| 1. |
- Fang, Yurui, 1983, et al.
(författare)
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Plasmon Enhanced Internal Photoemission in Antenna-Spacer-Mirror Based Au/TiO2 Nanostructures
- 2015
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Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 15:6, s. 4059-4065
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Tidskriftsartikel (refereegranskat)abstract
- Emission of photoexcited hot electrons from plasmonic metal nanostructures to semiconductors is key to a number of proposed nanophotonics technologies for Solar harvesting, water splitting, photocatalysis, and a variety of optical sensing and photodetector applications. Favorable materials and catalytic properties make systems based on gold and TiO2 particularly interesting, but the internal photo emission efficiency for visible light is low because of the wide bandgap of the semiconductor. We investigated the incident photon-to-electron conversion efficiency of thin TiO2 films decorated with Au nanodisk antennas in an electrochemical circuit and found that incorporation of a Au mirror beneath the semiconductor amplified the photoresponse for light with wavelength lambda = 500-950 nm by a factor 2-10 compared to identical structures lacking the mirror component. Classical electrodynamics simulations showed that the enhancement effect is caused by a favorable interplay between localized surface plasmon excitations and cavity modes that together amplify the light absorption in the Au/TiO2 interface. The experimentally determined internal quantum efficiency for hot electron transfer decreases monotonically with wavelength, similar to the probability for interband excitations with energy higher than the Schottky barrier obtained from a density functional theory band structure simulation of a thin Au/TiO2 slab.
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| 2. |
- Junesch, Juliane, 1987, et al.
(författare)
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Location-specific nanoplasmonic sensing of biomolecular binding to lipid membranes with negative curvature
- 2015
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3372 .- 2040-3364. ; 7:37, s. 15080-15085
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Tidskriftsartikel (refereegranskat)abstract
- The biochemical processes of cell membranes are sensitive to the geometry of the lipid bilayer. We show how plasmonic "nanowells" provide label-free real-time analysis of molecules on membranes with detection of preferential binding at negative curvature. It is demonstrated that norovirus accumulate in invaginations due to multivalent interactions with glycosphingolipids.
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| 3. |
- Malekian, Bita, 1986, et al.
(författare)
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Optical properties of plasmonic nanopore arrays prepared by electron beam and colloidal lithography
- 2019
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Ingår i: Nanoscale Advances. - : Royal Society of Chemistry (RSC). - 2516-0230. ; 1:11, s. 4282-4289
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Tidskriftsartikel (refereegranskat)abstract
- Solid state nanopores are central structures for many applications. To date, much effort has been spent on controlled fabrication of single nanopores, while relatively little work has focused on large scale fabrication of arrays of nanopores. In this work we show wafer-scale fabrication of plasmonic nanopores in 50 nm thick silicon nitride membranes with one or two 30 nm gold films, using electron beam lithography with a negative resist or a new version of colloidal lithography. Both approaches offer good control of pore diameter (even below 100 nm) and with high yield (>90%) of intact membranes. Colloidal lithography has the advantage of parallel patterning without expensive equipment. Despite its serial nature, electron beam lithography provides high throughput and can make arbitrary array patterns. Importantly, both methods prevent metal from ending up on the membrane pore sidewalls. The new fabrication methods make it possible to compare the optical properties of structurally identical plasmonic nanopore arrays with either long-range order (e-beam) or short-range order (colloidal). The resonance features in the extinction spectrum are very similar for both structures when the pitch is the same as the characteristic spacing in the self-assembled colloidal pattern. Long-range ordering slightly enhances the magnitude of the extinction maximum and blueshift the transmission maximum by tens of nm. Upon reducing the diameter in long-range ordered arrays, the resonance is reduced in magnitude and the transmission maximum is further blue shifted, just like for short-range ordered arrays. These effects are well explained by interpreting the spectra as Fano interference between the grating-type excitation of propagating surface plasmons and the broad transmission via individual pores in the metal film. Furthermore, we find that only the short-range ordered arrays scatter light, which we attribute to the highly limited effective period in the short-range ordered system and the corresponding lack of coherent suppression of scattering by interference effects.
