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Functional structures as well as materials provided by nature have always been a great source of inspiration for new technologies. Adapting and improving the discovered concepts, however, demands a detailed understanding of their working principles, while employing natural materials for fabrication tasks requires suitable functionalization and modification.
In this thesis, the white scales of the beetle Cyphochilus are examined in order to reveal unknown aspects of their light transport properties. In addition, the monomer of the material they are made of is utilized for 3D microfabrication.
White beetle scales have been fascinating scientists for more than a decade because they display brilliant whiteness despite their small thickness and the low refractive index contrast. Their optical properties arise from highly efficient light scattering within the disordered intra-scale network structure.
To gain a better understanding of the scattering properties, several previous studies have investigated the light transport and its connection to the structural anisotropy with the aid of diffusion theory. While this framework allows to relate the light scattering to macroscopic transport properties, an accurate determination of the effective refractive index of the structure is required. Due to its simplicity, the Maxwell-Garnett mixing rule is frequently used for this task, although its constraint to particle and feature sizes much smaller than the wavelength is clearly violated for the scales.
To provide a correct calculation of the effective refractive index, here, finite-difference time-domain simulations are used to systematically examine the impact of size effects on the effective refractive index. Deploying this simulation approach, the Maxwell-Garnett mixing rule is shown to break down for large particles. In contrast, it is found that a quadratic polynomial function describes the effective refractive index in close approximation, while its coefficients can be obtained from an empirical linear function. As a result, a simple mixing rule is reported that unambiguously surpasses classical mixing rules when composite media containing large feature sizes are considered. This is important not only for the accurate description of white beetle scales, but also for other turbid media, such as biological tissues in opto-biomedical diagnostics.
Describing light transport by means of diffusion theory moreover neglects any coherent effects, such as interference. Hence, their impact on the generation of brilliant whiteness is currently unknown. To shed a light on their role, spatial- and time-resolved light scattering spectromicroscopy is applied to investigate the scales and a model structure of them based on disordered Bragg stacks. For both structures the occurrence of weakly localized photonic modes, i.e., closed scattering loops, is observed, which is further verified in accompanying simulations. As shown in this thesis, leakage from these random photonic modes contributes at least 20% to the overall reflected light. This reveals the importance of coherent effects for a complete description of the underlying light transport properties; an aspect that is entirely missing in the purely diffusive transport presumed so far. Identifying the importance of weak localization for the generation of brilliant whiteness paves the way to further enhance the design of efficient optical scattering media, an issue that recently drawn great attention.
Unlike their plant-based counterparts, rigid carbohydrates, such as chitin, are currently unavailable for 3D microfabrication via direct laser writing, despite their great significance in the animal kingdom for the construction of functional microstructures. To overcome this gap, the monomeric unit of chitin, N-acetyl-D-glucosamine, is here functionalized to serve as a photo-crosslinkable monomer in a non-hydrogel photoresist. Since all previous photoresists based on animal carbohydrates are in the form of hydrogel formulations, a new group of photoresists is established for direct laser writing.
Moreover, it is exhibited that the sensitization effect, previously used only in the context of UV curing, can be successfully transferred to direct laser writing to increase the maximum writing speed. This effect is based on the beneficial combination of two photoinitiators.
In this, one photoinitiator is an efficient crosslinking agent for the monomer used, but a rather poor two-photon absorber. The other photoinitiator (called sensitizer) possesses, conversely, a much higher two-photon absorption coefficient at the applied wavelength but is not well suited as a crosslinking agent. In combination, the energy absorbed by the sensitizer is passed to the photoinitiator, resulting in the formation of radicals needed to start the polymerization. As this greatly increases the rate at which the photoinitiator is radicalized, resists containing a photoinitiator and a sensitizer are shown to outperform resists containing only one of the components. Deploying the sensitization effect in direct laser writing therefore offers a simple way to individually tune the crosslinking ability and the two-photon absorption properties by combining existing compounds, compared to the costly chemical synthesis of novel, customized photoinitiators.
