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Conjugated Polyelectrolytes in Interactions with Biomolecules for Supramolecular assembly and Sensing
Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Conjugated polyelectrolytes (CP) show interesting electrical and optical properties for organic electronics as well as for life science applications. Their possibilities of supramolecular assembly with nanowire like misfolded proteins, amyloids, as well as synthetic polypeptides or DNA forming conducting or luminescent nano composites is highly interesting as being a truly bottom up approach for fabrication of OLEDs, photovoltaic’s as well as logic devices. The conformation and aggregation dependent luminescence properties from the special class of CPs, Luminescent conjugated polyelectrolytes (LCP), have been utilised and developed as sensors to follow and study biomolecular interactions, DNA hybridisation, protein-protein interactions and staining of living cell cultures and tissue slides. In this thesis we are bringing the evolution a few steps further by applying new types of experimental techniques, such as light scattering and fluorescence correlation spectroscopy, combined with standard techniques as soft lithography and different spectroscopy techniques, to gain better knowledge of the optical behaviour of LCPs and their interactions with biomolecules. We explore the optical properties and vibronic transitions of LCPs; their ability of resonance energy transfer with LCPs indicating super lightning behaviour; the opposite fluorescence shift when interacting with α-helical rich polypeptides compared to earlier reports of interactions upon staining of β-rich amyloids; and the possibility of LCPs to influence protein aggregation as well as the possibility of fabricating biochips based on LCPs and soft lithography. Here we also show fundamental limitations to patterning using macromolecular fluids, of general relevance to soft lithography and nanoimprint lithography with low viscosity polymers.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2010. , 60 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1308
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-54902ISBN: 978-91-7393-408-4 (print)OAI: oai:DiVA.org:liu-54902DiVA: diva2:311100
Public defence
2010-05-14, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 14:00 (English)
Opponent
Supervisors
Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2014-04-08Bibliographically approved
List of papers
1. Limits to Nanopatterning of Fluids on Surfaces in Soft Lithography
Open this publication in new window or tab >>Limits to Nanopatterning of Fluids on Surfaces in Soft Lithography
2008 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 18, no 17, 2563-2571 p.Article in journal (Refereed) Published
Abstract [en]

Soft lithographic microcontact printing using the residual polydimethylsiloxane (PDMS) found in elastomeric PDMS stamps is demonstrated to lead to unstable prints with sub-micrometer dimensions. The statics and dynamics of the process have been followed with time-resolved atomic force microscopy, imaging ellipsometry, water contact angle measurement, and optical diffraction. It is proposed that this instability places a fundamental limitation on patterning by macromolecular fluids, which is of general relevance to soft lithography and nanoimprint lithography with low viscosity polymers.

Keyword
Lithography, microcontact printing (µCP), nanostructures, nanowires, surface patterning
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-42810 (URN)10.1002/adfm.200800073 (DOI)68960 (Local ID)68960 (Archive number)68960 (OAI)
Available from: 2009-10-10 Created: 2009-10-10 Last updated: 2017-12-13
2. Protein biochips patterned by microcontact printing or by adsorption-soft lithography in two modes
Open this publication in new window or tab >>Protein biochips patterned by microcontact printing or by adsorption-soft lithography in two modes
2008 (English)In: BIOINTERPHASES, ISSN 1559-4106 , Vol. 3, no 3, 75-82 p.Article in journal (Refereed) Published
Abstract [en]

Patterning of proteins is critical to protein biochips. Printing of layers of proteins is well established, as is adsorption of proteins to surfaces properly modified with surface chemical functionalities. The authors show that simple methods based on soft lithography stamps can be used to prepare functional antibody chips through both these routes. Both methods incorporate transfer of the stamp material poly (dimethylsiloxane) (PDMS) to the biochip, whether intended or not intended. The results indicate that microcontact printing of proteins always includes PDMS transfer, thereby creating a possibility of unspecific adsorption to a hydrophobic domain.

