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- W2003706049 abstract "Enhancement of the nonresonant second order molecular hyperpolarizabilities y were observed in stacked macrocyclic molecular systems, previously in a t-oxo silicon phthalocyanme (SiPcO) monomer, dimer and trimer series, and now in bacteriochiorophyll a (BChla) arrays oflight harvesting (LH) proteins. Compared to monomeric BChla in a tetrahydrofuran (TifF) solution, the <γ> for each macrocycle was enhanced in naturally occurring stacked macrocyclic molecular systems in the bacterial photosynthetic LH proteins where BChla 's are arranged in tilted face-to-face arrays. In addition, the γ enhancement is more significant in B875 of LH1 than in B850 in LH2. Theoretical modeling of the nonresonant γ enhancement using simplified molecular orbitals for model SiPcO indicated that the energy level of the two photon state is crucial to the γ enhancement when a two photon process is involved. Additionally, charge transfer between the monomers may be important if this produces states which are close to one-photon resonance. The calculated results can be extended to γ enhancement in B875 and B850 arrays, suggesting that BChla in B875 are more strongly coupled than in B850. In addition, a 50-160 fold increase in <γ> for the S1 excited state ofrelative to S0 ofbacteriochlorophyll in vivo was observed which provides an alternative method for probing excited state dynamics and a potential application for molecular switching." @default.
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- W2003706049 date "1997-10-13" @default.
- W2003706049 modified "2023-09-23" @default.
- W2003706049 title "Third-order nonlinear optical properties of stacked bacteriochlorophylls in bacterial photosynthetic light-harvesting proteins" @default.
- W2003706049 doi "https://doi.org/10.1117/12.284247" @default.
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