Contributions of inner-valence molecular orbitals and multiphoton resonances to high-order-harmonic generation of N2: A time-dependent density-functional-theory study

Xi Chu and Gerrit C. Groenenboom
Phys. Rev. A 93, 013422 – Published 25 January 2016

Abstract

Using a time-dependent density-functional-theory (TDDFT) method, we calculated the high-harmonic generation (HHG) spectra of N2 in 800- and 1300-nm intense lasers. The calculations reproduce the experimentally observed minimum near 40 eV and the shift of the minimum due to interference of different molecular orbitals. They also support the proposed shape resonance near 30 eV. The TDDFT method allows us to analyze the involvement of different electronic configurations in the HHG process. We identified a significant role of Rydberg states and autoionizing states in enhancing HHG. This finding is consistent with studies of photoelectron spectra in a similar energy range. Moreover, we discover a significant contribution of the 2σg orbital above 40 eV, demonstrating the complexity of electronic structure information contained in molecular HHG. At high energy not only the HOMO and HOMO-1 are important, as suggested by earlier studies, but the HOMO-3 contributes substantially as well.

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  • Received 14 December 2015

DOI:https://doi.org/10.1103/PhysRevA.93.013422

©2016 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Xi Chu

  • Department of Chemistry and Biochemistry, The University of Montana, Missoula, Montana 59812, USA

Gerrit C. Groenenboom

  • Institute for Molecules and Materials, Radboud University Nijmegen, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands

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Issue

Vol. 93, Iss. 1 — January 2016

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