National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-17907 (URN)10.1116/1.2988771 (DOI)
Available from: 2009-04-26 Created: 2009-04-24 Last updated: 2010-04-20
3. DNA Chips with Conjugated Polyelectrolytes in Resonance Energy Transfer Mode
Open this publication in new window or tab >>DNA Chips with Conjugated Polyelectrolytes in Resonance Energy Transfer Mode
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2010 (English)In: LANGMUIR, ISSN 0743-7463, Vol. 26, no 5, 3753-3759 p.Article in journal (Refereed) Published
Abstract [en]

We show how to use well-defined conjugated polyelectrolytes (CPEs) combined With Surface energy patterning to Fabricate DNA Chips utilizing A fluorescence signal amplification. Cholesterol-modified DNA strands in complex with it CPE are adsorbed to a surface energy pattern, formed by printing with soft elastomer stamps. Hybridization of the surface bound DNA strands with it short complementary strand from Solution is monitored using both fluorescence microscopy and imaging surface plasmon resonance. The CPEs act as antennas, enhancing resonance energy transfer to the dye-labeled DNA when complementary hybridization of the double strand occurs.

National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-54255 (URN)10.1021/la903101v (DOI)000274636900113 ()
Available from: 2010-03-05 Created: 2010-03-05 Last updated: 2015-05-29
4. Oligothiophene Assemblies Defined by DNA Interaction: From Single Chains to Disordered Clusters
Open this publication in new window or tab >>Oligothiophene Assemblies Defined by DNA Interaction: From Single Chains to Disordered Clusters
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2009 (English)In: SMALL, ISSN 1613-6810 , Vol. 5, no 1, 96-103 p.Article in journal (Refereed) Published
Abstract [en]

The organization of conjugated polyelectrolytes (CPEs) interacting with biomolecules sets conditions for the biodetection of biological processes and identity, through the use of optical emission from the CPE. Herein, a well-defined CPE and its binding to DNA is studied. By using dynamic light scattering and circular dichroism spectroscopy, it is shown that the CPE forms a multimolecule ensemble in aqueous solution that is more than doubled it? size when interacting with a small DNA chain, while single chains are evident in ethanol. The related changes in the fluorescence spectra upon polymer aggregation are assigned to oscillator strength redistribution between vibronic transitions in weakly coupled H-aggregates. An enhanced single-molecule spectroscopy technique that allows full control of excitation and emission light polarization is applied to combed and decorated;,DNA chains. It is found that the organization of combed CPE-lambda DNA complexes (when dry on the surface) allows considerable variation of CPE distances and direction relative to the DNA chain. By analysis of the polarization data. energy transfer between the polymer chains in individual complexes is confirmed and their sizes estimated.

Keyword
aggregation, conjugated polymers, DNA, fluorescence, single-molecule spectroscopy
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-16829 (URN)10.1002/smll.200800855 (DOI)
Available from: 2009-02-20 Created: 2009-02-20 Last updated: 2010-04-20
5. Dark states in oligothiophenes: evidence from fluorescence correlation spectroscopy and dynamic light scattering
Open this publication in new window or tab >>Dark states in oligothiophenes: evidence from fluorescence correlation spectroscopy and dynamic light scattering
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

We report studies of the conjugated pentameric oligothiophene derivative p-FTAA, which changes optical properties in aqueous buffers of varying pH and concentration. Using dynamic light scattering, luminescence spectroscopy and fluorescence correlation spectroscopy, we find evidence for the formation of large clusters of p-FTAA in aqueous environment, formation of very large non-emissive clusters, and the presence of at least two dark transient states, one presumably being a triplet state. The clustering of p-FTAA is therefore an important mechanism. This work provides an interpretation of fluorescence spectra used for the detection of misfolding proteins through interaction with p-FTAA.

