical Society
- ISSN
- 0031-9007
- Appears in Collections:
- Department of Physics and Photon Science > 1. Journal Articles
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