Publikationen
Lin, Yuexi | Bhatti, Muniba | David, Michael S. | Brasse, Yannic | Harberts, Jann | Kister, Thomas | Dervisevic, Muamer | Kraus, Tobias | Voelcker, Nicolas H.
DOI:
Wearable electrochemical biosensors offer a promising alternative to conventional invasive blood-based methods for monitoring biomarkers in diagnostic or therapeutic applications. Microneedle (MN)-based technology provides direct access to the skin's interstitial fluid (ISF), enabling real-time monitoring of biomarkers. Nevertheless, current micro- and nanofabrication techniques do not adequately support the development of MN-based wearable technology that can utilize soft hybrid conductive inks, limiting its use in transdermal biosensing. Herein, an MN-based biosensing platform is developed by integrating 3D printing, soft lithography, and hybrid conductive ink technology, featuring a fenestrated MN shell (FMNS) that serves as a protective layer for the inner hybrid conductive ink coating and prevents delamination during skin application. This FMNS patch demonstrates a wide pH monitoring range, high selectivity and accurate detection of subtle ISF pH changes, safe integration of hybrid conductive inks, and reduced fabrication time and cost when compared to other microfabrication methods such as lithography and deep reactive ion etching. The biosensor excels in protecting the biosensing layer and demonstrates excellent analytical performance in monitoring changes in pH levels of the skin ISF. This micro- and nanofabrication approach has great potential in integrating hybrid conductive ink technology into transdermal wearable devices for health monitoring and diagnostics.
Alam, Shawon | Kister, Thomas | Scholz, Alexander | Sauva, Sophie | Lay, Makara | Kraus, Tobias | Aghassi-Hagmann, Jasmin
DOI:
In this work, we present a proof-of-concept demonstration of inkjet-printed resistive temperature sensors based on nanoparticle platinum ink on flexible polyimide substrates. The resistive temperature sensors are designed as meander structures with a target nominal resistance of 100 and 1000 Ω to be compared to conventional bulk Pt100 and Pt1000 resistors. Thermogravimetric analysis and in situ resistance measurements identified 250°C as the optimal sintering temperature, enabling sufficient solvent removal for conductive structure formation while avoiding Pt surface oxidation and polyimide substrate degradation. Electrical characterization in the 20°C–80°C range revealed a linear relationship between resistance and temperature with effective temperature coefficients of resistance (~48%/57%) and sensitivities (~72%/87%) compared to Pt100/Pt1000 standards, respectively. Mechanical testing over 400 bending cycles showed less than 1% change in electrical resistance, confirming robust flexibility. This study demonstrates the feasibility of translating nanoparticle Pt-based resistive temperature sensors into flexible and automotive sensing applications, offering low-temperature processability, stable temperature coefficients of resistance, linear sensitivity, mechanical robustness, and chemical stability across 20°C–80°C range.
Scholz, Alexander | Alam, Shawon | Hadrich, Wacime | Schröder, André | Wolfer, Tim | Friedrich, Martin | Kister, Thomas | Lay, Makara | Sauva, Sophie | Passlack, Ulrike | Campana, Manuel | Koker, Liane | Sikora, Axel | Kraus, Tobias | Aghassi-Hagmann, Jasmin
DOI:
Flexible hybrid electronics allow for seamless integration of sensing functionalities within materials, non-conformal surfaces and products and thus can enable novel value chains. Next to new functionalities, product authenticity plays a crucial role in complex global supply chains. This holds especially true, when products are deployed in critical environments, such as the industrial or automotive sector, where product failure can be fatal. In this work, we present a secure hybrid system, which contains a custom-designed, thinned ASIC in foil, as well as two printed temperature sensing elements that are seamlessly embedded in an industrial process fabricated automotive coolant hose and an inkjet-printed unique identifier in the form of a physically unclonable function to derive the system’s authenticity. We show the results of the standalone hose-integrated temperature sensors, the bulk ASIC verification results prior to thinning and foil integration, as well as the fully assembled integrated hybrid system. The thinned ASIC in foil communication interfaces, its circuit building blocks, as well as the integrated printed components were successfully commissioned. We show the obtained temperature response as well as the unique identification by generating the challenge response pairs of the physically unclonable function over 1000 repetitions. The security circuit shows only 0.0084% of flipped bits at T = 25 °C, which makes it well suited to be used as physically unclonable function.
