This work is devoted to investigate light confinement in rolled-up microtubular cavities and their optofluidic applications. The microcavities are fabricated by a roll-up mechanism based on releasing pre-strained silicon-oxide nanomembranes. By defining the shape and thickness of the nanomembranes, the geometrical tube structure is well controlled. Micro-photoluminescence spectroscopy at room temperature is employed to study the optical modes and their dependence on the structural characteristics of the microtubes. Finite-difference-time-domain simulations are performed to elucidate the experimental results. In addition, a theoretical model (based on a wave description) is applied to describe the optical modes in the tubular microcavities, supporting quantitatively and qualitatively the experimental findings. Precise spectral tuning of the optical modes is achieved by two post-fabrication methods. One method employs conformal coating of the tube wall with Al2O3 monolayers by atomic-layer-deposition, which permits a mode tuning over a wide spectral range (larger than one free-spectral-range). An average mode tuning to longer wavelengths of 0.11nm/ Al2O3-monolayer is obtained. The other method consists in asymmetric material deposition onto the tube surface. Besides the possibility of mode tuning, this method permits to detect small shape deformations (at the nanometer scale) of an optical microcavity. Controlled confinement of resonant light is demonstrated by using an asymmetric cone-like microtube, which is fabricated by unevenly rolling-up circular-shaped nanomembranes. Localized three-dimensional optical modes are obtained due to an axial confinement mechanism that is defined by the variation of the tube radius and wall windings along the tube axis. Optofluidic functions of the rolled-up microtubes are explored by immersing the tubes or filling their core with a liquid medium. Refractive index sensing of liquids is demonstrated by correlating spectral shift of the optical modes when a liquid interacts with the resonant light of the microtube. In addition, a novel sensing methodology is proposed by monitoring axial mode spacing changes. Lab-on-a-chip methods are employed to fabricate an optofluidic chip device, allowing a high degree of liquid handling. A maximum sensitivity of 880 nm/refractive-index-unit is achieved. The developed optofluidic sensors show high potential for lab-on-a-chip applications, such as real-time bio/chemical analytic systems.

Vertically rolled-up microcavities are fabricated using differentially strained nanomembranes by employing rate and temperature gradients during electron beam evaporation of SiO2. The geometry of the rolled-up tubes is defined by a photo-lithographically patterned polymer sacrificial layer beneath the SiO2 layers that is dissolved to start the rolling. Rolled-up tubes support resonances formed by constructive interference of light propagating along the circumference. Optical studies are performed in the visible spectral range using a micro-photoluminescence (µPL) setup to excite and detect optical modes. Record high quality factors (Q factors) of 5400 for rolled-up resonators probed in PL-emission mode are found and their limits are theoretically investigated. Axial modes can also be supported when an increased winding number in the center is realized by appropriate pattern designs. In addition, higher order radial modes can be confined when atomic layer deposition (ALD) coatings are applied. Both types of modes are identified using polarization and spatially resolved µPL maps. Evanescent-wave coupling by tapered fibers and tubes on substrates is the second method used to study light confinement and to demonstrate frequency filtering in ALD coated rolled-up microcavities. Scans are performed by monitoring light from a tunable laser in the range of 1520-1570 nm after transmission through the tapered fiber. Dips in the spectrum are found and attributed to fundamental and axial resonant modes. Moreover, by coupling two tapered fibers to a lifted rolled-up microcavity, a four-port add-drop filter is demonstrated as a future component for vertical resonant light transfer in on-chip optical networks. Simulations show that the subwavelength tube wall thickness limits the Q factor at infrared wavelengths and ALD coatings are necessary to enhance the light confinement. After coating, two linear polarization states are found in experiment and fundamental and axial modes can be selectively excited by coupling the fiber to different positions along the tube axis. Spatially and polarization resolved transmission maps reveal a polarization dependent axial mode distribution which is verified theoretically. The results of this thesis are important for lab-on-chip applications where rolled-up microcavities are employed as high resolution optofluidic sensors as well as for future uses as waveguide coupled components in three-dimensional multi-level optical data processing units to provide resonant interlayer signal transfer.

