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The recent discovery of an intricate and nontrivial interaction topology among the elements of a wide range of natural systems has altered the manner we understand complexity. For example, the axonal fibres transmitting electrical information between cortical regions form a network which is neither regular nor completely random. Their structure seems to follow functional principles to balance between segregation (functional specialisation) and integration. Cortical regions are clustered into modules specialised in processing different kinds of information, e.g. visual or auditory. However, in order to generate a global perception of the real world, the brain needs to integrate the distinct types of information. Where this integration happens, nobody knows. We have performed an extensive and detailed graph theoretical analysis of the cortico-cortical organisation in the brain of cats, trying to relate the individual and collective topological properties of the cortical areas to their function. We conclude that the cortex possesses a very rich communication structure, composed of a mixture of parallel and serial processing paths capable of accommodating dynamical processes with a wide variety of time scales. The communication paths between the sensory systems are not random, but largely mediated by a small set of areas. Far from acting as mere transmitters of information, these central areas are densely connected to each other, strongly indicating their functional role as integrators of the multisensory information. In the quest of uncovering the structure-function relationship of cortical networks, the peculiarities of this network have led us to continuously reconsider the stablished graph measures. For example, a normalised formalism to identify the “functional roles” of vertices in networks with community structure is proposed. The tools developed for this purpose open the door to novel community detection techniques which may also characterise the overlap between modules. The concept of integration has been revisited and adapted to the necessities of the network under study. Additionally, analytical and numerical methods have been introduced to facilitate understanding of the complicated statistical interrelations between the distinct network measures. These methods are helpful to construct new significance tests which may help to discriminate the relevant properties of real networks from side-effects of the evolutionary-growth processes.
In this work the first observation of new type of liquid crystals is presented. This is ionic self-assembly (ISA) liquid crystals formed by introduction of oppositely charged ions between different low molecular tectonic units. As practically all conventional liquid crystals consist of rigid core and alkyl chains the attention is focused to the simplest case where oppositely charged ions are placed between a rigid core and alkyl tails. The aim of this work is to investigate and understand liquid crystalline and alignment properties of these materials. It was found that ionic interactions within complexes play the main role. Presence of these interactions restricts transition to isotropic phase. In addition, these interactions hold the system (like network) allowing crystallization into a single domain from aligned LC state. Alignment of these simple ISA complexes was spontaneous on a glass substrate. In order to show potentials for application perylenediimide and azobenzene containing ISA complexes have been investigated for correlations between phase behavior and their alignment properties. The best results of macroscopic alignment of perylenediimide-based ISA complexes have been obtained by zone-casting method. In the aligned films the columns of the complex align perpendicular to the phase-transition front. The obtained anisotropy (DR = 18) is thermally stable. The investigated photosensitive (azobenzene-based) ISA complexes show formation of columnar LC phases. It was demonstrated that photo alignment of such complexes was very effective (DR = 50 has been obtained). It was shown that photo-reorientation in the photosensitive ISA complexes is cooperative process. The size of domains has direct influence on efficiency of the photo-reorientation process. In the case of small domains the photo-alignment is the most effective. Under irradiation with linearly polarized light domains reorient in the plane of the film leading to macroscopic alignment of columns parallel to the light polarization and joining of small domains into big ones. Finally, the additional distinguishable properties of the ISA liquid crystalline complexes should be noted: (I) the complexes do not solve in water but readily solve in organic solvents; (II) the complexes have good film-forming properties when cast or spin-coated from organic solvent; (III) alignment of the complexes depends on their structure and secondary interactions between tectonic units.
