74-05 Experimental work
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Institute
In the present thesis I investigate the lattice dynamics of thin film hetero structures of magnetically ordered materials upon femtosecond laser excitation as a probing and manipulation scheme for the spin system. The quantitative assessment of laser induced thermal dynamics as well as generated picosecond acoustic pulses and their respective impact on the magnetization dynamics of thin films is a challenging endeavor. All the more, the development and implementation of effective experimental tools and comprehensive models are paramount to propel future academic and technological progress.
In all experiments in the scope of this cumulative dissertation, I examine the crystal lattice of nanoscale thin films upon the excitation with femtosecond laser pulses. The relative change of the lattice constant due to thermal expansion or picosecond strain pulses is directly monitored by an ultrafast X-ray diffraction (UXRD) setup with a femtosecond laser-driven plasma X-ray source (PXS). Phonons and spins alike exert stress on the lattice, which responds according to the elastic properties of the material, rendering the lattice a versatile sensor for all sorts of ultrafast interactions. On the one hand, I investigate materials with strong magneto-elastic properties; The highly magnetostrictive rare-earth compound TbFe2, elemental Dysprosium or the technological relevant Invar material FePt. On the other hand I conduct a comprehensive study on the lattice dynamics of Bi1Y2Fe5O12 (Bi:YIG), which exhibits high-frequency coherent spin dynamics upon femtosecond laser excitation according to the literature. Higher order standing spinwaves (SSWs) are triggered by coherent and incoherent motion of atoms, in other words phonons, which I quantified with UXRD. We are able to unite the experimental observations of the lattice and magnetization dynamics qualitatively and quantitatively. This is done with a combination of multi-temperature, elastic, magneto-elastic, anisotropy and micro-magnetic modeling.
The collective data from UXRD, to probe the lattice, and time-resolved magneto-optical Kerr effect (tr-MOKE) measurements, to monitor the magnetization, were previously collected at different experimental setups. To improve the precision of the quantitative assessment of lattice and magnetization dynamics alike, our group implemented a combination of UXRD and tr-MOKE in a singular experimental setup, which is to my knowledge, the first of its kind. I helped with the conception and commissioning of this novel experimental station, which allows the simultaneous observation of lattice and magnetization dynamics on an ultrafast timescale under identical excitation conditions. Furthermore, I developed a new X-ray diffraction measurement routine which significantly reduces the measurement time of UXRD experiments by up to an order of magnitude. It is called reciprocal space slicing (RSS) and utilizes an area detector to monitor the angular motion of X-ray diffraction peaks, which is associated with lattice constant changes, without a time-consuming scan of the diffraction angles with the goniometer. RSS is particularly useful for ultrafast diffraction experiments, since measurement time at large scale facilities like synchrotrons and free electron lasers is a scarce and expensive resource. However, RSS is not limited to ultrafast experiments and can even be extended to other diffraction techniques with neutrons or electrons.
Transient permeability in porous and fractured sandstones mediated by fluid-rock interactions
(2021)
Understanding the fluid transport properties of subsurface rocks is essential for a large number of geotechnical applications, such as hydrocarbon (oil/gas) exploitation, geological storage (CO2/fluids), and geothermal reservoir utilization. To date, the hydromechanically-dependent fluid flow patterns in porous media and single macroscopic rock fractures have received numerous investigations and are relatively well understood. In contrast, fluid-rock interactions, which may permanently affect rock permeability by reshaping the structure and changing connectivity of pore throats or fracture apertures, need to be further elaborated. This is of significant importance for improving the knowledge of the long-term evolution of rock transport properties and evaluating a reservoir’ sustainability. The thesis focuses on geothermal energy utilization, e.g., seasonal heat storage in aquifers and enhanced geothermal systems, where single fluid flow in porous rocks and rock fracture networks under various pressure and temperature conditions dominates.
In this experimental study, outcrop samples (i.e., Flechtinger sandstone, an illite-bearing Lower Permian rock, and Fontainebleau sandstone, consisting of pure quartz) were used for flow-through experiments under simulated hydrothermal conditions. The themes of the thesis are (1) the investigation of clay particle migration in intact Flechtinger sandstone and the coincident permeability damage upon cyclic temperature and fluid salinity variations; (2) the determination of hydro-mechanical properties of self-propping fractures in Flechtinger and Fontainebleau sandstones with different fracture features and contrasting mechanical properties; and (3) the investigation of the time-dependent fracture aperture evolution of Fontainebleau sandstone induced by fluid-rock interactions (i.e., predominantly pressure solution). Overall, the thesis aims to unravel the mechanisms of the instantaneous reduction (i.e., direct responses to thermo-hydro-mechanical-chemical (THMC) conditions) and progressively-cumulative changes (i.e., time-dependence) of rock transport properties.
Permeability of intact Flechtinger sandstone samples was measured under each constant condition, where temperature (room temperature up to 145 °C) and fluid salinity (NaCl: 0 ~ 2 mol/l) were stepwise changed. Mercury intrusion porosimetry (MIP), electron microprobe analysis (EMPA), and scanning electron microscopy (SEM) were performed to investigate the changes of local porosity, microstructures, and clay element contents before and after the experiments. The results indicate that the permeability of illite-bearing Flechtinger sandstones will be impaired by heating and exposure to low salinity pore fluids. The chemically induced permeability variations prove to be path-dependent concerning the applied succession of fluid salinity changes. The permeability decay induced by a temperature increase and a fluid salinity reduction operates by relatively independent mechanisms, i.e., thermo-mechanical and thermo-chemical effects.
Further, the hydro-mechanical investigations of single macroscopic fractures (aligned, mismatched tensile fractures, and smooth saw-cut fractures) illustrate that a relative fracture wall offset could significantly increase fracture aperture and permeability, but the degree of increase depends on fracture surface roughness. X-ray computed tomography (CT) demonstrates that the contact area ratio after the pressure cycles is inversely correlated to the fracture offset. Moreover, rock mechanical properties, determining the strength of contact asperities, are crucial so that relatively harder rock (i.e., Fontainebleau sandstone) would have a higher self-propping potential for sustainable permeability during pressurization. This implies that self-propping rough fractures with a sufficient displacement are efficient pathways for fluid flow if the rock matrix is mechanically strong.
Finally, two long-term flow-through experiments with Fontainebleau sandstone samples containing single fractures were conducted with an intermittent flow (~140 days) and continuous flow (~120 days), respectively. Permeability and fluid element concentrations were measured throughout the experiments. Permeability reduction occurred at the beginning stage when the stress was applied, while it converged at later stages, even under stressed conditions. Fluid chemistry and microstructure observations demonstrate that pressure solution governs the long-term fracture aperture deformation, with remarkable effects of the pore fluid (Si) concentration and the structure of contact grain boundaries. The retardation and the cessation of rock fracture deformation are mainly induced by the contact stress decrease due to contact area enlargement and a dissolved mass accumulation within the contact boundaries. This work implies that fracture closure under constant (pressure/stress and temperature) conditions is likely a spontaneous process, especially at the beginning stage after pressurization when the contact area is relatively small. In contrast, a contact area growth yields changes of fracture closure behavior due to the evolution of contact boundaries and concurrent changes in their diffusive properties. Fracture aperture and thus permeability will likely be sustainable in the long term if no other processes (e.g., mineral precipitations in the open void space) occur.