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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 first ab initio calculations 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.

SUBMITTER: Friese DH

PROVIDER: S-EPMC4477907 | biostudies-literature | 2015 May

REPOSITORIES: biostudies-literature

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Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes.

Friese Daniel H DH Bast Radovan R Ruud Kenneth K

ACS photonics 20150512 5

We study one-, two-, three-, four-, and five-photon absorption of three centrosymmetric molecules using density functional theory. These calculations are the first <i>ab initio</i> calculations 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 ...[more]

PMID: 26120588

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