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Karol Kołątaj

Publications and source records attributed to Karol Kołątaj.

4 recordsLinked to original sources

Modifying Electrochemical Doping in Light-Emitting Electrochemical Cells with Gold Nanoparticles

Electrochemical doping offers dynamic control of the electronic properties of organic semiconductors, and it is the enabling feature of a range of technologies, including electrochemical transistors, energy-storage devices, light-emitting electrochemical cells (LECs), and bioelectronics. Electrochemical doping is commonly controlled by the selection of the constituents in the active material of the device or the applied voltage bias, but herein we report that the incorporation of Au nanoparticles (Au-NPs) at an electrode interface can constitute an alternative control parameter. The LEC features balanced p- and n-type electrochemical doping that forms a p-n junction doping structure in its active material, and we find that it is possible to reshape this doping profile by incorporating Au-NPs at an electrode interface. Specifically, we establish that the inclusion of neat non-capped Au-NPs at the anodic interface shifts the p-n junction (i.e., the emission zone) away from the anode. In contrast, the inclusion of Au-NPs capped with sodium citrate is found to reverse this behavior, so that the emission zone is instead moved towards the anode. We utilize this control parameter to shift the emission zone towards a position of constructive (destructive) interference, as manifested in a strong increase (decrease) of the LEC emission efficiency. Our findings establish an interfacial strategy for modulating the spatial profile of electrochemical doping and tuning device performance without altering the chemistry of the active material, relying instead on the surface modification of one electrode. This approach is important because it provides a versatile and minimally invasive route to optimize electrochemical devices while preserving the intrinsic properties and formulation of the active material.

cond-mat.mtrl-sci↗

DNA-Origami-Assembled Rhodium Nanoantennas for Deep-UV Label-Free Single-Protein Detection

Nanoparticles of plasmonic metals have significantly to the development of spectroscopic techniques, enabling strong confinement of electromagnetic fields at the nanoscale and corresponding signal amplification. However, to date, plasmonic applications have been limited mainly to the visible and near-infrared range, as materials supporting ultraviolet resonances typically exhibit poor chemical stability and lack robust surface functionalisation methods. In this work, we address these limitations by introducing a fully programmable approach to UV plasmonics based on rhodium nanocube dimers assembled using DNA origami templates. We have developed a reliable ligand exchange strategy that allows the functionalisation of rhodium nanocubes with DNA while maintaining their colloidal stability. These DNA-modified nanocubes act as modular building blocks that can be assembled into dimers with 69% efficiency and an average gap size of 10 nm. The DNA origami design also allows for the deterministic placement of a single streptavidin protein in the plasmonic gap, unlike previous methods based on stochastic diffusion. Experiments with single-molecule autofluorescence in UV, supported by numerical simulations, show an increase in brightness of up to 22, a reduction in fluorescence lifetime, and a more than tenfold increase in the total number of detected photons. By creating a robust and versatile platform for the production of UV-resonant plasmonic nanoantennas, this work extends the functionality of plasmonics to the deep UV spectrum and opens up new possibilities for labelling-free single-protein spectroscopy.

physics.optics↗

UV-SERS monitoring of plasmons photodegradation of biomolecules on Aluminum platforms decorated with Rhodium nanoparticles

In the search for novel nanostructured materials for UV plasmonics a limited number of choices can be done. Materials such as aluminum, rhodium, gallium and few others can be used. One of the most interesting application for UV plasmonics is Surface Enhanced Raman Spectroscopy. It can be extended to this spectral range to explore spectral properties of biomolecules that have only a small cross section in the visible spectral range. We have recently reported on a functional substrates based on nanoporous aluminum decorated with rhodium nanoparticles. This system showed an interesting behavior for UV excitation at 266 nm, with an unexpected decreasing Raman intensity for increasing rhodium nanoparticles concentrations. We proposed that this effect can be due to the difficult access to the hot spots for the molecules deposited via thermal evaporation. Here we extend this study exploring the performance of the system at another UV excitation wavelengths (325 nm) reporting on experimental results obtained using a deposition process that can bring the molecules at the hot-spots in a more efficient way. Extensive spectroscopic acquisitions, combined with 3D maps, allow to shade a more clear view on the performance of this plasmonic platform. In particular, the photodegration and the potential oxidation of biomolecules driven by the hot-electron/hot-holes produced by the rhodium nanoparticles will be reported.

physics.app-ph↗

Distance dependent interaction between a single emitter and a single dielectric nanoparticle using DNA origami

Optical nanoantennas can manipulate light-matter interactions at the nanoscale, modifying the emission properties of nearby single photon emitters. To date, most optical antennas are based on metallic nanostructures that exhibit unmatched performance in terms of electric field enhancement but suffer from substantial ohmic losses that limit their applications. To circumvent these limitations, there is a growing interest in alternative materials. In particular, high-refractive-index dielectrics have emerged as promising candidates, offering negligible ohmic losses, and supporting both electric and magnetic resonances in the visible and near-infrared range that can unlock novel effects. Currently, the few available studies on dielectric nanoantennas focus on ensemble measurements. Here, we exploit the DNA origami technique to study the interaction between silicon nanoparticles and organic fluorophores at the single molecule level, in controlled geometries and at different spectral ranges within the visible spectrum. We characterize their distance-dependent interaction in terms of fluorescence intensity and lifetime, revealing a significant modification of the decay rate together with minimal quenching and a high fluorescence quantum yield even at short distances from the dielectric nanoparticle. This work demonstrates the advantages of dielectric nanoantennas over their metallic counterparts and paves the way for their applications in single-molecule spectroscopy and sensing.

physics.optics↗