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Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes

Permanent link
https://hdl.handle.net/10037/8979
DOI
https://doi.org/10.1021/acsphotonics.5b00053
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Accepted manuscript version (PDF)
Date
2015-05-12
Type
Journal article
Tidsskriftartikkel
Peer reviewed

Author
Friese, Daniel Henrik; Bast, Radovan; Ruud, Kenneth
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 behaviour of all even-and odd-photon absorption properties shows a semi-quantitative 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.
Description
This is accepted manuscript version.Published version available at http://dx.doi.org/10.1021/acsphotonics.5b00053
Publisher
American Chemical Society
Citation
ACS Photonics 2015, 2(5):572-577
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