Hot electron assisted femtochemistry at surfaces - A time-dependent density functional theory approach
Physical Review B 79, 195405 - 10 (2009)
Hot electron assisted femtochemistry at surfaces - A time-dependent density functional theory approach
Using time-evolution time-dependent density functional theory (TDDFT) we study the interactions between single electrons and molecular resonances at surfaces. We perform a number of calculations on an electron hitting an adsorbed molecule from inside the surface and establish a picture, where the resonance is being probed by the incoming electron. This enables us to extract the position of the resonance energy through a fitting procedure. It is demonstrated that with the model we can extract several properties of the system, such as the presence of resonance peaks, the time electrons stay on the molecule before returning to the surface when hitting a molecular resonance and the lowering of the resonance energy due to an image charge effect. Finally we apply the TDDFT procedure to only consider the decay of molecular excitatioUsing time-evolution time-dependent density functional theory (TDDFT) we study the interactions between single electrons and molecular resonances at surfaces. We perform a number of calculations on an electron hitting an adsorbed molecule from inside the surface and establish a picture, where the resonance is being probed by the incoming electron. This enables us to extract the position of the resonance energy through a fitting procedure. It is demonstrated that with the model we can extract several properties of the system, such as the presence of resonance peaks, the time electrons stay on the molecule before returning to the surface when hitting a molecular resonance and the lowering of the resonance energy due to an image charge effect. Finally we apply the TDDFT procedure to only consider the decay of molecular excitations and find that it agrees quite well with the width of the projected density of Kohn-Sham states.
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- http://dx.doi.org/10.1103/PhysRevB.79.195405
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- Physical Review Editors' Suggestion. Selected for the June 2009 issue of Virtual Journal of Ultrafast Science. The Virtual Journal.