| 1. |
- Shiran Chaharsoughi, Mina, 1986-
(author)
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Hybrid Plasmonics for Energy Harvesting and Sensing of Radiation and Heat
- 2020
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Doctoral thesis (other academic/artistic)abstract
- The special optical properties of subwavelength metallic structures have opened up for numerous applications in different fields. The interaction of light with metal nanostructures leads to the excitation of collective oscillations of conduction-band electrons, known as plasmons. These plasmon excitations are responsible for the high absorption and high scattering of light in metallic nanostructures. High absorption of light and the subsequent temperature increase in the nanostructures make them suitable as point-like heat sources that can be controlled remotely by light.The research presented in this thesis focuses on the development and studies of hybrid devices that combine light-induced heating in plasmonic nanostructures with other materials and systems. Particular focus is put on hybrid organic-inorganic systems for applications in energy harvesting as well as in heat and radiation sensing. Harvesting energy from light fluctuations was achieved in a hybrid device consisting of plasmonic gold nanodisk arrays and a pyroelectric copolymer. In this concept, fast and efficient light-induced heating in the gold nanodisks modulated the temperature of the pyroelectric layer, which could be used to extract electrical energy from fluctuations in simulated sunlight.Integrating plasmonic nanostructures with complementary materials can also provide novel hybrid sensors, for monitoring of temperature, heat flux and radiation. In this thesis work, a hybrid sensor was designed based on the combination of a plasmonic gold nanohole layer with a pyroelectric copolymer and an ionic thermoelectric gel. The gold nanohole arrays acted both as broadband light absorbers in the visible to near-infrared spectral range of the solar spectrum and also as one of the electrodes of the sensor. In contrast to the constituent components when used separately, the hybrid sensor could provide both fast and stable signals upon heat or radiation stimuli, as well as enhanced equilibrium signals.Furthermore, a concept for heat and radiation mapping was developed that was highly sensitive and stable despite its simple structure. The concept consisted of a gel-like electrolyte connecting two separated metal nanohole electrodes on a substrate. Resembling traditional thermocouples, this concept could autonomously detect temperature changes but with several orders of magnitudes higher sensitivity. Owing to its promising sensing properties as well as its compatibility with inexpensive mass production methods on flexible substrates, such concept may be particularly interesting for electronic skin applications for health monitoring and for humanoid robotics. Finally, we improved the possibilities for the temperature mapping of the concept by modifying the structure from lateral to vertical form. Similar to the lateral device, the vertical temperature sensor showed high temperature sensitivity and stability in producing signals upon temperature changes.
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| 2. |
- Winkler, Thomas, Ph.D., et al.
(author)
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Molecular processes in an electrochemical clozapine sensor
- 2017
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In: Biointerphases. - : American Institute of Physics (AIP). - 1934-8630 .- 1559-4106. ; 12:2
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Journal article (peer-reviewed)abstract
- Selectivity presents a crucial challenge in direct electrochemical sensing. One example is schizophrenia treatment monitoring of the redox-active antipsychotic clozapine. To accurately assess efficacy, differentiation from its metabolite norclozapine-similar in structure and redox potentialis critical. Here, the authors leverage biomaterials integration to study, and effect changes in, diffusion and electron transfer kinetics of these compounds. Specifically, the authors employ a catechol-modified chitosan film, which the authors have previously presented as the first electrochemical detection mechanism capable of quantifying clozapine directly in clinical serum. A key finding in our present work is differing dynamics between clozapine and norclozapine once the authors interface the electrodes with chitosan-based biomaterial films. These additional dimensions of redox information can thus enable selective sensing of largely analogous small molecules.
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| 3. |
- Winkler, Thomas, Ph.D., et al.
(author)
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The interplay of electrode- and bio-materials in a redox-cycling-based clozapine sensor
- 2017
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In: Electrochemistry communications. - : Elsevier. - 1388-2481 .- 1873-1902. ; 79, s. 33-36
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Journal article (peer-reviewed)abstract
- We investigate gold, TiN, and platinum in combination with a chitosan catechol-based redox-cycling system (RCS) for electrochemical detection of the antipsychotic clozapine. We have previously demonstrated the RCS for detection of clozapine in serum, but challenges remain regarding low signal-to-noise ratios. This can be mitigated by selection of electrode materials with beneficial surface morphologies and/or compositions. We employ cyclic voltammetry to assess the redox current generated by clozapine, and differentiate solely surface area-based effects from clozapine-specific ones using a standard redox couple. We find that nano- and microstructured platinum greatly amplifies the clozapine signal compared to gold (up to 1490-fold for platinum black). However, the material performs poorly in the presence of chloride ions, and RCS modification provides no further amplification. The RCS combined with atomic-layer-deposited (ALD) TiN, on the other hand, increases the signal by 7.54 times, versus 2.86 times for RCS on gold, with a 9.2-fold lower variability, indicating that the homogenous and chemically inert properties of ALD-TiN may make it an ideal electrode material.
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| 4. |
- Winkler, Thomas, Ph.D., et al.
(author)
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The Role of Microsystems Integration Towards Point-of-Care Clozapine Treatment Monitoring in Schizophrenia.
- 2018
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In: IEEE sensors letters. - : Institute of Electrical and Electronics Engineers (IEEE). - 2475-1472. ; 2:1
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Journal article (peer-reviewed)abstract
- We present a perspective on microsystems integration aspects for concurrent cellular and molecular sensing in a lab-on-a-chip device. While of interest for a range of applications, very few - narrowly focused - examples of such devices can be found in the literature. Here, we approach the challenge from a systems level, considering sensor integration both in parallel and in series. Our study is specifically geared toward schizophrenia treatment, where concurrent blood monitoring of the antipsychotic clozapine and white blood cells could lead to improved treatment outcomes. We evaluate the critical system components for either design, namely plasma skimming (parallel) and in-blood clozapine detection (series). We find that plasma skimming is infeasible, but for the first time demonstrate direct detection of clozapine in whole blood. With a corresponding series-integrated microsystem, we finally demonstrate downstream white blood cell analysis on the same samples using impedance cytometry. We thus present the first lab-on-a-chip device capable of label- and reagent-free concurrent sensing of cellular and molecular markers.
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