CHAMP (CHAllenging Minisatellite Payload) is a German small satellite mission to study the earth's gravity field, magnetic field and upper atmosphere. Thanks to the good condition of the satellite so far, the planned 5 years mission is extended to year 2009. The satellite provides continuously a large quantity of measurement data for the purpose of Earth study. The measurements of the magnetic field are undertaken by two Fluxgate Magnetometers (vector magnetometer) and one Overhauser Magnetometer (scalar magnetometer) flown on CHAMP. In order to ensure the quality of the data during the whole mission, the calibration of the magnetometers has to be performed routinely in orbit. The scalar magnetometer serves as the magnetic reference and its readings are compared with the readings of the vector magnetometer. The readings of the vector magnetometer are corrected by the parameters that are derived from this comparison, which is called the scalar calibration. In the routine processing, these calibration parameters are updated every 15 days by means of scalar calibration. There are also magnetic effects coming from the satellite which disturb the measurements. Most of them have been characterized during tests before launch. Among them are the remanent magnetization of the spacecraft and fields generated by currents. They are all considered to be constant over the mission life. The 8 years of operation experience allow us to investigate the long-term behaviors of the magnetometers and the satellite systems. According to the investigation, it was found that for example the scale factors of the FGM show obvious long-term changes which can be described by logarithmic functions. The other parameters (offsets and angles between the three components) can be considered constant. If these continuous parameters are applied for the FGM data processing, the disagreement between the OVM and the FGM readings is limited to \pm1nT over the whole mission. This demonstrates, the magnetometers on CHAMP exhibit a very good stability. However, the daily correction of the parameter Z component offset of the FGM improves the agreement between the magnetometers markedly. The Z component offset plays a very important role for the data quality. It exhibits a linear relationship with the standard deviation of the disagreement between the OVM and the FGM readings. After Z offset correction, the errors are limited to \pm0.5nT (equivalent to a standard deviation of 0.2nT). We improved the corrections of the spacecraft field which are not taken into account in the routine processing. Such disturbance field, e.g. from the power supply system of the satellite, show some systematic errors in the FGM data and are misinterpreted in 9-parameter calibration, which brings false local time related variation of the calibration parameters. These corrections are made by applying a mathematical model to the measured currents. This non-linear model is derived from an inversion technique. If the disturbance field of the satellite body are fully corrected, the standard deviation of scalar error \triangle B remains about 0.1nT. Additionally, in order to keep the OVM readings a reliable standard, the imperfect coefficients of the torquer current correction for the OVM are redetermined by solving a minimization problem. The temporal variation of the spacecraft remanent field is investigated. It was found that the average magnetic moment of the magneto-torquers reflects well the moment of the satellite. This allows for a continuous correction of the spacecraft field. The reasons for the possible unknown systemic error are discussed in this thesis. Particularly, both temperature uncertainties and time errors have influence on the FGM data. Based on the results of this thesis the data processing of future magnetic missions can be designed in an improved way. In particular, the upcoming ESA mission Swarm can take advantage of our findings and provide all the auxiliary measurements needed for a proper recovery of the ambient magnetic field.
The aim of this thesis is to achieve a deep understanding of the working mechanism of polymer based solar cells and to improve the device performance. Two types of the polymer based solar cells are studied here: all-polymer solar cells comprising macromolecular donors and acceptors based on poly(p-phenylene vinylene) and hybrid cells comprising a PPV copolymer in combination with a novel small molecule electron acceptor. To understand the interplay between morphology and photovoltaic properties in all-polymer devices, I compared the photocurrent characteristics and excited state properties of bilayer and blend devices with different nano-morphology, which was fine tuned by using solvents with different boiling points. The main conclusion from these complementary measurements was that the performance-limiting step is the field-dependent generation of free charge carriers, while bimolecular recombination and charge extraction do not compromise device performance. These findings imply that the proper design of the donor-acceptor heterojunction is of major importance towards the goal of high photovoltaic efficiencies. Regarding polymer-small molecular hybrid solar cells I combined the hole-transporting polymer M3EH-PPV with a novel Vinazene-based electron acceptor. This molecule can be either deposited from solution or by thermal evaporation, allowing for a large variety of layer architectures to be realized. I then demonstrated that the layer architecture has a large influence on the photovoltaic properties. Solar cells with very high fill factors of up to 57 % and an open circuit voltage of 1V could be achieved by realizing a sharp and well-defined donor-acceptor heterojunction. In the past, fill factors exceeding 50 % have only been observed for polymers in combination with soluble fullerene-derivatives or nanocrystalline inorganic semiconductors as the electron-accepting component. The finding that proper processing of polymer-vinazene devices leads to similar high values is a major step towards the design of efficient polymer-based solar cells.
