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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.
Lattice dynamics
(2020)
In this thesis I summarize my contribution to the research field of ultrafast structural dynamics in condensend matter. It consists of 17 publications that cover the complex interplay between electron, magnon, and phonon subsystems in solid materials and the resulting lattice dynamics after ultrafast photoexcitation. The investigation of such dynamics is necessary for the physical understanding of the processes in materials that might become important in the future as functional materials for technological applications, for example in data storage applications, information processing, sensors, or energy harvesting.
In this work I present ultrafast x-ray diffraction (UXRD) experiments based on the optical pump – x-ray probe technique revealing the time-resolved lattice strain. To study these dynamics the samples (mainly thin film heterostructures) are excited by femtosecond near-infrared or visible light pulses. The induced strain dynamics caused by stresses of the excited subsystems are measured in a pump-probe scheme with x-ray diffraction (XRD) as a probe. The UXRD setups used during my thesis are a laser-driven table-top x-ray source and large-scale synchrotron facilities with dedicated time-resolved diffraction setups. The UXRD experiments provide quantitative access to heat reservoirs in nanometric layers and monitor the transient responses of these layers with coupled electron, magnon, and phonon subsystems. In contrast to optical probes, UXRD allows accessing the material-specific information, which is unavailable for optical light due to the detection of multiple indistinguishable layers in the range of the penetration depth.
In addition, UXRD facilitates a layer-specific probe for layers buried opaque heterostructures to study the energy flow. I extended this UXRD technique to obtain the driving stress profile by measuring the strain dynamics in the unexcited buried layer after excitation of the adjacent absorbing layers with femtosecond laser pulses. This enables the study of negative thermal expansion (NTE) in magnetic materials, which occurs due to the loss of the magnetic order. Part of this work is the investigation of stress profiles which are the source of coherent acoustic phonon wave packets (hypersound waves). The spatiotemporal shape of these stress profiles depends on the energy distribution profile and the ability of the involved subsystems to produce stress. The evaluation of the UXRD data of rare-earth metals yields a stress profile that closely matches the optical penetration profile: In the paramagnetic (PM) phase the photoexcitation results in a quasi-instantaneous expansive stress of the metallic layer whereas in the antiferromagnetic (AFM) phase a quasi-instantaneous contractive stress and a second contractive stress contribution rising on a 10 ps time scale adds to the PM contribution. These two time scales are characteristic for the magnetic contribution and are in agreement with related studies of the magnetization dynamics of rare-earth materials.
Several publications in this thesis demonstrate the scientific progress in the field of active strain control to drive a second excitation or engineer an ultrafast switch. These applications of ultrafast dynamics are necessary to enable control of functional material properties via strain on ultrafast time scales.
For this thesis I implemented upgrades of the existing laser-driven table-top UXRD setup in order to achieve an enhancement of x-ray flux to resolve single digit nanometer thick layers. Furthermore, I developed and built a new in-situ time-resolved magneto-optic Kerr effect (MOKE) and optical reflectivity setup at the laser-driven table-top UXRD setup to measure the dynamics of lattice, electrons and magnons under the same excitation conditions.