Eugen Stulz

Multistep DNA‐Templated Reactions for the Synthesis of Functional Sequence Controlled Oligomers

Biomimetic: A strand displacement mechanism was designed to permit DNA-templated synthesis of functional oligomers of arbitrary length (see scheme). Key features of the mechanism are that successive coupling reactions take place in near-identical environments and that purification is only necessary in the last synthesis step.

Duplex Stabilization and Energy Transfer in Zipper Porphyrin-DNA

Zip it up: Attachment of porphyrins onto complementary DNA strands leads to zipper-porphyrin arrays and, in the presence of eleven modifications, an increase in the melting temperature of the duplex. Mixed zinc and free-base porphyrin arrays undergo energy transfer from the zinc porphyrin to the free-base porphyrin in the annealed duplex but not in the denatured form (see scheme), giving access to reversible formation of potential photonic wires.

Lipid-bilayer-spanning DNA nanopores with a bifunctional porphyrin anchor

Holding tight: An artificial membrane nanopore assembled from DNA oligonucleotides carries porphyrin tags (red), which anchor the nanostructure into the lipid bilayer. The porphyrin moieties also act as fluorescent dyes to aid the microscopic visualization of the DNA nanopore.

DNA Architectonics: towards the Next Generation of Bio‐inspired Materials

The use of DNA in nanobiotechnology has advanced to a stage at which almost any two or three dimensional architecture can be designed with high precision. The choice of the DNA sequences is essential for successful self-assembly, and opens new ways of making nanosized monomolecular assemblies with predictable structure and size. The inclusion of designer nucleoside analogues further adds functionality with addressable groups, which have an influence on the function of the DNA nano-objects. This article highlights the recent achievements in this emerging field and gives an outlook on future perspectives and applications.

Programmable One-Pot Multistep Organic Synthesis Using DNA Junctions

A system for multistep DNA-templated synthesis is controlled by the sequential formation of DNA junctions. Reactants are attached to DNA adapters which are brought together by hybridization to DNA template strands. This process can be repeated to allow sequence-controlled oligomer synthesis while maintaining a constant reaction environment, independent of oligomer length, at each reaction step. Synthesis can take place in a single pot containing all required reactive monomers. Different oligomers can be synthesized in parallel in the same vessel, and the products of parallel synthesis can be ligated, reducing the number of reaction steps required to produce an oligomer of a given length.

Sequence-specific synthesis of macromolecules using DNA-templated chemistry

Using a strand exchange mechanism we have prepared, by DNA templated chemistry, two 10-mers with defined and tunable monomer sequences. An optimized reaction protocol achieves 85% coupling yield per step, demonstrating that DNA-templated chemistry is a powerful tool for the synthesis of macromolecules with full sequence control.

EIS-based biosensor for ultra-sensitive detection of TNF-α from non-diluted human serum

Serum background is a critical issue for biosensor development as it interferes with the detection of target molecules and may give rise to false positive signal. We present here highly sensitive and selective TNF-α biosensor which is able to detect TNF-α from non-diluted human serum using magnetic bead coupled antibody and electrochemical impedance spectroscopy (EIS) techniques. The process is designed to detect TNF-α from human serum in three stages; (1) abundant protein backgrounds are depleted from the serum using magnetic bead coupled albumin and IgG antibodies, (2) after background depletion TNF-α is captured using magnetic bead coupled TNF-α antibody, and (3) the captured TNF-α is eluted from the magnetic beads and measured using EIS technique in which comb structured gold microelectrodes array (CSGM) is utilized to enhance the detection sensitivity. The system is able to achieve the limit of detection (LOD) at 1 pg/ml (57 fM) and a linear relationship between increasing TNF-α concentrations and charge-transfer resistance in a dynamic range of 1-1000 pg/ml.

Supramolecular helical porphyrin arrays using DNA as a scaffold

A diphenyl porphyrin substituted nucleotide was incorporated site specifically into DNA, leading to helical stacked porphyrin arrays in the major groove of the duplexes. The porphyrins show an electronic interaction which is significantly enhanced compared to the analogous tetraphenyl porphyrin (TPP) as shown in the large exciton coupling of the porphyrin B-band absorbance. Analogous to the TPP-DNA, an induced helical secondary structure is observed in the single strand porphyrin-DNA. The modified DNA can be hybridised to an immobilised complementary strand leading to fluorescent beads.

A highly sensitive electrochemical genosensor based on Co-porphyrin-labelled DNA

We report the use of Co-porphyrins as electrochemical tags for a highly sensitive and selective genosensor. An avian influenza virus-based DNA sequence characteristic of H5N1 was detected at femtomolar levels from competing non-complementary sequences through hybridisation with the labeled DNA.

Programmed Assembly of Peptide-Functionalized Gold Nanoparticles on DNA Templates

We present a novel nanoparticle building block system based on the interactions between short synthetic oligonucleotides and peptides. Gold nanoparticles coated with DNA-binding peptides can be attached to self-organized oligonucleotide templates to formulate well-ordered structures of nanoparticles. By regulating the amount of DNA-binding peptide attached to the nanoparticle surface and using specifically designed oligonucleotides, the nanoparticle assembly can be controlled to form dimers, trimers, and adjustable-length nanoparticle chains as well as more complex structures.