Nexha, Albenc | Mariani, Stefano | Cikalleshi, Kliton | Kister, THomas | Mazzolai, Barbara | Kraus, Tobias
DOI:
Plant-inspired soft robots enable distributed environmental monitoring. Fliers, i.e. soft robots that are carried passively by the wind, can be effectively deployed and cover large areas and distances. State-of-the-art fliers for humidity sensing are largely composed of electronic components, which increase cost and generate electronic waste. Here, we introduce self-deployable and biodegradable fliers inspired by natural Ailanthus altissima seeds. These artificial fliers are composed of fluorescent, cellulose-based composites with sensing capabilities. The material is shaped into artificial seeds using scalable 3D extrusion processing. Red-emitting Mn2+-doped Er3+, Yb3+:NaYF4 nanoparticles in the composite provide a strong optical emission upon excitation at 980 nm wavelength. The cellulose matrix absorbs water, which quenches the intensity of fluorescence of the nanoparticles. Increasing humidity thus changes the color of the fluorescence emission from red to green. We used ratiometric sensing to detect the humidity of the surroundings.
Mustafa, H. | Nexha, Albenc | Kister, Thomas | Bartholomeus, H. | Kraus, Tobias | Kooistra, L.
DOI:
Lanthanide-doped upconversion microparticles (UCMP) enable composites for luminescence thermometry with long luminescence lifetime and narrowband absorption and emission spectra. Being non-toxic, easily synthesizable, and having a bright, stable emission makes them an attractive candidate for in-vivo monitoring of key environmental parameters such as temperature. We use them to create soft, biodegradable, miniaturized seed-like robots endowed with fluorescence tags for the sustainable environmental monitoring of topsoil and air above soil environments. Our aim is an airborne platform with a sufficient signal-to-noise ratio to identify the concentration of targeted soil parameters. Here, we study the photoluminescence of Er, Yb: NaYF4 UCMPs embedded in polylactic acid (PLA) polymeric matrix to assess their suitability for remote read-out. We assessed the signal-to-noise ratio in terms of excitation intensity, UCMP concentration, working distance, and sample orientation. We evaluated the signal stability over long exposure time as well as for amplitude-modulated excitation. Finally, we carried out ratiometric and lifetime measurements of luminescence emission in order to demonstrate the feasibility of such sensors in measuring the variation of temperature. Overall, the rare-earth doped UCMPs embedded in biodegradable polymer can be used for remote thermometry, displaying a significant signal-to-noise ratio for luminescence emission detection and subsequent derivation of temperature.

Burgstaller, Anna | Piernitzki, Nils | Küchler, Nadja | Koch, Marcus | Kister, Thomas | Eichler, Hermann | Kraus, Tobias | Schwarz, Eva C. | Dustin, Michael | Lautenschlaeger, Franziska | Staufer, Oskar
DOI:
The expansion of T cells ex vivo is crucial for effective immunotherapy but currently limited by a lack of expansion approaches that closely mimic in vivo T cell activation. Taking inspiration from bottom-up synthetic biology, a new synthetic cell technology is introduced based on dispersed liquid-liquid phase-separated droplet-supported lipid bilayers (dsLBs) with tunable biochemical and biophysical characteristics, as artificial antigen presenting cells (aAPCs) for ex vivo T cell expansion. These findings obtained with the dsLB technology reveal three key insights: first, introducing laterally mobile stimulatory ligands on soft aAPCs promotes expansion of IL-4/IL-10 secreting regulatory CD8+ T cells, with a PD-1 negative phenotype, less prone to immune suppression. Second, it is demonstrated that lateral ligand mobility can mask differential T cell activation observed on substrates of varying stiffness. Third, dsLBs are applied to reveal a mechanosensitive component in bispecific Her2/CD3 T cell engager-mediated T cell activation. Based on these three insights, lateral ligand mobility, alongside receptor- and mechanosignaling, is proposed to be considered as a third crucial dimension for the design of ex vivo T cell expansion technologies.
