Multi-channel dynamics in high harmonic generation of aligned CO₂: ab initio analysis with time-dependent B-spline algebraic diagrammatic construction
File(s)PCCP2018.pdf (510.92 KB)
Accepted version
Author(s)
Ruberti, M
Decleva, P
Averbukh, V
Type
Journal Article
Abstract
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 (12Πu, 12Σ), 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.
Date Issued
2018-03-13
Date Acceptance
2018-03-02
Citation
Physical Chemistry Chemical Physics, 2018, 20 (12), pp.8311-8325
ISSN
1463-9076
Publisher
Royal Society of Chemistry
Start Page
8311
End Page
8325
Journal / Book Title
Physical Chemistry Chemical Physics
Volume
20
Issue
12
Copyright Statement
© the Owner Societies 2018
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/29532820
Subjects
02 Physical Sciences
03 Chemical Sciences
Chemical Physics
Publication Status
Published
Coverage Spatial
England