Abstract：
:Under acidic conditions and at high ionic strength, the zinc cation is removed from its metal complex with 5,10,15,20-tetrakis(4-sulfonatophenyl)porphyrin (TPPS4) thus leading to the diacid free porphyrin, that subsequently self-organize into J-aggregates. The kinetics of the demetallation step and the successive supramolecular assembly formation have been investigated as a function of pH and ionic strength (controlled by adding ZnSO4). The demetallation kinetics obey to a rate law that is first order in [ZnTPPS4] and second order in [H+], according to literature, with k2 = 5.5 ± 0.4 M-2 s-1 at 298 K (IS = 0.6 M, ZnSO4). The aggregation process has been modeled according to an autocatalytic growth, where after the formation of a starting seed containing m porphyrin units, the rate evolves as a power of time. A complete analysis of the extinction time traces at various wavelengths allows extraction of the relevant kinetic parameters, showing that a trimer or tetramer should be involved in the rate-determining step of the aggregation. The extinction spectra of the J-aggregates evidence quite broad bands, suggesting an electronic coupling mechanism different to the usual Frenkel exciton coupling. Resonance light scattering intensity in the aggregated samples increases with increasing both [H+] and [ZnSO4]. Symmetry breaking occurs in these samples and the J-aggregates show circular dichroism spectra with unusual bands. The asymmetry g-factor decreases in its absolute value with increasing the catalytic rate kc, nulling and eventually switching the Cotton effect from negative to positive. Some inferences on the role exerted by zinc cations on the kinetics and structural features of these nanostructures have been discussed.
journal_name
Int J Mol Scijournal_title
International journal of molecular sciencesauthors
Occhiuto IG,Castriciano MA,Trapani M,Zagami R,Romeo A,Pasternack RF,Monsù Scolaro Ldoi
10.3390/ijms21114001subject
Has Abstractpub_date
2020-06-03 00:00:00issue
11issn
1422-0067pii
ijms21114001journal_volume
21pub_type
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