Cikalleshi, Kliton | Nexha, Albenc | Kister, Thomas | Ronzan, Marilena | Mondini, Alessio | Mariani, Stefano | Kraus, Tobias | Mazzolai, Barbara
DOI:
Continuous and distributed monitoring of environmental parameters may pave the way for developing sustainable strategies to tackle climate challenges. State-of-the-art technologies, made with electronic systems, are often costly, heavy, and generate e-waste. Here, we propose a new generation of self-deployable, biocompatible, and luminescent artificial flying seeds for wireless, optical, and eco-friendly monitoring of environmental parameters (i.e., temperature). Inspired by natural Acer campestre plant seeds, we developed three-dimensional functional printed luminescent seed–like fliers, selecting polylactic acid as a biocompatible matrix and temperature as a physical parameter to be monitored. The artificial seeds mimic the aerodynamic and wind dispersal performance of the natural ones. The sensing properties are given by the integration of fluorescent lanthanide–doped particles, whose photoluminescence properties depend on temperature. The luminescent artificial flying seeds can be optically read from a distance using eye-safe near-infrared wavelengths, thus acting as a deployable sensor for distributed monitoring of topsoil environmental temperatures.
Kister, Thomas | Maurer, Johannes H. M. | González-García, Lola | Kraus, Tobias
DOI:
Metal grids with submicron line diameters are optically transparent, mechanically flexible, and suitable materials for transparent and flexible electronics. Printing such narrow lines with dilute metal nanoparticle inks is challenging because it requires percolation throughout the particle packing. Here, we print fully connected submicron lines of 3.2 nm diameter gold nanoparticles and vary the organic ligand shell to study the relation between colloidal interactions, ligand binding to the metal core, and conductivity of the printed lines. We find that particles with repulsive potentials aid the formation of continuous lines, but the required long ligand molecules impede conductivity and need to be removed after printing. Weakly bound alkylamines provided sufficient interparticle repulsion and were easy to remove with a soft plasma treatment after printing, so that grids with a transparencies above 90% and a conductivity of 150 Ω sq–1 could be printed.
Kister, Thomas | Monego, Debora | Mulvaney, Paul | Widmer-Cooper, Asaph | Kraus, Tobias
DOI:
Being able to predict and tune the colloidal stability of nanoparticles is essential for a wide range of applications, yet our ability to do so is currently poor due to a lack of understanding of how they interact with one another. Here, we show that the agglomeration of apolar particles is dominated by either the core or the ligand shell, depending on the particle size and materials. We do this by using Small-Angle X-ray Scattering and molecular dynamics simulations to characterize the interaction between hexadecanethiol passivated gold nanoparticles in decane solvent. For smaller particles, the agglomeration temperature and interparticle spacing are determined by ordering of the ligand shell into bundles of aligned ligands that attract one another and interdigitate. In contrast, the agglomeration of larger particles is driven by van der Waals attraction between the gold cores, which eventually becomes strong enough to compress the ligand shell. Our results provide a microscopic description of the forces that determine the colloidal stability of apolar nanoparticles and explain why classical colloid theory fails.
Wintzheimer, Susanne | Granath, Tim | Oppmann, Maximilian | Kister, Thomas | Thai, Thibaut | Kraus, Tobias | Vogel, Nicolas | Mandel, Karl
DOI:
Under the right process conditions, nanoparticles can cluster together to form defined particular structures, which can be termed supraparticles. Controlling the size, shape, and morphology of such entities is a central step in various fields of science and technology, ranging from colloid chemistry and soft matter physics to powder technology and pharmaceutical and food sciences. These diverse scientific communities have been investigating formation processes and structure/property relations of such supraparticles under completely different boundary conditions. On the fundamental side, the field is driven by the desire to gain maximum control of the assembly structures using very defined and tailored colloidal building-blocks, while more applied disciplines focus on optimizing the functional properties from rather ill-defined starting materials. With this review article, we aim to provide a connecting perspective by outlining fundamental principles that govern the formation and functionality of supraparticles. We discuss the formation of supraparticulates as a result of colloidal properties interplaying with external process parameters. We then outline how the structure of the supraparticles gives rise to different functional properties. They can be a result of the structure itself (emergent properties), of the colocalization of different, functional building-blocks, or of coupling between individual particles in close proximity. Taken together, we aim to establish structure-property and process-structure relationships that provide unifying guidelines for the rational design of functional supraparticles with optimized properties. Finally, we aspire to connect the different disciplines by providing a categorized overview of the existing, diverging nomenclature of seemingly similar supraparticle structures.
