The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field

Hui Xiong; Benoit Mignolet; Li Fang; Timur Osipov; Thomas J A Wolf; Emily Sistrunk; Markus Gühr; Francoise Remacle; Nora Berrah

doi:10.1038/s41598-017-00124-9

The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field

Sci Rep. 2017 Mar 9;7(1):121. doi: 10.1038/s41598-017-00124-9.

Authors

Hui Xiong¹, Benoit Mignolet², Li Fang³, Timur Osipov⁴, Thomas J A Wolf⁵, Emily Sistrunk^{5

6}, Markus Gühr^{5

7}, Francoise Remacle², Nora Berrah⁸

Affiliations

¹ Physics Department, University of Connecticut, Storrs, CT, 06269, USA.
² Departement de Chimie, B6c, Université de Liege, B4000, Liege, Belgium.
³ Center for High Energy Density Science, University of Texas, Austin, TX, 78712, USA.
⁴ LCLS, National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁵ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁶ Lawrence Livermoor National Laboratory, CA, USA.
⁷ Institut für Physik und Astronomie, Universität Potsdam, 14476, Potsdam, Germany.
⁸ Physics Department, University of Connecticut, Storrs, CT, 06269, USA. [email protected].

Abstract

The interaction of gas phase endohedral fullerene Ho₃N@C₈₀ with intense (0.1-5 × 10¹⁴ W/cm²), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho₃N@C₈₀^q+, q = 1-2, was found to be different from that of C₆₀. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C_60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho₃N@C₈₀ is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 × 10¹⁴ W/cm².

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.