Five-photon absorption and selective enhancement of multiphoton absorption processes
2015 (English)In: ACS Photonics, ISSN 2330-4022, Vol. 2, no 5, 572-577 p.Article in journal (Refereed) Published
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.
ab initio calculations, molecular modeling, nonlinear optical properties, quantum chemistry, response theory, structure-activity relations, UV/vis spectroscopy
Other Engineering and Technologies
IdentifiersURN: urn:nbn:se:kth:diva-170262DOI: 10.1021/acsphotonics.5b00053ISI: 000355066900002ScopusID: 2-s2.0-84930225427OAI: oai:DiVA.org:kth-170262DiVA: diva2:827999
FunderEU, European Research Council, 279619
QC 201506292015-06-292015-06-292015-08-17Bibliographically approved