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Nano Research 2022, 15(6): 5527-5537 https://doi.org/10.1007/s12274-021-4048-x
Research Article | Open Access | Issue | Published: 14 March 2022

Structure and principles of self-assembly of giant “sea urchin” type sulfonatophenyl porphine aggregates

Show Author's Information Marijus Pleckaitis12,  Fayez Habach3,  Lukas Kontenis14,  Gábor Steinbach567,  Greta Jarockyte12,  Agne Kalnaityte1,  Ildikó Domonkos8,  Parveen Akhtar8,  Mehdi Alizadeh1,  Saulius Bagdonas1,  Vitalijus Karabanovas129,  Győző Garab7810,  Ricardas Rotomskis12,  Virginijus Barzda1311( )
Laser Research Center, Faculty of Physics, Vilnius University, Sauletekio av. 10, Vilnius LT-10223, Lithuania
Biomedical Physics Laboratory, National Cancer Institute, P. Baublio str. 3b, Vilnius LT-08406, Lithuania
Department of Chemical and Physical Sciences, University of Toronto Mississauga, 3359 Mississauga Rd, Mississauga L5L 1C6, Canada
Light Conversion, Keramiku str. 2B, Vilnius LT-10233, Lithuania
Cellular Imaging Laboratory, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Institute of Biophysics, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Biofotonika Research and Development Ltd., Dózsa u. 7, Szeged 6720, Hungary
Institute of Plant Biology, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Department of Chemistry and Bioengineering, Vilnius Gediminas Technical University, Sauletekio av. 11, Vilnius LT-10223, Lithuania
Department of Physics, Faculty of Science, University of Ostrava, Chittussiho 10, Ostrava CZ-710 00, Czech Republic
Department of Physics, University of Toronto, 60 St. George St. Toronto, Toronto M5S 1A7, Canada
Keywords:
self-assembly, nanostructures, meso-tetra(4-sulfonatophenyl)porphine (TPPS4) aggregates , harmonophores, polarimetric second harmonic generation microscopy, third harmonic generation microscopy
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Pleckaitis M, Habach F, Kontenis L, et al. Structure and principles of self-assembly of giant “sea urchin” type sulfonatophenyl porphine aggregates. Nano Research, 2022, 15(6): 5527-5537. https://doi.org/10.1007/s12274-021-4048-x
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Abstract Full text Electronic supplementary material About this article

Principles of molecular self-assembly into giant hierarchical structures of hundreds of micrometers in size are studied in aggregates of meso-tetra(4-sulfonatophenyl)porphine (TPPS4). The aggregates form a central tubular core, which is covered with radially protruding filamentous non-branching aggregates. The filaments cluster and orient at varying angles from the core surface and some filaments form bundles. Due to shape resemblance, the structures are termed giant sea urchin (GSU) aggregates. Spectrally resolved fluorescence microscopy reveals J- and H-bands of TPPS4 aggregates in both the central core and the filaments. The fluorescence of the core is quenched while filaments exhibit strong fluorescence. Upon drying, the filament fluorescence gets quenched while the core is less affected, showing stronger relative fluorescence. Fluorescence-detected linear dichroism (FDLD) microscopy reveals that absorption dipoles corresponding to J-bands are oriented along the filament axis. The comparison of FDLD with scanning electron microscopy (SEM) reveals the structure of central core comprised of multilayer ribbons, which wind around the core axis forming a tube. Polarimetric second-harmonic generation (SHG) and third-harmonic generation microscopy exhibits strong signal from the filaments with nonlinear dipoles oriented close to the filament axis, while central core displays very low SHG due to close to centrosymmetric organization. Large chiral nonlinear susceptibility points to helical arrangement of the filaments. The investigation shows that TPPS4 molecules form distinct aggregate types, including chiral nanotubes and nanogranular aggregates that associate into the hierarchical GSU structure, prototypical to complex biological structures. The chiral TPPS4 aggregates can serve as harmonophores for nonlinear microscopy.