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| 4. |
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| 5. |
- Dahlin, Andreas, 1980, et al.
(författare)
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Plasmonic Nanopores in Metal-Insulator-Metal Films
- 2014
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Ingår i: Advanced Optical Materials. - : Wiley. - 2195-1071. ; 2:6, s. 556-564
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Tidskriftsartikel (refereegranskat)abstract
- A novel type of plasmonic nanopore array in a metal-insulator-metal thin film is presented. The optical properties of this structure are described using a generic theoretical framework for surface waves in a coupled multilayer system. The characteristic spacing (short-range order) of the pores enables grating-type coupling to hybridized surface plasmons, with stronger coupling to some modes than others. The nature of the optical resonances and their excitation mechanisms can be conceptually understood from a charge distribution argument. The experimental results are further verified by numerical simulations, which also enable visualization of the near field. This study illustrates the surface plasmon characteristics (sensitive to periodicity) of the extinction maximum in the asymmetric spectral resonance induced by aperture arrays, while the transmission maximum corresponds to a resonance of localized character (sensitive to pore shape). Finally, the use of these nanopores for sensing applications through changes in the refractive index is evaluated.
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| 6. |
- Emilsson, Gustav, 1989, et al.
(författare)
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Gating Protein Transport in Solid State Nanopores by Single Molecule Recognition
- 2018
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Ingår i: ACS Central Science. - : American Chemical Society (ACS). - 2374-7951 .- 2374-7943. ; 4:8, s. 1007-1014
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Tidskriftsartikel (refereegranskat)abstract
- Control of molecular translocation through nanoscale apertures is of great interest for DNA sequencing, biomolecular filters, and new platforms for single molecule analysis. However, methods for controlling the permeability of nanopores are very limited. Here, we show how nanopores functionalized with poly(ethylene glycol) brushes, which fully prevent protein translocation, can be reversibly gated to an "open" state by binding of single IgG antibodies that disrupt the macromolecular barrier. On the basis of surface plasmon resonance data we propose a two-state model describing the antibody-polymer interaction kinetics. Reversibly (weakly) bound antibodies decrease the protein exclusion height while irreversibly (strongly) bound antibodies do not. Our results are further supported by fluorescence readout from pore arrays and high-speed atomic force microscopy on single pores. This type of dynamic barrier control on the nanoscale provides new possibilities for biomolecular separation and analysis.
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| 7. |
- Emilsson, Gustav, et al.
(författare)
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Nanoplasmonic Sensor Detects Preferential Binding of IRSp53 to Negative Membrane Curvature
- 2019
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Ingår i: Frontiers in Chemistry. - : Frontiers Media SA. - 2296-2646. ; 7:FEB
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Tidskriftsartikel (refereegranskat)abstract
- Biosensors based on plasmonic nanostructures are widely used in various applications and benefit from numerous operational advantages. One type of application where nanostructured sensors provide unique value in comparison with, for instance, conventional surface plasmon resonance, is investigations of the influence of nanoscale geometry on biomolecular binding events. In this study, we show that plasmonic "nanowells" conformally coated with a continuous lipid bilayer can be used to detect the preferential binding of the insulin receptor tyrosine kinase substrate protein (IRSp53) I-BAR domain to regions of negative surface curvature, i.e., the interior of the nanowells. Two different sensor architectures with and without an additional niobium oxide layer are compared for this purpose. In both cases, curvature preferential binding of IRSp53 (at around 0.025 nm(-1) and higher) can be detected qualitatively. The high refractive index niobium oxide influences the near field distribution and makes the signature for bilayer formation less clear, but the contrast for accumulation at regions of negative curvature is slightly higher. This work shows the first example of analyzing preferential binding of an average-sized and biologically important protein to negative membrane curvature in a label-free manner and in real-time, illustrating a unique application for nanoplasmonic sensors.
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| 8. |
- Emilsson, Gustav, 1989, et al.