Synchronization is a fundamental phenomenon in nature. It can be considered as a general property of self-sustained oscillators to adjust their rhythm in the presence of an interaction.
In this work we investigate complex regimes of synchronization phenomena by means of theoretical analysis, numerical modeling, as well as practical analysis of experimental data.
As a subject of our investigation we consider chimera state, where due to spontaneous symmetry-breaking of an initially homogeneous oscillators lattice split the system into two parts with different dynamics. Chimera state as a new synchronization phenomenon was first found in non-locally coupled oscillators system, and has attracted a lot of attention in the last decade. However, the recent studies indicate that this state is also possible in globally coupled systems. In the first part of this work, we show under which conditions the chimera-like state appears in a system of globally coupled identical oscillators with intrinsic delayed feedback. The results of the research explain how initially monostable oscillators became effectivly bistable in the presence of the coupling and create a mean field that sustain the coexistence of synchronized and desynchronized states. Also we discuss other examples, where chimera-like state appears due to frequency dependence of the phase shift in the bistable system.
In the second part, we make further investigation of this topic by modeling influence of an external periodic force to an oscillator with intrinsic delayed feedback. We made stability analysis of the synchronized state and constructed Arnold tongues. The results explain formation of the chimera-like state and hysteric behavior of the synchronization area. Also, we consider two sets of parameters of the oscillator with symmetric and asymmetric Arnold tongues, that correspond to mono- and bi-stable regimes of the oscillator.
In the third part, we demonstrate the results of the work, which was done in collaboration with our colleagues from Psychology Department of University of Potsdam. The project aimed to study the effect of the cardiac rhythm on human perception of time using synchronization analysis. From our part, we made a statistical analysis of the data obtained from the conducted experiment on free time interval reproduction task. We examined how ones heartbeat influences the time perception and searched for possible phase synchronization between heartbeat cycles and time reproduction responses. The findings support the prediction that cardiac cycles can serve as input signals, and is used for reproduction of time intervals in the range of several seconds.
When azobenzene-modified photosensitive polymer films are irradiated with light interference patterns, topographic variations in the film develop that follow the electric field vector distribution resulting in the formation of surface relief grating (SRG). The exact correspondence of the electric field vector orientation in interference pattern in relation to the presence of local topographic minima or maxima of SRG is in general difficult to determine. In my thesis, we have established a systematic procedure to accomplish the correlation between different interference patterns and the topography of SRG. For this, we devise a new setup combining an atomic force microscope and a two-beam interferometer (IIAFM). With this set-up, it is possible to track the topography change in-situ, while at the same time changing polarization and phase of the impinging interference pattern. To validate our results, we have compared two photosensitive materials named in short as PAZO and trimer. This is the first time that an absolute correspondence between the local distribution of electric field vectors of interference pattern and the local topography of the relief grating could be established exhaustively. In addition, using our IIAFM we found that for a certain polarization combination of two orthogonally polarized interfering beams namely SP (↕, ↔) interference pattern, the topography forms SRG with only half the period of the interference patterns. Exploiting this phenomenon we are able to fabricate surface relief structures below diffraction limit with characteristic features measuring only 140 nm, by using far field optics with a wavelength of 491 nm. We have also probed for the stresses induced during the polymer mass transport by placing an ultra-thin gold film on top (5–30 nm). During irradiation, the metal film not only deforms along with the SRG formation, but ruptures in regular and complex manner. The morphology of the cracks differs strongly depending on the electric field distribution in the interference pattern even when the magnitude and the kinetic of the strain are kept constant. This implies a complex local distribution of the opto-mechanical stress along the topography grating. The neutron reflectivity measurements of the metal/polymer interface indicate the penetration of metal layer within the polymer resulting in the formation of bonding layer that confirms the transduction of light induced stresses in the polymer layer to a metal film.
The correlations between the chemical structures of the 2,5-diphenyl-1,3,4-oxadiazole compounds and their corresponding vapour deposited film structures on Si/SiO2 were systematically investigated with AFM, XSR and IR for the first time. The result shows that the film structure depends strongly on the substrate temperature (Ts). For the compounds with ether bridge group, the film periodicity depends linearly on the length of the aliphatic chain. The films based on those oxadiazols have ordered structure in the investigated substrate temperature region, while die amide bridged compounds form ordered film only at high Ts due to the formation of intermolecular H-bond. The tilt angle of most molecules is determined by the pi-pi complexes between the molecules. The intermolecular interaction between head groups leads to the structural transformation during the thermal treatment after deposition. All the ether bridged oxadiazoles form films with bilayer structure, while amide bridged oxadiazole form film bilayer structure only when the molecule has a head group.
