Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 20, Issue 12, Pages 8311-8325Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7cp07849h
Keywords
-
Funding
- EPSRC/DSTL MURI-MIR grant [EP/I08680/1]
Ask authors/readers for more resources
Here we present a fully ab initio study of the high-order harmonic generation (HHG) spectrum of aligned CO2 molecules. The calculations have been performed by using the molecular time-dependent (TD) B-spline algebraic diagrammatic construction (ADC) method. We quantitatively study how the sub-cycle laser-driven multi-channel dynamics, as reflected in the position of the dynamical minimum in the HHG spectrum, is affected by the full inclusion of both correlation-driven and laser-driven dipole interchannel couplings. We calculate channel-resolved spectral intensities as well as the phase differences between contributions of the different ionization-recombination channels to the total HHG spectrum. Our results show that electron correlation effectively controls the relative contributions of the different channels to the total HHG spectrum, leading to the opening of the new ones (1(u)(2), 1(2)sigma+g), previously disregarded for the aligned molecular setup. We conclude that inclusion of many-electron effects into the theoretical interpretation of molecular HHG spectra is essential in order to correctly extract ultrafast electron dynamics using HHG spectroscopy.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available