03 Fakultät Chemie
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/4
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Item Open Access Designing covalent organic framework‐based light‐driven microswimmers toward therapeutic applications(2023) Sridhar, Varun; Yildiz, Erdost; Rodríguez‐Camargo, Andrés; Lyu, Xianglong; Yao, Liang; Wrede, Paul; Aghakhani, Amirreza; Akolpoglu, Birgul M.; Podjaski, Filip; Lotsch, Bettina V.; Sitti, MetinWhile micromachines with tailored functionalities enable therapeutic applications in biological environments, their controlled motion and targeted drug delivery in biological media require sophisticated designs for practical applications. Covalent organic frameworks (COFs), a new generation of crystalline and nanoporous polymers, offer new perspectives for light‐driven microswimmers in heterogeneous biological environments including intraocular fluids, thus setting the stage for biomedical applications such as retinal drug delivery. Two different types of COFs, uniformly spherical TABP‐PDA‐COF sub‐micrometer particles and texturally nanoporous, micrometer‐sized TpAzo‐COF particles are described and compared as light‐driven microrobots. They can be used as highly efficient visible‐light‐driven drug carriers in aqueous ionic and cellular media. Their absorption ranging down to red light enables phototaxis even in deeper and viscous biological media, while the organic nature of COFs ensures their biocompatibility. Their inherently porous structures with ≈2.6 and ≈3.4 nm pores, and large surface areas allow for targeted and efficient drug loading even for insoluble drugs, which can be released on demand. Additionally, indocyanine green (ICG) dye loading in the pores enables photoacoustic imaging, optical coherence tomography, and hyperthermia in operando conditions. This real‐time visualization of the drug‐loaded COF microswimmers enables unique insights into the action of photoactive porous drug carriers for therapeutic applications.Item Open Access Dynamic ultrasound projector controlled by light(2022) Ma, Zhichao; Joh, Hyungmok; Fan, Donglei Emma; Fischer, PeerDynamic acoustic wavefront control is essential for many acoustic applications, including biomedical imaging and particle manipulation. Conventional methods are either static or in the case of phased transducer arrays are limited to a few elements and hence limited control. Here, a dynamic acoustic wavefront control method based on light patterns that locally trigger the generation of microbubbles is introduced. As a small gas bubble can effectively stop ultrasound transmission in a liquid, the optical images are used to drive a short electrolysis and form microbubble patterns. The generation of microbubbles is controlled by structured light projection at a low intensity of 65 mW cm-2 and only requires about 100 ms. The bubble pattern is thus able to modify the wavefront of acoustic waves from a single transducer. The method is employed to realize an acoustic projector that can generate various acoustic images and patterns, including multiple foci and acoustic phase gradients. Hydrophone scans show that the acoustic field after the modulation by the microbubble pattern forms according to the prediction. It is believed that combining a versatile optical projector to realize an ultrasound projector is a general scheme, which can benefit a multitude of applications based on dynamic acoustic fields.Item Open Access Soft urinary bladder phantom for endoscopic training(2021) Choi, Eunjin; Waldbillig, Frank; Jeong, Moonkwang; Li, Dandan; Goyal, Rahul; Weber, Patricia; Miernik, Arkadiusz; Grüne, Britta; Hein, Simon; Suarez-Ibarrola, Rodrigo; Kriegmair, Maximilian Christian; Qiu, TianBladder cancer (BC) is the main disease in the urinary tract with a high recurrence rate and it is diagnosed by cystoscopy (CY). To train the CY procedures, a realistic bladder phantom with correct anatomy and physiological properties is highly required. Here, we report a soft bladder phantom (FlexBlad) that mimics many important features of a human bladder. Under filling, it shows a large volume expansion of more than 300% with a tunable compliance in the range of 12.2 ± 2.8 - 32.7 ± 5.4 mL cmH2O-1 by engineering the thickness of the bladder wall. By 3D printing and multi-step molding, detailed anatomical structures are represented on the inner bladder wall, including sub-millimeter blood vessels and reconfigurable bladder tumors. Endoscopic inspection and tumor biopsy were successfully performed. A multi-center study was carried out, where two groups of urologists with different experience levels executed consecutive CYs in the phantom and filled in questionnaires. The