The availability of large data sets has allowed researchers to uncover complex properties in complex systems, such as complex networks and human dynamics. A vast number of systems, from the Internet to the brain, power grids, ecosystems, can be represented as large complex networks. Dynamics on and of complex networks has attracted more and more researchers’ interest. In this thesis, first, I introduced a simple but effective dynamical optimization coupling scheme which can realize complete synchronization in networks with undelayed and delayed couplings and enhance the small-world and scale-free networks’ synchronizability. Second, I showed that the robustness of scale-free networks with community structure was enhanced due to the existence of communities in the networks and some of the response patterns were found to coincide with topological communities. My results provide insights into the relationship between network topology and the functional organization in complex networks from another viewpoint. Third, as an important kind of nodes of complex networks, human detailed correspondence dynamics was studied by both data and the model. A new and general type of human correspondence pattern was found and an interacting priority-queues model was introduced to explain it. The model can also embrace a range of realistic social interacting systems such as email and letter communication. My findings provide insight into various human activities both at the individual and network level. Fourth, I present clearly new evidence that human comment behavior in on-line social systems, a different type of interacting human dynamics, is non-Poissonian and a model based on the personal attraction was introduced to explain it. These results are helpful for discovering regular patterns of human behavior in on-line society and the evolution of the public opinion on the virtual as well as real society. Finally, there are conclusion and outlook of human dynamics and complex networks.
Perovskite solar cells have become one of the most studied systems in the quest for new, cheap and efficient solar cell materials. Within a decade device efficiencies have risen to >25% in single-junction and >29% in tandem devices on top of silicon. This rapid improvement was in many ways fortunate, as e. g. the energy levels of commonly used halide perovskites are compatible with already existing materials from other photovoltaic technologies such as dye-sensitized or organic solar cells. Despite this rapid success, fundamental working principles must be understood to allow concerted further improvements. This thesis focuses on a comprehensive understanding of recombination processes in functioning devices.
First the impact the energy level alignment between the perovskite and the electron transport layer based on fullerenes is investigated. This controversial topic is comprehensively addressed and recombination is mitigated through reducing the energy difference between the perovskite conduction band minimum and the LUMO of the fullerene. Additionally, an insulating blocking layer is introduced, which is even more effective in reducing this recombination, without compromising carrier collection and thus efficiency. With the rapid efficiency development (certified efficiencies have broken through the 20% ceiling) and thousands of researchers working on perovskite-based optoelectronic devices, reliable protocols on how to reach these efficiencies are lacking. Having established robust methods for >20% devices, while keeping track of possible pitfalls, a detailed description of the fabrication of perovskite solar cells at the highest efficiency level (>20%) is provided. The fabrication of low-temperature p-i-n structured devices is described, commenting on important factors such as practical experience, processing atmosphere & temperature, material purity and solution age. Analogous to reliable fabrication methods, a method to identify recombination losses is needed to further improve efficiencies. Thus, absolute photoluminescence is identified as a direct way to quantify the Quasi-Fermi level splitting of the perovskite absorber (1.21eV) and interfacial recombination losses the transport layers impose, reducing the latter to ~1.1eV. Implementing very thin interlayers at both the p- and n-interface (PFN-P2 and LiF, respectively), these losses are suppressed, enabling a VOC of up to 1.17eV. Optimizing the device dimensions and the bandgap, 20% devices with 1cm2 active area are demonstrated. Another important consideration is the solar cells’ stability if subjected to field-relevant stressors during operation. In particular these are heat, light, bias or a combination thereof. Perovskite layers – especially those incorporating organic cations – have been shown to degrade if subjected to these stressors. Keeping in mind that several interlayers have been successfully used to mitigate recombination losses, a family of perfluorinated self-assembled monolayers (X-PFCn, where X denotes I/Br and n = 7-12) are introduced as interlayers at the n-interface. Indeed, they reduce interfacial recombination losses enabling device efficiencies up to 21.3%. Even more importantly they improve the stability of the devices. The solar cells with IPFC10 are stable over 3000h stored in the ambient and withstand a harsh 250h of