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Three-Photon Spectroscopy of Porphyrins

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dc.contributor.authorRavotto, L.
dc.contributor.authorMeloni, S. L.
dc.contributor.authorEsipova, T. V.
dc.contributor.authorAnna, J. M.
dc.contributor.authorMasunov, A. E.
dc.date.accessioned2024-11-27T15:40:26Z
dc.date.available2024-11-27T15:40:26Z
dc.date.issued2020
dc.description.abstract© 2020 American Chemical Society.Recent advances in laser technology have made three-photon (3P) microscopy a real possibility, raising interest in the phenomenon of 3P absorption (3PA). Understanding 3PA of organic chromophores is especially important in view of those imaging applications that rely on exogenous probes, whose optical properties can be manipulated and optimized. Here, we present measurements and theoretical analysis of the degenerate 3PA spectra of several phosphorescent metalloporphyrins, which are used in the construction of biological oxygen probes. The effective 3PA cross sections (σ(3)) of these porphyrins near 1700 nm, a new promising biological optical window, were found to be on the order of 1000 GM3 (1 GM3 = 10-83 cm6 s2), therefore being among the highest values reported to date for organic chromophores. To interpret our data, we developed a qualitative four-state model specific for porphyrins and used it in conjunction with quantitative analysis based on the time-dependent density functional theory (TDDFT)/a posteriori Tamm-Dancoff approximation (ATDA)/sum-over-states (SOS) formalism. The analysis revealed that B (Soret) state plays a key role in the enhancement of 3PA of porphyrins in the Q band region, while the low-lying two-photon (2P)-allowed gerade states interfere negatively and diminish the 3PA strength. This study features the first systematic examination of 3PA properties of porphyrins, suggesting ways to improve their performance and optimize them for imaging and other biomedical applications.
dc.identifier.citationThree-Photon Spectroscopy of Porphyrins / Ravotto, L. [et al.] // Journal of Physical Chemistry A. - 2020. - 10.1021/acs.jpca.0c08334
dc.identifier.doi10.1021/acs.jpca.0c08334
dc.identifier.urihttps://www.doi.org/10.1021/acs.jpca.0c08334
dc.identifier.urihttps://www.scopus.com/record/display.uri?eid=2-s2.0-85098801895&origin=resultslist
dc.identifier.urihttp://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcAuth=Alerting&SrcApp=Alerting&DestApp=WOS_CPL&DestLinkType=FullRecord&UT=WOS:000608856500012
dc.identifier.urihttps://openrepository.mephi.ru/handle/123456789/22998
dc.relation.ispartofJournal of Physical Chemistry A
dc.titleThree-Photon Spectroscopy of Porphyrins
dc.typeArticle
dspace.entity.typePublication
relation.isOrgUnitOfPublication06e1796d-4f55-4057-8d7e-bb2f3b5676f5
relation.isOrgUnitOfPublication.latestForDiscovery06e1796d-4f55-4057-8d7e-bb2f3b5676f5
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