By implementing the rolled-up microfabrication method based on strain engineering, several systems are investigated within the contents of this thesis. The structural morphing of planar geometries into three-dimensional structures opens up many doors for the creation of unique material configurations and devices. An exploration into several novel microsystems, encompassing various scientific subjects, is made and methods for on-chip integration of these devices are presented. The roll-up of a metal and oxide allows for a cylindrical hollow-core structure with a cladding layer composed of a multilayer stack, plasmonic metamaterial. This structure can be used as a platform for a number of optical metamaterial devices. By guiding light radially through this structure, a theoretical investigation into the system makeup of a rolled-up hyperlens, is given. Using the same design, but rather propagating light parallel to the cylinder, a novel device known as a metamaterial optical fiber is defined. This fiber allows light to be guided classically and plasmonically within a single device. These fibers are developed experimentally and are integrated into preexisting on-chip structures and characterized. A system known as lab-in-a-tube is introduced. The idea of lab-in-a-tube combines various rolled-up components into a single all-encompassing biosensor that can be used to detect and monitor single bio-organisms. The first device specifically tailored to this system is developed, flexible split-wall microtube resonator sensors. A method for the capturing of embryonic mouse cells into on-chip optical resonators is introduced. The sensor can optically detect, via photoluminescence, living cells confined within the resonator through the compression and expansion of a nanogap built within its walls. The rolled-up fabrication method is not limited to the well-investigated systems based on the roll-up from semiconductor material or from a photoresist layer. A new approach, relying on the delamination of polymers, is presented. This offers never-before-realized microscale structures and configurations. This includes novel magnetic configurations and flexible fluidic sensors which can be designed for on-chip and roving detector applications.

Rolled-up nanotechnology based on strain-engineering is a powerful tool to manufacture three-dimensional hollow structures made of virtually any kind of material on a large variety of substrates. The aim of this thesis is to address the key features of different on- and off-chip applications of rolled-up microtubes through modification of their basic framework. The modification of the framework pertains to the tubular structure, in particular the diameter of the microtube, and the material which it is made of, hence achieving different functionalities of the final rolled-up structure. The tuning of the microtube diameter which is adjusted to the individual size of an object allows on-chip studies of single cells in artificial narrow cavities, for example. Another modification of the framework is the addition of a catalytic layer which turns the microtube into a self-propelled catalytic micro-engine. Furthermore, the tuneability of the diameter can have applications ranging from nanotools for drilling into cells, to cargo transporters in microfluidic channels. Especially rolled-up microtubes based on low-cost and easy to deposit materials, such as silicon oxides, can enable the exploration of novel systems for several scientific topics. The main objective of this thesis is to combine microfluidic features of rolled-up structures with optical sensor capabilities of silicon oxide microtubes acting as optical ring resonators, and to integrate these into a Lab-on-a-Chip system. Therefore, a new concept of microfluidic integration is developed in order to establish an inexpensive, reliable and reproducible fabrication process which also sustains the optical capabilities of the microtubes. These integrated microtubes act as optofluidic refractrometric sensors which detect changes in the refractive index of analytes using photoluminescence spectroscopy. The thesis concludes with a demonstration of a functional portable sensor device with several integrated optofluidic sensors. / Die auf verspannten Dünnschichten basierende „rolled-up nanotechnologie“ ist eine leistungsfähige Methode um dreidimensionale hohle Strukturen (Mikroröhrchen) aus nahezu jeder Art von Material auf einer großen Vielfalt von Substraten herzustellen. Ausgehend von der Möglichkeit der Skalierung des Röhrchendurchmessers und der Modifikation der Funktionalität des Röhrchens durch Einsatz verschiedener Materialien und Oberflächenfunktionalisierungen kann eine große Anzahl an verschiedenen Anwendungen ermöglicht werden. Eine Anwendung behandelt unter anderem on-chip Studien einzelner Zellen wobei die Mikroröhrchen, an die Größe der Zelle angepasste, Reaktionscontainer darstellen. Eine weitere Modifikation der Funktionalität der Mikroröhrchen kann durch das Aufbringen einer katalytischen Schicht realisiert werden, wodurch das Mikroröhrchen zu einem selbstangetriebenen katalytischen Mikro-Motor wird. Hauptziel dieser Arbeit ist es Mikrometer große optisch aktive Glasröhrchen herzustellen, diese mikrofluidisch zu kontaktieren und als Sensoren in Lab-on-a-Chip Systeme zu integrieren. Die integrierten Glasröhrchen arbeiten als optofluidische Ringresonatoren, welche die Veränderungen des Brechungsindex von Fluiden im inneren des Röhrchens durch Änderungen im Evaneszenzfeld detektieren können. Die Funktionsfähigkeit eines Demonstrators wird mit verschiedenen Flüssigkeiten gezeigt, dabei kommt ein Fotolumineszenz Spektrometer zum Anregen des Evaneszenzfeldes und Auslesen des Signals zum Einsatz. Die entwickelte Integrationsmethode ist eine Basis für ein kostengünstiges, zuverlässiges und reproduzierbares Herstellungsverfahren von optofluidischen Mikrochips basierend auf optisch aktiven Mikroröhrchen.