National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-54897 (URN)
Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2014-04-08
6. Interactions between a luminescent conjugated oligoelectrolyte and insulin during early phases of amyloid formation
Open this publication in new window or tab >>Interactions between a luminescent conjugated oligoelectrolyte and insulin during early phases of amyloid formation
2011 (English)In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 11, no 8, 1120-1127 p.Article in journal (Refereed) Published
Abstract [en]

Folding of an amino acid polypeptide chain into its native three-dimensional protein is a delicate process. Misfolding may cause assembly of dysfunctional proteins leading to aggregated assemblies, in medicine denoted amyloids, causing Alzheimer’s, Parkinson and a number of other protein related diseases. Amyloids have also shown promising results as building blocks in organic electronic applications, associated to conjugated polymers. Luminescent conjugated oligo- and polythiophenes (LCPs) have been further developed for biosensor applications exhibiting good ability to discriminate and determine different types of amyloid enrichment in complex environments, such as in tissue sections. The nature of interaction between the amyloid assemblies and LCPs is still not fully understood. In this study we use steady-state fluorescence spectroscopy, dynamic light scattering, transmission electron microscopy and fluorescence correlation spectroscopy to follow the interplay between the anionic oligothiophene derivative 4',3'''-Bis-carboxymethyl-[2,2';5',2'';5'',2''';5''',2'''']quinque thiophene-5,5''''-dicarboxylic acid (p-FTAA), and prefibrillar protein assemblies present during the earlier stage of in vitro fibrillation of bovine insulin. Our findings confirm that p-FTAA interacts with pre-fibrillar species of insulin preceding the formation of mature insulin amyloid fibrils, and insights regarding the molecular interplay between p-FTAA and these species are provided.

Place, publisher, year, edition, pages
Wiley, 2011
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-54898 (URN)10.1002/mabi.201100016 (DOI)000294160900011 ()
Note
Funding Agencies|Swedish Science Council (VR)||Strategic Research Foundation (SSF) through the center for organic bioelectronics (OBOE)||Knut and Alice Wallenberg foundation||Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2017-12-12
7. Supramolecular Assembly of Designed α-Helical Polypeptide-Based Nanostructures and Luminescent Conjugated Polyelectrolytes
Open this publication in new window or tab >>Supramolecular Assembly of Designed α-Helical Polypeptide-Based Nanostructures and Luminescent Conjugated Polyelectrolytes
2010 (English)In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 10, no 8, 836-841 p.Article in journal (Refereed) Published
Abstract [en]

Designed polypeptides with controllable folding properties are utilized as supramolecular templates for fabrication of ordered nanoscale molecular and fibrous assemblies of luminescent conjugated polymers (LCPs). The properties of the LCPs as well as the three dimensional conformation of the polypeptide-scaffold determine how the polymers are arranged in the supramolecular construct, which highly affects the properties of the hybrid material. The ability to control the polypeptide conformation and assembly into fibers provide a promising route for tuning the optical properties of LCPs and for fabrication of complex functional supramolecules with well defined structural properties.

Place, publisher, year, edition, pages
John Wiley & Sons, 2010
Keyword
α-helical; conjugated polymers; hybrid materials; peptides; self-assembly
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-54899 (URN)10.1002/mabi.200900463 (DOI)000281387900002 ()
Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2017-12-12Bibliographically approved
8. Synthetic Polypeptides as Scaffolds for Supramolecular Assembly of Conducting Polymer Nanocomposites
Open this publication in new window or tab >>Synthetic Polypeptides as Scaffolds for Supramolecular Assembly of Conducting Polymer Nanocomposites
Show others...
2010 (English)Manuscript (preprint) (Other academic)
Abstract [en]

The development of nanoelectronics has resulted in enormous advancements in fabrication techniques that have enabled massproduction of CMOS circuits with feature sizes below 45nm. There is a large interest in new methods to further push the size limits, lower the production costs and to facilitate the design of more advanced three-dimensional structures beyond today’s 2.5 dimensional architectures. Self-assembly is probably the most important scheme in this development and is currently applied to many different areas and classes of nanoelectronics. Self-assembly enables fabrication of structures well below 10 nm in feature size and allows for incorporation of novel nanomaterials, such as metallic and semiconducting nanoparticles with many interesting optical and electrical properties. The controlled self-assembly of electro-active nanocomposites is of great interest for the development of novel functional materials including biosensors, electrochromic/plasmonic hybrid devices, and polymer/nanoparticle-based memories.

Keyword
Conducting Polymers, Organic Electronics, Conducting Nanowires, Self- Assembly, Supramolecular Materials
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-54901 (URN)
Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2010-04-20

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