Cooperative Enhancement of Two-Photon Absorption in Self-Assembled Zinc-Porphyrin Nanostructures

Femtosecond two-photon absorption (2PA) spectra were measured of a series of butadiyne-linked zinc-porphyrin oligomers assembled in single- and double-strand linear and cyclic structures containing 6, 12, or 24 porphyrin units, in the excitation wavelength range 900–1600 nm. We observe strong enhanc...

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Bibliographic Details
Published in:Journal of physical chemistry. C 2016-06, Vol.120 (21), p.11663-11670
Main Authors: Mikhaylov, Alexander, Kondratuk, Dmitry V, Cnossen, Arjen, Anderson, Harry L, Drobizhev, Mikhail, Rebane, Aleksander
Format: Article
Language:English
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Summary:Femtosecond two-photon absorption (2PA) spectra were measured of a series of butadiyne-linked zinc-porphyrin oligomers assembled in single- and double-strand linear and cyclic structures containing 6, 12, or 24 porphyrin units, in the excitation wavelength range 900–1600 nm. We observe strong enhancement of the 2PA cross-section in the Soret region, with maximum values up to σ2PA ∼ 105 GM depending on the geometry of the construct, which we quantitatively explain in terms of a three essential energy level model and cooperative enhancement of the transition dipole moments between the states. The Zn-coordinated template-bound ring of 6 porphyrin units, which resembles some natural light-harvesting systems, results in the highest 2PA cross-section per porphyrin unit (∼104 GM). It is remarkable that this molecule gives such strong σ2PA, when the S0–S1 (0–0) transition is essentially forbidden for one photon transition.
ISSN:1932-7447
1932-7455
DOI:10.1021/acs.jpcc.6b01394