Following the intensive development of isolated (i.e., not coupled with on-chip waveguide) vertically rolled-up microtube ring resonators (VRU-MRRs) for both active and passive applications, a variety of microtube-based devices has been realized. These include microcavity lasers, optical sensors, directional couplers, and active elements in lab-on-a-chip devices. To provide more advanced and complex functionality, the focus of tubular geometry research is now shifting toward (i) refined vertical light transfer in 3D stacks of multiple photonic layers and (ii) to make microfluidic cooling system in the integrated optoelectronic system. Based on this motivation, this PhD research is devoted to the demonstration and the implementation of monolithic integration of VRU-MRRs with photonic waveguides for 3D photonic integration and their optofluidic applications. Prior to integration, high-quality isolated VRU-MRRs on the flat Si substrate are firstly fabricated by the controlled release of differentially strained titanium-dioxide (TiO2) bilayered nanomembranes. The fabricated microtubes support resonance modes for both telecom and visible photonics. The outcome of the isolated VRU-MRRs is a record high Q (≈3.8×10^3) in the telecom wavelength range with optimum tapered optical fiber resonator interaction. To further study the optical modes in the visible and near infrared spectral range, μPL spectroscopy is performed on the isolated VRU-MRRs, which are activated by entrapping various sizes of luminescent nanoparticles (NPs) within the windings of rolled-up nanomembranes based on a flexible, robust and economical method. Moreover, it is realized for the first time, in addition to serving as light sources that NPs-aggregated in isolated VRU-MRRs can produce an optical potential well that can be used to trap optical resonant modes. After achieving all the required parameters for creating a high-quality TiO2 VRU-MRR, the monolithic integration of VRU-MRRs with Si nanophotonic waveguides is experimentally demonstrated, exhibiting a significant step toward 3D photonic integration. The on-chip integration is realized by rolling up 2D pre-strained TiO2 nanomembranes into 3D VRU-MRRs on a microchip which seamlessly expanded over several integrated waveguides. In this intriguing vertical transmission configuration, resonant filtering of optical signals at telecom wavelengths is demonstrated based on ultra-smooth and subwavelength thick-walled VRU-MRRs. Finally, to illustrate the usefulness of the fully integrated VRU-MRRs with photonic waveguides, optofluidic functionalities of the integrated system is investigated. In this work, two methods are performed to explore optofluidic applications of the integrated system. First, the hollow core of an integrated VRU-MRR is uniquely filled with a liquid solution (purified water) by setting one end of the VRU-MRRs in contact with a droplet placed onto the photonic chip via a glass capillary. Second, the outside of an integrated VRU-MRR is fully covered with a big droplet of liquid. Both techniques lead to a significant shift in the WGMs (Δλ≈46 nm). A maximum sensitivity of 140 nm/refractive index unit, is achieved. The achievements of this PhD research open up fascinating opportunities for the realization of massively parallel optofluidic microsystems with more functionality and flexibility for analysis of biomaterials in lab-on-a-tube systems on single chips. It also demonstrates 3D photonic integration in which optical interconnects between multiple photonic layers are required.