Lubricated tribological contact processes are important in both nature and in many technical applications. Fluid lubricants play an important role in contact processes, e.g. they reduce friction and cool the contact zone. The fundamentals of lubricated contact processes on the atomistic scale are, however, today not fully understood. A lubricated contact process is defined here as a process, where two solid bodies that are in close proximity and eventually in parts in direct contact, carry out a relative motion, whereat the remaining volume is submersed by a fluid lubricant. Such lubricated contact processes are difficult to examine experimentally. Atomistic simulations are an attractive alternative for investigating the fundamentals of such processes. In this work, molecular dynamics simulations were used for studying different elementary processes of lubricated tribological contacts. A simplified, yet realistic simulation setup was developed in this work for that purpose using classical force fields. In particular, the two solid bodies were fully submersed in the fluid lubricant such that the squeeze-out was realistically modeled. The velocity of the relative motion of the two solid bodies was imposed as a boundary condition. Two types of cases were considered in this work: i) a model system based on synthetic model substances, which enables a direct, but generic, investigation of molecular interaction features on the contact process; and ii) real substance systems, where the force fields describe specific real substances. Using the model system i), also the reproducibility of the findings obtained from the computer experiments was critically assessed. In most cases, also the dry reference case was studied. Both mechanical and thermodynamic properties were studied -- focusing on the influence of lubrication. The following properties were studied: The contact forces, the coefficient of friction, the dislocation behavior in the solid, the chip formation and the formation of the groove, the squeeze-out behavior of the fluid in the contact zone, the local temperature and the energy balance of the system, the adsorption of fluid particles on the solid surfaces, as well as the formation of a tribofilm. Systematic studies were carried out for elucidating the influence of the wetting behavior, the influence of the molecular architecture of the lubricant, and the influence of the lubrication gap height on the contact process. As expected, the presence of a fluid lubricant reduces the temperature in the vicinity of the contact zone. The presence of the lubricant is, moreover, found to have a significant influence on the friction and on the energy balance of the process. The presence of a lubricant reduces the coefficient of friction compared to a dry case in the starting phase of a contact process, while lubricant molecules remain in the contact zone between the two solid bodies. This is a result of an increased normal and slightly decreased tangential force in the starting phase. When the fluid molecules are squeezed out with ongoing contact time and the contact zone is essentially dry, the coefficient of friction is increased by the presence of a fluid compared to a dry case. This is attributed to an imprinting of individual fluid particles into the solid surface, which is energetically unfavorable. By studying the contact process in a wide range of gap height, the entire range of the Stribeck curve is obtained from the molecular simulations. Thereby, the three main lubrication regimes of the Stribeck curve and their transition regions are covered, namely boundary lubrication (significant elastic and plastic deformation of the substrate), mixed lubrication (adsorbed fluid layers dominate the process), and hydrodynamic lubrication (shear flow is set up between the surface and the asperity). The atomistic effects in the different lubrication regimes are elucidated. Notably, the formation of a tribofilm is observed, in which lubricant molecules are immersed into the metal surface. The formation of a tribofilm is found to have important consequences for the contact process. The work done by the relative motion is found to mainly dissipate and thereby heat up the system. Only a minor part of the work causes plastic deformation. Finally, the assumptions, simplifications, and approximations applied in the simulations are critically discussed, which highlights possible future work.
With the transition of fluid-capillary-based “Lab on a chip 1.0″ concepts in analytical chemistry to “Lab on a chip
2.0″ approaches relying on distinct fluid droplets (“digital microfluidics”, DMF), the need for reliable methods for
droplet actuation has increasingly come into focus. One possible approach is based on “electrowetting on
dielectric” (EWOD). This technique has the disadvantage that any possible desired later positions of the droplets
on the chip have to be defined prior to chip realization because one of the EWOD electrode layers has to be
structured accordingly. “Optoelectrowetting” (OEW) goes a step further in the sense that the later droplet positions
do not have to be known before, and none of the electrode layers has to be structured. Instead, the
electrical parameters of the layer sequence can be altered locally by an impinging (and movable) light spot.
