Laser-induced preferential dehydrogenation of graphane

Abstract

We have used first-principles simulations based on time-dependent density functional theory to show that short laser pulses can trigger preferential hydrogen desorption from the upper or lower side of suspended graphane (H-terminated graphene). This control is achieved by using intense ultrashort p-polarized laser pulses (∼2 fs) with an asymmetric time envelope. The dynamical Stark effect induced by the pulse creates an asymmetric charge distribution and force field on the H ions, even at low laser fluence. At finite temperatures the carbon-hydrogen stretching softens, favoring H desorption from one side. This transient geometry can be modified by halogen functionalization, which results in a two-dimensional dipolar structure. © 2012 American Physical Society.