Medical devices have made a big step forward in the past decades. One of the most noticeable medical events of the twenties century was the development of long-lasting, wireless electronic implants such as identification tags, pacemakers and neuronal stimulators. These devices were only made possible after the development of small scale radio frequency electronics. Small radio electronic circuits provided a way to operate in both transmission and reception mode allowing an implant to communicate with an external world from inside a living organism. Bidirectional communication is a vital feature that has been increasingly implemented in similar systems to continuously record biological parameters, to remotely configure the implant, or to wirelessly stimulate internal organs. Further miniaturisation of implantable devices to make the operation of the device more comfortable for the patient requires rethinking of the whole radio system concept making it both power efficient and of high performance. Nowadays, high data throughput, large bandwidth, and long term operation requires new radio systems to operate at UHF (ultra-high frequency) bands as this is the most suitable for implantable applications. For instance, the MICS (Medical Implant Communication System) band was introduced for the communication with implantable devices. However, this band could only enable communication at low data rates. This was acceptable for the transmission of telemetry data such as heart beat rate, respiratory and temperature with sub Mbps rates. Novel developments such as neuronal and prosthetic implants require significantly higher data rates more than 10 Mbps that can be achieved with large bandwidth communicating systems operating at higher frequencies in a GHz range. Higher operating frequency would also resolve a strong issue of MICS devices, namely the scale of implants defined by dimensions of antennas used at this band. Operation at 2.4 GHz ISM band was recognized to be the most adequate as it has a moderate absorption in the human body providing a compromise between an antenna/implant scale and a total power efficiency of the communicating system. This thesis addresses a key challenge of implantable radio communicating systems namely an efficient and small scale antenna design which allows a high yield fabrication in a microelectronic fashion. It was demonstrated that a helical antenna design allows the designer to precisely tune the operating frequency, input impedance, and bandwidth by changing the geometry of a self-assembled 3D structure defined by an initial 2D planar layout. Novel stimuli responsive materials were synthesized, and the rolled-up technology was explored for fabrication of 5.5-mm-long helical antenna arrays operating in ISM bands at 5.8 and 2.4 GHz. Characterization and various applications of the fabricated antennas are successfully demonstrated in the thesis.

Over the past two decades, organic semiconductors played a growing part as active layers in several electronic systems such as sensors, field‑effect transistors or light emitting diodes to cite a few. In fact, organic materials offer a high versatility and flexibility. However, pure organic systems often lack stability and robustness, which can be overcome by combining them with inorganic scaffolds. In this work, a conducting polymer, polypyrrole (PPy) is employed to create new sensor elements based on the combination of both inorganic and organic layers. Electrical measurements, infrared spectroscopy and current sensing atomic force microscopy provides a better understanding of the polymer behavior upon immersion in aqueous solutions. The observed discharge in water leads to a straightforward application of the device as an in‑flow sensor for several acids like HCl, H2SO4 and H3PO4. The wide range of sensing concentrations as well as the low detection limit place the present detector among the best reported so far in the literature. In a further step to turn towards lab‑in‑a‑tube devices, tubular‑shaped‑integrated microelectrodes are developed by using the rolled‑up technology. As a proof of concept, the successful integration of PPy as an active layer and its use as a gas sensor for volatile organic compounds (VOCs) is demonstrated. Finally, by adapting the rolled‑up top electrodes, as developed by Bof Bufon et al. for self‑assembled monolayers (SAMs), thin PPy films (<50 nm) are vertically contacted and their electrical characteristics measured as a function of temperature and electric field. From the transport investigations, it is observed that an insulating‑to‑metallic transition occurs in the polymeric film by increasing the bias voltage. Other molecular layers like CuPc can be incorporated in these platforms, opening the way towards emerging organic devices.

