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Issue 12, 2018
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Multi-channel dynamics in high harmonic generation of aligned CO2: ab initio analysis with time-dependent B-spline algebraic diagrammatic construction

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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+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.

Graphical abstract: Multi-channel dynamics in high harmonic generation of aligned CO2: ab initio analysis with time-dependent B-spline algebraic diagrammatic construction

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Publication details

The article was received on 21 Nov 2017, accepted on 02 Mar 2018 and first published on 13 Mar 2018


Article type: Paper
DOI: 10.1039/C7CP07849H
Citation: Phys. Chem. Chem. Phys., 2018,20, 8311-8325
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    Multi-channel dynamics in high harmonic generation of aligned CO2: ab initio analysis with time-dependent B-spline algebraic diagrammatic construction

    M. Ruberti, P. Decleva and V. Averbukh, Phys. Chem. Chem. Phys., 2018, 20, 8311
    DOI: 10.1039/C7CP07849H

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