(författare)
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Polymer brushes in solid-state nanopores form an impenetrable entropic barrier for proteins
- 2018
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3372 .- 2040-3364. ; 10:10, s. 4663-4669
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Tidskriftsartikel (refereegranskat)abstract
- Polymer brushes are widely used to prevent the adsorption of proteins, but the mechanisms by which they operate have remained heavily debated for many decades. We show conclusive evidence that a polymer brush can be a remarkably strong kinetic barrier towards proteins by using poly(ethylene glycol) grafted to the sidewalls of pores in 30 nm thin gold films. Despite consisting of about 90% water, the free coils seal apertures up to 100 nm entirely with respect to serum protein translocation, as monitored label-free through the plasmonic activity of the nanopores. The conclusions are further supported by atomic force microscopy and fluorescence microscopy. A theoretical model indicates that the brush undergoes a morphology transition to a sealing state when the ratio between the extension and the radius of curvature is approximately 0.8. The brush-sealed pores represent a new type of ultrathin filter with potential applications in bioanalytical systems.
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| 9. |
- Emilsson, Gustav, 1989, et al.
(författare)
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Surface plasmon resonance methodology for monitoring polymerization kinetics and morphology changes of brushes-evaluated with poly(N-isopropylacrylamide)
- 2017
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Ingår i: Applied Surface Science. - : Elsevier BV. - 0169-4332. ; 396, s. 384-392
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Tidskriftsartikel (refereegranskat)abstract
- Polymerization from surfaces and the resulting “brushes” have many uses in the development of novel materials and functional interfaces. However, it is difficult to accurately monitor the polymerization rate, which limits the use of polymer brushes in applications where control of thickness is desirable. We present a new methodology based on angular surface plasmon resonance (SPR) which provides real-time measurements of the thickness evolution during atom transfer radical polymerization, using poly(N-isopropylacrylamide) as an example. Our data analysis shows that the growth is linear with a rate of ?20 nm/min in a water/methanol mixture up to ?100 nm after which chain termination gradually reduces the growth rate. Further, we introduce an improved method in SPR which makes it possible to determine changes in brush height and refractive index during switching of responsive polymers. The ratio between heights in the coil to globule transition at 32 °C in water was found to be almost 5, independent of the initial absolute height up to ?200 nm, in agreement with theory. Complementary quartz crystal microbalance and atomic force microscopy data confirm the accuracy of our results. With the methodology presented here the established SPR technique can be used for quantitative characterization of surface-initiated polymerization and responsive polymer brushes.
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| 10. |
- Ferhan, Abdul Rahim, et al.
(författare)
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Nanoplasmonic Sensing Architectures for Decoding Membrane Curvature-Dependent Biomacromolecular Interactions
- 2018
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Ingår i: Analytical Chemistry. - : American Chemical Society (ACS). - 0003-2700 .- 1520-6882. ; 90:12, s. 7458-7466
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Tidskriftsartikel (refereegranskat)abstract
- Nanoplasmonic sensors have emerged as a promising measurement approach to track biomacromolecular interactions involving lipid membrane interfaces. By taking advantage of nanoscale fabrication capabilities, it is possible to design sensing platforms with various architectural configurations. Such capabilities open the door to fabricating lipid membrane-coated nanoplasmonic sensors with varying degrees of membrane curvature in order to understand how biomacromolecular interaction processes are influenced by membrane curvature. Herein, we employed an indirect nanoplasmonic sensing approach to characterize the fabrication of supported lipid bilayers (SLBs) on silica-coated nanowell and nanodisk sensing platforms and to investigate how membrane curvature influences membrane-peptide interactions by evaluating the corresponding measurement responses from different spectral signatures that are sensitive to specific regions of the sensor geometries. SLBs were prepared by the vesicle fusion method, as monitored in real-time by nanoplasmonic sensing measurements and further characterized by fluorescence recovery after photobleaching (FRAP) experiments. By resolving different spectral signatures in the nanoplasmonic sensing measurements, it was determined that peptide binding induces membrane disruption at positively curved membrane regions, while peptide binding without subsequent disruption was observed at planar and negatively curved regions. These findings are consistent with the peptide's known preference to selectively form pores in positively curved membranes, providing validation to the nanoplasmonic sensing approach and highlighting how the integration of nanoplasmonic sensors with different nanoscale architectures can be utilized to study the influence of membrane curvature on biomacromolecular interaction processes.
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