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Electronic supplementary material
About this article

Structure and principles of self-assembly of giant “sea urchin” type sulfonatophenyl porphine aggregates

Show Author's information Marijus Pleckaitis12, Fayez Habach3, Lukas Kontenis14, Gábor Steinbach567, Greta Jarockyte12, Agne Kalnaityte1, Ildikó Domonkos8, Parveen Akhtar8, Mehdi Alizadeh1, Saulius Bagdonas1, Vitalijus Karabanovas129, Győző Garab7810, Ricardas Rotomskis12, Virginijus Barzda1311( )
Laser Research Center, Faculty of Physics, Vilnius University, Sauletekio av. 10, Vilnius LT-10223, Lithuania
Biomedical Physics Laboratory, National Cancer Institute, P. Baublio str. 3b, Vilnius LT-08406, Lithuania
Department of Chemical and Physical Sciences, University of Toronto Mississauga, 3359 Mississauga Rd, Mississauga L5L 1C6, Canada
Light Conversion, Keramiku str. 2B, Vilnius LT-10233, Lithuania
Cellular Imaging Laboratory, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Institute of Biophysics, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Biofotonika Research and Development Ltd., Dózsa u. 7, Szeged 6720, Hungary
Institute of Plant Biology, Biological Research Centre, Eötvös Loránd Research Network, Temesvári körút 62, Szeged 6726, Hungary
Department of Chemistry and Bioengineering, Vilnius Gediminas Technical University, Sauletekio av. 11, Vilnius LT-10223, Lithuania
Department of Physics, Faculty of Science, University of Ostrava, Chittussiho 10, Ostrava CZ-710 00, Czech Republic
Department of Physics, University of Toronto, 60 St. George St. Toronto, Toronto M5S 1A7, Canada

Abstract

Principles of molecular self-assembly into giant hierarchical structures of hundreds of micrometers in size are studied in aggregates of meso-tetra(4-sulfonatophenyl)porphine (TPPS4). The aggregates form a central tubular core, which is covered with radially protruding filamentous non-branching aggregates. The filaments cluster and orient at varying angles from the core surface and some filaments form bundles. Due to shape resemblance, the structures are termed giant sea urchin (GSU) aggregates. Spectrally resolved fluorescence microscopy reveals J- and H-bands of TPPS4 aggregates in both the central core and the filaments. The fluorescence of the core is quenched while filaments exhibit strong fluorescence. Upon drying, the filament fluorescence gets quenched while the core is less affected, showing stronger relative fluorescence. Fluorescence-detected linear dichroism (FDLD) microscopy reveals that absorption dipoles corresponding to J-bands are oriented along the filament axis. The comparison of FDLD with scanning electron microscopy (SEM) reveals the structure of central core comprised of multilayer ribbons, which wind around the core axis forming a tube. Polarimetric second-harmonic generation (SHG) and third-harmonic generation microscopy exhibits strong signal from the filaments with nonlinear dipoles oriented close to the filament axis, while central core displays very low SHG due to close to centrosymmetric organization. Large chiral nonlinear susceptibility points to helical arrangement of the filaments. The investigation shows that TPPS4 molecules form distinct aggregate types, including chiral nanotubes and nanogranular aggregates that associate into the hierarchical GSU structure, prototypical to complex biological structures. The chiral TPPS4 aggregates can serve as harmonophores for nonlinear microscopy.

Keywords: self-assembly, nanostructures, meso-tetra(4-sulfonatophenyl)porphine (TPPS4) aggregates , harmonophores, polarimetric second harmonic generation microscopy, third harmonic generation microscopy

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Received: 08 September 2021
Revised: 04 December 2021
Accepted: 05 December 2021
Published: 14 March 2022
Issue date: June 2022

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© The Author(s) 2021

Acknowledgements

Acknowledgements

The authors dedicate this paper to the memory of Teodor Silviu Balaban (1958–2016) for his pioneering contributions on the structure and spectroscopy of ordered self-assembling nanorods.

This work was supported by European Regional Development Fund (No. 01.2.2.-LMT-K-718-02-0016) under grant agreement with the Research Council of Lithuania (LMTLT). Support was also provided by the Natural Sciences and Engineering Research Council of Canada (NSERC) (Nos. RGPIN-2017-06923 and DGDND-2017-00099). I. D. was supported by GINOP-2.3.2-15-2016-00058 and G. S. by GINOP-2.3.2-15-2016-00001 and ELKH KÜ-37/2020 grants from the Hungarian Ministry for National Economy and the Eötvös Loránd Research Network, respectively.

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