learning curves reveal that the FlexBlad has a positive effect in the endourological training across different skill levels. The statistical results validate the usability of the phantom as a valuable educational tool, and the dynamic feature expands its use as a versatile endoscopic training platform.Item Open Access Light- and magnetically actuated FePt microswimmers(2021) Kadiri, Vincent Mauricio; Günther, Jan-Philipp; Kottapalli, Sai Nikhilesh; Goyal, Rahul; Peter, Florian; Alarcón-Correa, Mariana; Son, Kwanghyo; Barad, Hannah-Noa; Börsch, Michael; Fischer, PeerExternally controlled microswimmers offer prospects for transport in biological research and medical applications. This requires biocompatibility of the swimmers and the possibility to tailor their propulsion mechanisms to the respective low Reynolds number environment. Here, we incorporate low amounts of the biocompatible alloy of iron and platinum (FePt) in its L10 phase in microstructures by a versatile one-step physical vapor deposition process. We show that the hard magnetic properties of L10 FePt are beneficial for the propulsion of helical micropropellers with rotating magnetic fields. Finally, we find that the FePt coatings are catalytically active and also make for Janus microswimmers that can be light-actuated and magnetically guided.Item Open Access Deposition and characterization of multi-functional, complex thin films using atomic layer deposition for copper corrosion protection(2022) Dogan, Gül; Schütz, Gisela (Prof. Dr.)This thesis focuses on ALD thin film protection properties against corrosion of copper to develop an understanding of material interface properties and to develop novel thin films processes. This understanding is then applied to enhance materials with potential use in semiconductor devices. The main research objectives are listed below: Understanding corrosion protection properties of ALD thin films: - Development of protective thin films by combining different oxide layers - To characterize the protection properties at high temperatures and in aggressive environments, - To understand the interaction of copper and ALD protection layers when exposed to high temperatures, - Finding the optimum deposition parameters to achieve defect-free thin layers for best corrosion protection Application of ALD oxide thin films for copper corrosion protection in semiconductor devices: - Structuring the ALD thin films to make reliable interface for copper-copper interconnects with micromachining methods such as laser drilling and plasma etching - To remove ALD layers in a localized, selective way without degradation of the underlying copper layerItem Open Access Chemically active micromotors(2021) Yu, Tingting; Fischer, Peer (Prof. Dr.)Item Open Access A complementary experimental and theoretical approach for probing the surface functionalization of ZnO with molecular catalyst linkers(2023) Kousik, Shravan R.; Solodenko, Helena; YazdanYar, Azade; Kirchhof, Manuel; Schützendübe, Peter; Richter, Gunther; Laschat, Sabine; Fyta, Maria; Schmitz, Guido; Bill, Joachim; Atanasova, PetiaThe application of ZnO materials as solid-state supports for molecular heterogeneous catalysis is contingent on the functionalization of the ZnO surface with stable self-assembled monolayers (SAMs) of catalyst linker molecules. Herein, experimental and theoretical methods are used to study SAMs of azide-terminated molecular catalyst linkers with two different anchor groups (silane and thiol) on poly and monocrystalline (0001, ) ZnO surfaces. Angle-resolved and temperature-dependent X-ray photoelectron spectroscopy (XPS) is used to study SAM binding modes, thermal stabilities, and coverages. The binding strengths and atomistic ordering of the SAMs are determined via atom-probe tomography (APT). Density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations provide insights on the influence of the ZnO surface polarity on the interaction affinity and conformational behavior of the SAMs. The investigations show that SAMs based on 3-azidopropyltriethoxysilane possess a higher binding strength and thermal stability than the corresponding thiol. SAM surface coverage is strongly influenced by the surface polarity of ZnO, and the highest coverage is observed on the polycrystalline surface. To demonstrate the applicability of linker-modified polycrystalline ZnO as a catalyst support, a chiral Rh diene complex is immobilized on the azide-terminal of the SAM and its coverage is evaluated via XPS.Item Open Access Soft materials for acoustic applications(2022) Choi, Eunjin; Fischer, Peer (Prof. Dr.)Ultrasound finds wide application in imaging and testing because ultrasound can