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Instruments / Technical Area	Publication Details	Published
B23-Circular Dichroism	Self-assembled porphyrazine-nucleoside on DNA templates: highly fluorescent chromophore arrays and sizing forensic tandem repeat sequences Mariia V. Ishutkina , Alice R. Berry , Rohanah Hussain , Olga G. Khelevina , Giuliano Siligardi , Eugen Stulz European Journal Of Organic Chemistry DOI: 10.1002/ejoc.201800683 Diamond Proposal Number(s): [13158] Show Abstract ▼ Abstract: The formation of chromophore arrays using a DNA templating approach leads to the creation of supramolecular assemblies, where the optical properties of the overall system can be fine‐tuned to a large extent. In particular porphyrin derivatives have shown to be versatile building blocks; mostly covalent chemistry was used for embedding the units into DNA strands. Self‐assembly of porphyrin modified nucleosides, on the other hand, has not been investigated as a simplified approach. We report on the synthesis of a magnesium(II) tetraaza porphine (MgTAP) coupled to deoxy‐uridine, and array formation on DNA templates which contain well‐defined oligo(dA) segments showing strong fluorescence enhancement which is significantly larger than with a Zn‐porphyrin. The use of the deep‐eutectic solvent glycholine is essential for successful assembly formation. The system allows for sizing of short tandem repeat markers with multiple adenosines, thus the concept could be adaptable to in vitro forensic DNA profiling with a suitable set of different chromophores on all nucleosides.	May 2018
B23-Circular Dichroism	Increased duplex stabilization in porphyrin-LNA zipper arrays with structure dependent exciton coupling Daniel Singleton , Rohanah Hussain , Giuliano Siligardi , Pawan Kumar , Patrick J. Hrdlicka , Nina Berova , Eugen Stulz Organic & Biomolecular Chemistry DOI: 10.1039/C5OB01681A Diamond Proposal Number(s): [5872, 6703, 6705] Show Abstract ▼ Abstract: Porphyrins were attached to LNA uridine building blocks via rigid 5-acetylene or more flexible propargylamide linkers and incorporated into DNA strands. The systems show a greatly increased thermodynamic stability when using as little as three porphyrins in a zipper arrangement. Thermodynamic analysis reveals clustering of the strands into more ordered duplexes with both greater negative ΔΔS and ΔΔH values, and less ordered duplexes with small positive ΔΔS differences, depending on the combination of linkers used. The exciton coupling between the porphyrins is dependent on the flanking DNA sequence in the single stranded form, and on the nature of the linker between the nucleobase and the porphyrin in the double stranded form; it is, however, also strongly influenced by intermolecular interactions. This system is suitable for the formation of stable helical chromophore arrays with sequence and structure dependent exciton coupling.	Sep 2015
B23-Circular Dichroism	Directed Formation of DNA Nanoarrays through Orthogonal Self-Assembly Jon Burns , Jurgita Zekonyte , Guiliano Siligardi , Rohanah Hussain , Eugen Stulz Molecules 16 (6), 4912 - 4922 DOI: 10.3390/molecules16064912 PMID: 21677604 Show Abstract ▼ Abstract: We describe the synthesis of terpyridine modified DNA strands which selectively form DNA nanotubes through orthogonal hydrogen bonding and metal complexation interactions. The short DNA strands are designed to self-assemble into long duplexes through a sticky-end approach. Addition of weakly binding metals such as Zn(II) and Ni(II) induces the formation of tubular arrays consisting of DNA bundles which are 50-200 nm wide and 2-50 nm high. TEM shows additional long distance ordering of the terpy-DNA complexes into fibers.	Jun 2011
B23-Circular Dichroism	Introducing Structural Flexibility Into Porphyrin-DNA Zipper Arrays Eugen Stulz , Ashley Brewer , Guiliano Siligardi , Cameron Neylon Organic & Biomolecular Chemistry 9, 777-782 DOI: 10.1039/c0ob00535e Diamond Proposal Number(s): [1815] Show Abstract ▼ Abstract: A more flexible nucleotide building block for the synthesis of new DNA based porphyrinzipper arrays is described. Changing the rigid acetylene linker between the porphyrin substituent and the 2′-deoxyuridine to a more flexible propargyl amide containing linkage leads in part to an increased duplex stability. The CD spectra reveal different electronic interactions between the porphyrins depending on the type of linker used. Molecular modelling suggests large variation of the relative orientation of the porphyrins within the major groove of the DNA. The porphyrins can be metallated post-synthetically with different metals as shown with zinc, cobalt and copper. The spectroscopic features do not alter drastically upon metallation apart from the CD spectra, and the stability of the metal complex is highly dependent on the nature of the metal. As shown by CD spectroscopy, the zinc porphyrin is rapidly demetallated at high temperatures. Globular structure determination using SAXS indicates that a molecular assembly comprised of a two to four helical bundle dominates in solution at higher concentrations (≥50 μM) which is not observed by spectroscopy at lower concentrations (≤1 μM).	Mar 2011
B23-Circular Dichroism	Energy Transfer & Self-Assembly of DNA based Nano-Structures Jon Burns , Guiliano Siligardi , Cameron Neylon , Eugen Stulz	Nov 2010
B23-Circular Dichroism	Synthesis of DNA-Porphyrin Arrays Daniel Singleton , Tom Bandy , Imenne Bouamaied , Ashley Brewer , Jon Burns , Simon Gerrard , Gabriella Marth , Thao Nguyen , Guiliano Siligardi , Eugen Stulz Sixth International Conference on Porphyrins and Phthalocyanines (ICPP-6),	Jul 2010
B23-Circular Dichroism	G-Quadruplexes with Covalently Bound Porphyrins Daniel Singleton , Keith Fox , Guiliano Siligardi , Eugen Stulz Sixth International Conference on Porphyrins and Phthalocyanines (ICPP-6),	Jul 2010

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