title: Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes.
abstract: We study one-, two-, three-, four-, and five-photon absorption of three centrosymmetric molecules using density functional theory. These calculations are the firstab initiocalculations of five-photon absorption. Even- and odd-order absorption processes show different trends in the absorption cross sections. The behavior of all even- and odd-photon absorption properties shows a semiquantitative similarity, which can be explained using few-state models. This analysis shows that odd-photon absorption processes are largely determined by the one-photon absorption strength, whereas all even-photon absorption strengths are largely dominated by the two-photon absorption strength, in both cases modulated by powers of the polarizability of the final excited state. We demonstrate how to selectively enhance a specific multiphoton absorption process.
authors.affiliation: Centre for Theoretical and Computational Chemisty, Department of Chemistry, University of Tromsø-The Arctic University of Norway , N-9037 Tromsø, Norway.
authors.forename: Daniel H
authors.initials: DH
authors.lastname: Friese
authors.affiliation: Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, AlbaNova University Centre , S-10691 Stockholm, Sweden ; PDC Centre for High Performance Computing, Royal Institute of Technology , S-10044 Stockholm, Sweden.
authors.forename: Radovan
authors.initials: R
authors.lastname: Bast
authors.affiliation: Centre for Theoretical and Computational Chemisty, Department of Chemistry, University of Tromsø-The Arctic University of Norway , N-9037 Tromsø, Norway.
authors.forename: Kenneth
authors.initials: K
authors.lastname: Ruud
keywords: UV/vis spectroscopy; ab initio calculations; molecular modeling; nonlinear optical properties; quantum chemistry; response theory; structure−activity relations