Die Menschheit steht vor der großen Herausforderung der Energieversorgung des 21. Jahrhundert. Nirgendwo ist diese noch dringlicher geworden als im Bereich der Energiespeicherung und Umwandlung. Konventionelle Energie kommt hauptsächlich aus fossilen Brennstoffen, die auf der Erde nur begrenzt vorhanden sind, und hat zu einer starken Belastung der Umwelt geführt. Zusätzlich nimmt der Energieverbrauch weiter zu, insbesondere durch die rasante Verbreitung von Fahrzeugen und verschiedener Kundenelektronik wie PCs und Mobiltelefone. Alternative Energiequellen sollten vor einer Energiekrise entwickelt werden. Die Gewinnung erneuerbarer Energie aus Sonne und Wind sind auf jeden Fall sehr wichtig, aber diese Energien sind oft nicht gleichmäßig und andauernd vorhanden. Energiespeichervorrichtungen sind daher von großer Bedeutung, weil sie für eine Stabilisierung der umgewandelten Energie sorgen. Darüber hinaus ist es eine enttäuschende Tatsache, dass der Akku eines Smartphones jeglichen Herstellers heute gerade einen Tag lang ausreicht, und die Nutzer einen zusätzlichen Akku zur Hand haben müssen. Die tragbare Elektronik benötigt dringend Hochleistungsenergiespeicher mit höherer Energiedichte. Der erste Teil der vorliegenden Arbeit beinhaltet Lithium-Ionen-Batterien unter Verwendung von einzelnen aufgerollten Siliziumstrukturen als Anoden, die durch nanotechnologische Methoden hergestellt werden. Eine Lab-on-Chip-Plattform wird für die Untersuchung der elektrochemischen Kinetik, der elektrischen Eigenschaften und die von dem Lithium verursachten strukturellen Veränderungen von einzelnen Siliziumrohrchen als Anoden in einer Lithium-Ionen-Batterie vorgestellt. In dem zweiten Teil wird ein neues Design und die Herstellung von flexiblen on-Chip, Festkörper Mikrosuperkondensatoren auf Basis von MnOx/Au-Multischichten vorgestellt, die mit aktueller Mikroelektronik kompatibel sind. Der Mikrosuperkondensator erzielt eine maximale Energiedichte von 1,75 mW h cm-3 und eine maximale Leistungsdichte von 3,44 W cm-3. Weiterhin wird ein flexibler und faserartig verwebter Superkondensator mit einem Cu-Draht als Substrat vorgestellt. Diese Dissertation wurde im Rahmen des Forschungsprojekts GRK 1215 "Rolled-up Nanotechnologie für on-Chip Energiespeicherung" 2010-2013, finanziell unterstützt von der International Research Training Group (IRTG), und dem PAKT Projekt "Elektrochemische Energiespeicherung in autonomen Systemen, no. 49004401" 2013-2014, angefertigt. Das Ziel der Projekte war die Entwicklung von fortschrittlichen Energiespeichermaterialien für die nächste Generation von Akkus und von flexiblen Superkondensatoren, um das Problem der Energiespeicherung zu addressieren. Hier bedanke ich mich sehr, dass IRTG mir die Möglichkeit angebotet hat, die Forschung in Deutschland stattzufinden. / Human beings are facing the grand energy challenge in the 21st century. Nowhere has this become more urgent than in the area of energy storage and conversion. Conventional energy is based on fossil fuels which are limited on the earth, and has caused extensive environmental pollutions. Additionally, the consumptions of energy are still increasing, especially with the rapid proliferation of vehicles and various consumer electronics like PCs and cell phones. We cannot rely on the earth’s limited legacy forever. Alternative energy resources should be developed before an energy crisis. The developments of renewable conversion energy from solar and wind are very important but these energies are often not even and continuous. Therefore, energy storage devices are of significant importance since they are the one stabilizing the converted energy. In addition, it is a disappointing fact that nowadays a smart phone, no matter of which brand, runs out of power in one day, and users have to carry an extra mobile power pack. Portable electronics demands urgently high-performance energy storage devices with higher energy density. The first part of this work involves lithium-ion micro-batteries utilizing single silicon rolled-up tubes as anodes, which are fabricated by the rolled-up nanotechnology approach. A lab-on-chip electrochemical device platform is presented for probing the electrochemical kinetics, electrical properties and lithium-driven structural changes of a single silicon rolled-up tube as an anode in lithium ion batteries. The second part introduces the new design and fabrication of on chip, all solid-state and flexible micro-supercapacitors based on MnOx/Au multilayers, which are compatible with current microelectronics. The micro-supercapacitor exhibits a maximum energy density of 1.75 mW h cm-3 and a maximum power density of 3.44 W cm-3. Furthermore, a flexible and weavable fiber-like supercapacitor is also demonstrated using Cu wire as substrate. This dissertation was written based on the research project supported by the International Research Training Group (IRTG) GRK 1215 "Rolled-up nanotech for on-chip energy storage" from the year 2010 to 2013 and PAKT project "Electrochemical energy storage in autonomous systems, no. 49004401" from 2013 to 2014. The aim of the projects was to design advanced energy storage materials for next-generation rechargeable batteries and flexible supercapacitors in order to address the energy issue. Here, I am deeply indebted to IRTG for giving me an opportunity to carry out the research project in Germany. September 2014, IFW Dresden, Germany Wenping Si

