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Resolving Multiple Molecular Orbitals Using Two-Dimensional High-Harmonic Spectroscopy

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Title
Resolving Multiple Molecular Orbitals Using Two-Dimensional High-Harmonic Spectroscopy
Author(s)
Hyeok Yun; Kyung-Min Lee; Jae Hee Sung; Kyung Taec Kim; Hyung Taek Kim; Chang Hee Nam
Publication Date
2015-04
Journal
PHYSICAL REVIEW LETTERS, v.114, no.15, pp.153901 -
Publisher
AMER PHYSICAL SOC
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
URI
http://pr.ibs.re.kr/handle/8788114/1770
DOI
10.1103/PhysRevLett.114.153901
ISSN
0031-9007
Appears in Collections:
Center for Relativistic Laser Science(초강력 레이저과학 연구단) > Journal Papers (저널논문)
Files in This Item:
PhysRevLett.114(초강력).pdfDownload

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