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Nonlinear Time-Dependent Density Functional Theory Studies of Ionization in CO2 and N2 by Intense Laser Pulses and Molecular Orbital Reconstruction

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High Performance Computing Systems and Applications (HPCS 2009)

Part of the book series: Lecture Notes in Computer Science ((LNTCS,volume 5976))

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Abstract

Time-dependent density functional theory, TDDFT, studies of the ionization of CO2 and N2, by intense laser pulses peak intensities (3.50×1014, 1.40×1015, 2.99×1015 and 5.59×1015 W/cm2) at 800 nm (ω = 0.0584 a.u.) are presented in the nonlinear nonpertubative regime using the LB94 potential which reproduces the ionization potential of our systems more accurately, without significant increase in computational costs over a local-density approximation. Special emphasis is placed on elucidating molecular orbital (MO) orientation and various peak intensities effects on the ionization processes. The results reveal that molecular orbital ionizations are strongly sensitive to their symmetry (MO shape), the induced dipole coupling between molecular orbitals, and the laser intensities. Notably, we found that with a proper choice of the laser intensity (3.5×1014 W/cm2), the sensitivity is strong enough so that the nature and symmetry of the highest occupied molecular orbital can be directly probed and visualized from the angular dependence of laser induced ionization. At higher intensities, ionization is found to occur also from inner orbitals, thus complicating imaging of simple orbitals.

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Authors and Affiliations

  1. Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec, J1K 2R1, Canada

    Emmanuel Penka Fowe & André Dieter Bandrauk

Authors
  1. Emmanuel Penka Fowe
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  2. André Dieter Bandrauk
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Editor information

Editors and Affiliations

  1. Dept. of Psychology, Queen‘s University, 62 Arch St, K7L 3N6, Kingston, Ontario, Canada

    Douglas J. K. Mewhort

  2. Dept of Chemistry, Queen’s University, Chernoff Hall, K7L 3N6, Kingston, Ontario, Canada

    Natalie M. Cann

  3. University of Ottawa, Hagen Hall, 115 Séraphin-Marion, K1N 6N5, Ottawa, Ontario, Canada

    Gary W. Slater

  4. Oak Ridge National Laboratory, 1 Bethel Valley Road, Bldg. 5100, MS-6173, Oak Ridge, 37831-6173, TN, USA

    Thomas J. Naughton

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Penka Fowe, E., Bandrauk, A.D. (2010). Nonlinear Time-Dependent Density Functional Theory Studies of Ionization in CO2 and N2 by Intense Laser Pulses and Molecular Orbital Reconstruction. In: Mewhort, D.J.K., Cann, N.M., Slater, G.W., Naughton, T.J. (eds) High Performance Computing Systems and Applications. HPCS 2009. Lecture Notes in Computer Science, vol 5976. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-12659-8_11

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  • DOI: https://doi.org/10.1007/978-3-642-12659-8_11

  • Publisher Name: Springer, Berlin, Heidelberg

  • Print ISBN: 978-3-642-12658-1

  • Online ISBN: 978-3-642-12659-8

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