Vertically rolled-up microcavities are fabricated using differentially strained nanomembranes by employing rate and temperature gradients during electron beam evaporation of SiO2. The geometry of the rolled-up tubes is defined by a photo-lithographically patterned polymer sacrificial layer beneath the SiO2 layers that is dissolved to start the rolling. Rolled-up tubes support resonances formed by constructive interference of light propagating along the circumference. Optical studies are performed in the visible spectral range using a micro-photoluminescence (µPL) setup to excite and detect optical modes. Record high quality factors (Q factors) of 5400 for rolled-up resonators probed in PL-emission mode are found and their limits are theoretically investigated. Axial modes can also be supported when an increased winding number in the center is realized by appropriate pattern designs. In addition, higher order radial modes can be confined when atomic layer deposition (ALD) coatings are applied. Both types of modes are identified using polarization and spatially resolved µPL maps. Evanescent-wave coupling by tapered fibers and tubes on substrates is the second method used to study light confinement and to demonstrate frequency filtering in ALD coated rolled-up microcavities. Scans are performed by monitoring light from a tunable laser in the range of 1520-1570 nm after transmission through the tapered fiber. Dips in the spectrum are found and attributed to fundamental and axial resonant modes. Moreover, by coupling two tapered fibers to a lifted rolled-up microcavity, a four-port add-drop filter is demonstrated as a future component for vertical resonant light transfer in on-chip optical networks. Simulations show that the subwavelength tube wall thickness limits the Q factor at infrared wavelengths and ALD coatings are necessary to enhance the light confinement. After coating, two linear polarization states are found in experiment and fundamental and axial modes can be selectively excited by coupling the fiber to different positions along the tube axis. Spatially and polarization resolved transmission maps reveal a polarization dependent axial mode distribution which is verified theoretically. The results of this thesis are important for lab-on-chip applications where rolled-up microcavities are employed as high resolution optofluidic sensors as well as for future uses as waveguide coupled components in three-dimensional multi-level optical data processing units to provide resonant interlayer signal transfer.

This work is devoted to investigate light confinement in rolled-up microtubular cavities and their optofluidic applications. The microcavities are fabricated by a roll-up mechanism based on releasing pre-strained silicon-oxide nanomembranes. By defining the shape and thickness of the nanomembranes, the geometrical tube structure is well controlled. Micro-photoluminescence spectroscopy at room temperature is employed to study the optical modes and their dependence on the structural characteristics of the microtubes. Finite-difference-time-domain simulations are performed to elucidate the experimental results. In addition, a theoretical model (based on a wave description) is applied to describe the optical modes in the tubular microcavities, supporting quantitatively and qualitatively the experimental findings. Precise spectral tuning of the optical modes is achieved by two post-fabrication methods. One method employs conformal coating of the tube wall with Al2O3 monolayers by atomic-layer-deposition, which permits a mode tuning over a wide spectral range (larger than one free-spectral-range). An average mode tuning to longer wavelengths of 0.11nm/ Al2O3-monolayer is obtained. The other method consists in asymmetric material deposition onto the tube surface. Besides the possibility of mode tuning, this method permits to detect small shape deformations (at the nanometer scale) of an optical microcavity. Controlled confinement of resonant light is demonstrated by using an asymmetric cone-like microtube, which is fabricated by unevenly rolling-up circular-shaped nanomembranes. Localized three-dimensional optical modes are obtained due to an axial confinement mechanism that is defined by the variation of the tube radius and wall windings along the tube axis. Optofluidic functions of the rolled-up microtubes are explored by immersing the tubes or filling their core with a liquid medium. Refractive index sensing of liquids is demonstrated by correlating spectral shift of the optical modes when a liquid interacts with the resonant light of the microtube. In addition, a novel sensing methodology is proposed by monitoring axial mode spacing changes. Lab-on-a-chip methods are employed to fabricate an optofluidic chip device, allowing a high degree of liquid handling. A maximum sensitivity of 880 nm/refractive-index-unit is achieved. The developed optofluidic sensors show high potential for lab-on-a-chip applications, such as real-time bio/chemical analytic systems.