Resolving multiple molecular orbitals using two-dimensional high-harmonic spectroscopy.
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.
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.
Hyeok
H
Yun
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.
Kyung-Min
KM
Lee
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.|Advanced Photonics Research Institute, Gwangju Institute of Science and Technology (GIST), Gwangju 500-712, Republic of Korea.
Jae Hee
JH
Sung
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.|Department of Physics and Photon Science, Gwangju Institute of Science and Technology (GIST), Gwangju 500-712, Republic of Korea.
Kyung Taec
KT
Kim
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.|Advanced Photonics Research Institute, Gwangju Institute of Science and Technology (GIST), Gwangju 500-712, Republic of Korea.
Hyung Taek
HT
Kim
Center for Relativistic Laser Science, Institute for Basic Science (IBS), Gwangju 500-712, Republic of Korea.|Department of Physics and Photon Science, Gwangju Institute of Science and Technology (GIST), Gwangju 500-712, Republic of Korea.
Chang Hee
CH
Nam