penetrate tissue and is benign. Gaseous microbubbles strongly scatter ultrasound and are therefore used as contrast agents. Ultrasound responsive materials can be used for many industrial and biomedical applications. Ultrasound can also be used to exert forces and manipulate particles solution and biological cells. In this thesis, material systems are developed for three application areas: 1) models of human organs for the quantitative evaluation of surgical procedures with ultrasound; 2) the fabrication of soft objects by assembling polymeric particles with ultrasound and the acoustic hologram; and 3) the characterization of antibubbles as novel contrast agents that can carry a fluid load. Organ phantoms serve as tools in medical fields to train and plan medical procedures. However, current organ phantoms miss important features or are not realistic. Current models tend to possess a Young’s modulus that is much higher than that of tissue. Furthermore, many of the current models do not show the correct contrast in a medical imaging setting. This thesis presents high fidelity organ phantoms that possess the correct elasticity, compliance, optical appearance, and correct ultrasound contrast. One model is developed for cystoscopy (CY) of the bladder. Another phantom for the transurethral resection of the prostate (TURP). The quality of the phantoms is validated by medical practitioners. For CY, the execution time of the medical practitioners is recorded to completely map the inside of the bladder phantom while localizing tumor models that have been embedded in the bladder wall. For TURP, the quality of the resection is compared with ultrasound imaging before and after the surgical simulation. Parameters are defined to quantify the success of the procedure. The phantoms developed as part of this thesis have received high satisfaction scores from medical practitioners. The parameters reflect the experience of the surgeons. In assembling soft matter, one challenge is that existing 3D printing methods are slow. In contrast, the use of ultrasound patterns shaped with a recently invented acoustic hologram allows objects to be built at once. In this thesis, polydimethylsiloxane (PDMS) particles have been assembled into two-dimensional shapes with ultrasound. To fix the assembly, the PDMS has been physically functionalized with an initiator using swelling. Suitable swelling solutions have been determined based on their solubility. The stability of the physisorbed initiators is evaluated, and the functionalized PDMS particles are fixed via photopolymerization after assembly in aqueous polyethylene glycol dimethacrylate (PEG-DMA) solutions. The fabrication steps can be repeated to increase the thickness of structures that are mechanically stable. The antibubble is an emerging ultrasound contrast agent. It has an inverse form to a conventional bubble in that a substance in the core is surrounded by a gaseous layer. The antibubble is acoustically responsive and, compared to conventional microbubbles, can carry a much greater load. In this thesis, the structure of antibubbles is examined. In particular, the volume of the load is quantified, and the amount of gas per bubble is estimated. The stability of the core substance against diffusion is investigated and shown to be stable for over 11 h.Item Open Access Soft liver phantom with a hollow biliary system(2021) Tan, Xiangzhou; Li, Dandan; Jeong, Moonkwang; Yu, Tingting; Ma, Zhichao; Afat, Saif; Grund, Karl-Enrst; Qiu, TianHepatobiliary interventions are regarded as difficult minimally-invasive procedures that require experience and skills of physicians. To facilitate the surgical training, we develop a soft, high-fidelity and durable liver phantom with detailed morphology. The phantom is anatomically accurate and feasible for the multi-modality medical imaging, including computer tomography (CT), ultrasound, and endoscopy. The CT results show that the phantom resembles the detailed anatomy of real livers including the biliary ducts, with a spatial root mean square error (RMSE) of 1.7 ± 0.7 mm and 0.9 ± 0.2 mm for the biliary duct and the liver outer shape, respectively. The sonographic signals and the endoscopic appearance highly mimic those of the real organ. An electric sensing system was developed for the real-time quantitative tracking of the transhepatic puncturing needle. The fabrication method herein is accurate and reproducible, and the needle tracking system offers a robust and general approach to evaluate the centesis outcome.Item Open Access Growth of nanowires and diffusion in bimetallic nanowires : a way to adaptable nanostructures(2023) Suadiye, Eylül; Richter, Gunther (Prof.)