MPP at 85◦C without appreciable efficiency losses. To advance further and improve device efficiencies, a sound understanding of the photophysics of a device is imperative. Many experimental observations in recent years have however drawn an inconclusive picture, often suffering from technical of physical impediments, disguising e. g. capacitive discharge as recombination dynamics. To circumvent these obstacles, fully operational, highly efficient perovskites solar cells are investigated by a combination of multiple optical and optoelectronic probes, allowing to draw a conclusive picture of the recombination dynamics in operation. Supported by drift-diffusion simulations, the device recombination dynamics can be fully described by a combination of first-, second- and third-order recombination and JV curves as well as luminescence efficiencies over multiple illumination intensities are well described within the model. On this basis steady state carrier densities, effective recombination constants, densities-of-states and effective masses are calculated, putting the devices at the brink of the radiative regime. Moreover, a comprehensive review of recombination in state-of-the-art devices is given, highlighting the importance of interfaces in nonradiative recombination. Different strategies to assess these are discussed, before emphasizing successful strategies to reduce interfacial recombination and pointing towards the necessary steps to further improve device efficiency and stability. Overall, the main findings represent an advancement in understanding loss mechanisms in highly efficient solar cells. Different reliable optoelectronic techniques are used and interfacial losses are found to be of grave importance for both efficiency and stability. Addressing the interfaces, several interlayers are introduced, which mitigate recombination losses and degradation.
Climate change affects societies across the globe in various ways. In addition to gradual changes in temperature and other climatic variables, global warming is likely to increase intensity and frequency of extreme weather events.
Beyond biophysical impacts, these also directly affect societal and economic activity. Additionally, indirect effects can occur; spatially, economic losses can spread along global supply-chains; temporally, climate impacts can change the economic development trajectory of countries.
This thesis first examines how climate change alters river flood risk and its local socio-economic implications. Then, it studies the global economic response to river floods in particular, and to climate change in general.
Changes in high-end river flood risk are calculated for the next three decades on a global scale with high spatial resolution. In order to account for uncertainties, this assessment makes use of an ensemble of climate and hydrological models as well as a river routing model, that is found to perform well regarding peak river discharge. The results show an increase in high-end flood risk in many parts of the world, which require profound adaptation efforts. This pressure to adapt is measured as the enhancement in protection level necessary to stay at historical high-end risk. In developing countries as well as in industrialized regions, a high pressure to adapt is observed - the former to increase low protection levels, the latter to maintain the low risk levels perceived in the past.
Further in this thesis, the global agent-based dynamic supply-chain model acclimate is developed. It models the cascading of indirect losses in the global supply network. As an anomaly model its agents - firms and consumers - maximize their profit locally to respond optimally to local perturbations. Incorporating quantities as well as prices on a daily basis, it is suitable to dynamically resolve the impacts of unanticipated climate extremes.
The model is further complemented by a static measure, which captures the inter-dependencies between sectors across regions that are only connected indirectly. These higher-order dependencies are shown to be important for a comprehensive assessment of loss-propagation and overall costs of local disasters.
In order to study the economic response to river floods, the acclimate model is driven by flood simulations. Within the next two decades, the increase in direct losses can only partially be compensated by market adjustments, and total losses are projected to increase by 17% without further adaptation efforts. The US and the EU are both shown to receive indirect losses from China, which is strongly affected directly. However, recent trends in the trade relations leave the EU in a better position to compensate for these losses.
Finally, this thesis takes a broader perspective when determining the investment response to the climate change damages employing the integrated assessment model DICE. On an optimal economic development path, the increase in damages is anticipated as emissions and consequently temperatures increase. This leads to a significant devaluation of investment returns and the income losses from climate damages almost double.
Overall, the results highlight the need to adapt to extreme weather events - local physical adaptation measures have to be combined with regional and global policy measures to prepare the global supply-chain network to climate change.