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Five-photon absorption and selective enhancement of multiphoton absorption processes
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology. KTH, School of Computer Science and Communication (CSC), Centres, Centre for High Performance Computing, PDC.
2015 (English)In: ACS Photonics, ISSN 2330-4022, Vol. 2, no 5, 572-577 p.Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2015. Vol. 2, no 5, 572-577 p.
Keyword [en]
ab initio calculations, molecular modeling, nonlinear optical properties, quantum chemistry, response theory, structure-activity relations, UV/vis spectroscopy
National Category
Other Engineering and Technologies
URN: urn:nbn:se:kth:diva-170262DOI: 10.1021/acsphotonics.5b00053ISI: 000355066900002ScopusID: 2-s2.0-84930225427OAI: diva2:827999
EU, European Research Council, 279619

QC 20150629

Available from: 2015-06-29 Created: 2015-06-29 Last updated: 2015-08-17Bibliographically approved

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Bast, Radovan
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Theoretical Chemistry and BiologyCentre for High Performance Computing, PDC
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