Although some research groups have succeeded in demonstrating OEW actuation of droplets, the optimization of
the relevant parameters of the layer sequence and the droplet – at least half a dozen parameters altogether – is
tedious and not straight-forward. In this contribution, for optimization purposes, the equations governing OEW
are revisited and altered again, e.g., by numerical implementation of the experimentally well-known saturation
of the contact angle change. Additionally, a Nelder-Mead algorithm is applied to find the parameters, on which
the optimization has to focus to maximize contact angle changes and, thus, mechanical forces on the droplets.
The numerical investigation yields diverse results, e.g., the finding that the droplet’s contact area on the
dielectric layer has a strong influence on the contact angle change and the question whether the droplet is pulled
or pushed. Moreover, the interplay between frequency and amplitude of the applied rectangular alternate voltage
is important for optimization.
In this work, we investigate and compare the condensation behavior of hydrophilic, hydrophobic, and biphilic microgrooved silicon samples etched by reactive ion etching. The microgrooves were 25 mm long and 17−19 μm deep with different
topologies depending on the etching process. Anisotropically etched samples had 30 μm wide rectangular microgrooves and silicon ridges between them. They were either left hydrophilic or covered with a hydrophobic fluorocarbon or photoresist layer.
Anisotropically etched samples consisted of 48 μm wide semicircular shaped microgrooves, 12 μm wide silicon ridges between them, and a 30 μm wide photoresist stripe centered on the ridges. The lateral dimensions were chosen to be much smaller than the capillary length of water to support drainage of droplets by coalescence rather than droplet sliding. Furthermore, to achieve a low thermal resistance of the periodic surface structure consisting of water-filled grooves and silicon ridges, the trench depth was also kept small. The dripped-off total amount of condensate (AoC) was measured for each sample for 12 h under the same boundary
conditions (chamber temperature 30 °C, cooling temperature 6 °C, and relative humidity 60%). The maximum increase in AoC of 15.9% (9.6%) against the hydrophilic (hydrophobic) reference sample was obtained for the biphilic samples. In order to elucidate their unique condensation behavior, in situ optical imaging was performed at normal incidence. It shows that the drainage of droplets from the stripe’s surface into the microgrooves as well as occasional droplet sliding events are the dominant processes to clear the surface. To rationalize this behavior, the Hough Circle Transform algorithm was implemented for image processing to receive
additional information about the transient droplet size and number distribution. Postprocessing of these data allows calculation
The great flexibility of direct laser writing (DLW) arises from the possibility to fabricate precise three-dimensional structures on very small scales as well as the broad range of applicable materials. However, there is still a vast number of promising materials, which are currently inaccessible requiring the continuous development of novel photoresists. Herein, a new bio-sourced resist is reported that uses the monomeric unit of chitin, N-acetyl-D-glucosamine, paving the way from existing hydrogel resists based on animal carbohydrates to a new class of non-hydrogel ones. In addition, it is shown that the combined use of two photoinitiators is advantageous over the use of a single one. In this approach, the first photoinitiator is a good two-photon absorber at the applied wavelength, while the second photoinitiator exhibits poor two-photon absorbtion abilities, but is better suited for cross-linking of the monomer. The first photoinitiator absorbs the light acting as a sensitizer and transfers the energy to the second initiator, which subsequently forms a radical and initializes the polymerization. This sensitization effect enables a new route to utilize reactive photointiators with a small two-photon absorption cross section for DLW without changing their chemical structure.
This paper is concerned with a theoretical analysis of the behavior of optically excited spin currents in bilayer and multilayer systems of ferromagnetic and normal metals. As the propagation, control, and manipulation of the spin currents created in ferromagnets by femtosecond optical pulses is of particular interest, we examine the influence of different thicknesses of the constituent layers for the case of electrons excited several electronvolts above the Fermi level. Using a Monte-Carlo simulation framework for such highly excited electrons, we first examine the spatiotemporal characteristics of the spin current density driven in a Fe layer, where the absorption profile of the light pulse plays an important role. Further, we examine how the combination of light absorption profile, spin-dependent transmission probabilities, and iron layer thickness affects spin current density in a Fe/Au bilayer system. For high-energy electrons studied here, the interface and secondary electron generation have a small influence on spin transport in the bilayer system. However, we find that spin injection from one layer to another is most effective within a certain range of iron layer thicknesses.
