The one-photon (1P) and two-photon (2P) absorption properties of three quadrupolar dyes, featuring thiophene as a donor and acceptors of varying strengths, are determined by a combination of experimental and computational methods employing the density functional theory (DFT). The emission shifts in different solvents are well reproduced by time-dependent DFT calculations with the linear response and state specific approaches in the framework of the polarizable continuum model. The calculations show that the energies of both 1P- and 2P-active states decrease with an increase of the strength of the acceptor. The 2P absorption cross-sections predicted by the response theory are accounted for by considering just one intermediate state (S1) in the sum-over-states formulation. For the chromophore featuring the stronger acceptor, the energetic positions of the 1P- and 2P-active states prevent the exploitation of the theoretically predicted very high 2P activity due to the competing 1P absorption into the S1 state.

One- and two-photon absorption properties of quadrupolar thiophene-based dyes with acceptors of varying strengths

Canola S.;Bergamini G.;Villa M.;Acocella A.;Ceroni P.
;
Negri F.
2019

Abstract

The one-photon (1P) and two-photon (2P) absorption properties of three quadrupolar dyes, featuring thiophene as a donor and acceptors of varying strengths, are determined by a combination of experimental and computational methods employing the density functional theory (DFT). The emission shifts in different solvents are well reproduced by time-dependent DFT calculations with the linear response and state specific approaches in the framework of the polarizable continuum model. The calculations show that the energies of both 1P- and 2P-active states decrease with an increase of the strength of the acceptor. The 2P absorption cross-sections predicted by the response theory are accounted for by considering just one intermediate state (S1) in the sum-over-states formulation. For the chromophore featuring the stronger acceptor, the energetic positions of the 1P- and 2P-active states prevent the exploitation of the theoretically predicted very high 2P activity due to the competing 1P absorption into the S1 state.
Canola S.; Mardegan L.; Bergamini G.; Villa M.; Acocella A.; Zangoli M.; Ravotto L.; Vinogradov S.A.; Di Maria F.; Ceroni P.; Negri F.
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/11585/700455
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