Optical saturation driven by exciton confinement in molecular-chains: a TDDFT study

Physical Review Letters 101, 13302 - 4 (2008)

Optical saturation driven by exciton confinement in molecular-chains: a TDDFT study

D. Varsano, A. Marini, A. Rubio

We have identified excitonic confinement in one-dimensional molecular chains (i.e. polyacetylene and H2) as the main driving force for the saturation of the chain polarizability as a function of the number of molecular units. This conclusion is based on first principles time-dependent density functional theory calculations performed with a new derived exchange{correlation kernel. The failure of simple local and semi{local functionals is shown to be related to the lack of memory effects, spatial ultranonlocality, and self{interaction corrections. These effects get smaller as the gap of the system reduces, and simple approximations do work better.

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Doi
http://dx.doi.org/10.1103/PhysRevLett.101.133002
arxiv
http://arxiv.org/abs/0710.2057v1

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