The concept of building logically functional networks employing spintronics or magnetic heterostructures is becoming more and more popular today. Incorporating logical segments into a circuit needs physical bonds between the magnetic molecules or clusters involved. In this framework, we systematically study ultrafast laser-induced spin-manipulation scenarios on a closed system of three carbon chains to which three Ni atoms are attached. After the inclusion of spin–orbit coupling and an external magnetic field, different ultrafast spin dynamics scenarios involving spin-flip and long-distance spin-transfer processes are achieved by various appropriately well-tailored time-resolved laser pulses within subpicosecond timescales. We additionally study the various effects of an external magnetic field on spin-flip and spin-transfer processes. Moreover, we obtain spin-dynamics processes induced by a double laser pulse, rather than a single one. We suggest enhancing the spatial addressability of spin-flip and spin-transfer processes. The findings presented in this article will improve our knowledge of the magnetic properties of carbon-based magnetic molecular structures. They also support the relevant experimental realization of spin dynamics and their potential applications in future molecular spintronics devices.
Rapid-prototyping of microscopic thermal landscapes in Brillouin light scattering spectroscopy
(2023)
Since temperature and its spatial, and temporal variations affect a wide range of physical properties of material systems, they can be used to create reconfigurable spatial structures of various types in physical and biological objects. This paper presents an experimental optical setup for creating tunable two-dimensional temperature patterns on a micrometer scale. As an example of its practical application, we have produced temperature-induced magnetization landscapes in ferrimagnetic yttrium iron garnet films and investigated them using micro-focused Brillouin light scattering spectroscopy. It is shown that, due to the temperature dependence of the magnon spectrum, spatial temperature distributions can be visualized even for microscale thermal patterns.
Finding new energy-efficient methods for exciting magnetization dynamics is one of the key challenges in magnonics. In this work, we present an approach to excite the gyrotropic dynamics of magnetic vortices through the phenomenon of inverse magnetostriction, also known as the Villari effect. We develop an analytical model based on the Thiele formalism that describes the gyrotropic motion of the vortex core including the energy contributions due to inverse magnetostriction. Based on this model, we predict excitations of the vortex core resonances by surface acoustic waves whose frequency is resonant with the frequency of the vortex core. We verify the model's prediction using micromagnetic simulations and show the dependence of the vortex core's oscillation radius on the surface acoustic wave amplitude and the static bias field. Our study contributes to the advancement of energy-efficient magnetic excitations by relying on voltage-induced driven dynamics, which is an alternative to conventional current-induced excitations.
The Born–Fock theorem is one of the most fundamental theorems of quantum mechanics and forms the basis for reliable and efficient navigation in the Hilbert space of a quantum system with a time-dependent Hamiltonian by adiabatic evolution. In the absence of level crossings, i.e. without degeneracies, and under adiabatic time evolution all eigenstates of the Hamiltonian keep their energetic order, labeled by a conserved integer quantum number. Thus, controlling the eigenstates of the Hamiltonian and their energetic order in asymptotic limits allows one to engineer a perfect adiabatic transfer between a large number of initial and target states. The fidelity of the state transfer is only limited by adiabaticity and the selection of target states is controlled by the integer invariant labeling the order of eigenstates. We show here, for the example of a finite superlattice Wannier-Stark ladder, i.e. a one-dimensional lattice with alternating hopping amplitudes and constant potential gradient, that such an adiabatic control of eigenstates can be used to induce perfectly quantized single-particle transport across a pre-determined number of lattice sites. We dedicate this paper to the memory of our late friend and colleague Bruce Shore, who was an expert in adiabatic processes and taught us much about this field.