Two-Dimensional Frequency Resolved Optomolecular Gating of High-Order Harmonic Generation

Phys Rev Lett. 2016 Feb 5;116(5):053002. doi: 10.1103/PhysRevLett.116.053002. Epub 2016 Feb 2.


Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation-ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N_{2}O_{4}, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.