Picosecond strain dynamics in Ge2_{2}Sb2_{2}Te5_{5} monitored by time-resolved x-ray diffraction

Coherent phonons (CP) generated by laser pulses on the femtosecond scale have been proposed as a means to achieve ultrafast, non-thermal switching in phase-change materials such as Ge$_{2}$Sb$_{2}$Te$_{5}$(GST). Here we use ultrafast optical pump pulses to induce coherent acoustic phonons and stroboscopically measure the corresponding lattice distortions in GST using 100 ps x-ray pulses from the ESRF storage ring. A linear-chain model provides a good description of the observed changes in the diffraction signal, however, the magnitudes of the measured shifts are too large to be explained by thermal effects alone implying the presence of transient non-equilibrium electron heating in addition to temperature driven expansion. The information on the movement of atoms during the excitation process can lead to greater insight into the possibilities of using CP-induced phase-transitions in GST.Comment: 7 pages, 4 figures, Phys. Rev. B, in pres

Molecular beam epitaxy of GeTe-Sb2Te3 phase change materials studied by X-ray diffraction

Die monolithische Integration von Phasenwechselmaterialien mit Halbleiter-Hetero\-strukturen er\"offnet neue Perspektiven f\"ur zuk\"unftige Generationen von nichtfl\"uchtigen Speicherbauelementen. %Epitaktische Phasenwechselmaterialien erm�glichen detaillierte %Studien der strukturellen �nderungen w�hrend des Phasen�bergangs und %erlauben eine Bestimmung der Skalierungslimits zuk�nftiger %Datenspeicher. Diese Arbeit befasst sich mit dem epitaktischen Wachstum von Ge-Sb-Te Phasenwechselmaterialien. Dazu wurden Ge-Sb-Te(GST) Schichten mittels Molekularstrahlepitaxie (MBE) auf GaSb(001)-Substraten abgeschieden. Die kristallografische Orientierung und die Ver\"anderungen der Gitterkonstante w\"ahrend des Wachstums wurden mittels R\"ontgenbeugung unter streifendem Einfall (GIXRD) bestimmt. Das Nukleationsverhalten zu Beginn des Wachstums wurde mittels Hochenergie-Elektronenbeugung unter streifendem Einfall (RHEED) untersucht.The integration of phase change materials into semiconductor heterostructures may lead to the development of a new generation of high density non-volatile phase change memories. Epitaxial phase change materials allow to study the detailed structural changes during the phase transition and to determine the scaling limits of the memory. This work is dedicated to the epitaxial growth of Ge-Sb-Te phase change alloys on GaSb(001). We deposit Ge-Sb-Te (GST) films on GaSb(001) substrates by means of molecular beam epitaxy (MBE). The film orientation and lattice constant evolution is determined in real time during growth using grazing incidence X-ray diffraction (GID). The nucleation stage of the growth is studied \emph{in situ} using reflection high energy electron diffraction (RHEED)

Hydrogen Solubility and Atomic Structure of Graphene Supported Pd Nanoclusters

We investigated the atomic structure of graphene supported Pd nanoclusters and their interaction with hydrogen up to atmospheric pressures at room temperature by surface X-ray diffraction and scanning tunneling microscopy. We find that Ir seeded Pd nanocluster superlattices with 1.2 nm cluster diameters can be grown on the graphene/Ir(111) moire ' template with high structural perfection. The superlattice clusters are anchored through the rehybridized graphene to the Ir support, which superimposes a 2.0% inplane compression onto the clusters. During hydrogen exposure at 10 mbar pressure and room temperature, a significant part of the clusters gets unpinned from the superlattice. The clusters in registry undergo an out-of-plane expansion only, whereas the detached clusters expand in in- and out-of-plane directions. The formation of a hydrogen rich PdHx alpha' phase was not observed. After exposure to 1 bar, the majority of the clusters are unpinned from superlattice sites, due to their surface interaction with hydrogen and possible spill over to the graphene support. Only minor sintering was observed, which is more pronounced for the unpinned clusters. The results give evidence that ultrasmall Pd clusters on graphene are a stable hydrogen storage system with reduced hydrogen storage hysteresis and maintain a large surface area for hydrogen chemisorption

Preparing for High-Repetition Rate Hard X-Ray Self-Seeding at the European X-Ray Free Electron Laser: Challenges and opportunities

A hard x-ray self-seeding (HXRSS) setup will soon be available at the European X-ray Free Electron Laser (XFEL). The availability of high repetition rate x-ray pulses poses novel challenges in the setup development, compared to the choices made at other facilities, mainly crystal heat-load and radiation-damage issues. However, high-repetition rate is expected to allow for unprecedented output characteristics. A two-chicane HXRSS setup is found to be optimal for the European XFEL. In this paper we discuss the physical choices peculiar to that facility and simulations done, which allow us to fix the parameter for the setup design

Nanosecond laser pulse heating of a platinum surface studied by pump-probe X-ray diffraction

We report on the quantitative determination of the transient surface temperature of Pt(110) upon nanosecond laser pulse heating. We find excellent agreement between heat transport theory and the experimentally determined transient surface temperature as obtained from time-resolved X-ray diffraction on timescales from hundred nanoseconds to milliseconds. Exact knowledge of the surface temperature's temporal evolution after laser excitation is crucial for future pump-probe experiments at synchrotron storage rings and X-ray free electron lasers

Dehydrogenation of Liquid Organic Hydrogen Carriers on Supported Pd Model Catalysts: Carbon Incorporation Under Operation Conditions

Liquid organic hydrogen carriers (LOHCs) have great potential as a hydrogen storage medium needed for a future sustainable energy system. Dehydrogenation of LOHCs requires a catalyst, such as supported Pd nanoparticles. Under reaction conditions, hydrogen and carbon may diffuse into the bulk of supported Pd catalyst particles and affect their activity and selectivity. The detailed understanding of this process is critical for the use of LOHCs in future hydrogen storage technologies. In this work, we studied these processes in-situ on a Pd model catalyst using high-energy grazing incidence X-ray diffraction. Pd nanoparticles were evaporated in ultra-high vacuum on a polished $α$-Al$_2$O$_3$(0001) substrate. The particles, with an initial average size of ~ 3.4 nm, were investigated at elevated temperature during their interaction with H$_2$ and methylcyclohexane (MCH) representing a model LOHC. The interaction with H$_2$ was studied in-situ at partial pressures up to 1 bar and temperatures between 300 and 500 K. At 300 K, the Pd nanoparticles (NPs) show a transition from $α$-PdH to $β$-PdH as a function of the H$_2$ pressure. The transition occurs gradually, which is attributed to the heterogeneity of the NP system. The hydrogen uptake in $β$-PdH$_x$ at 300 K and 1 bar is estimated to be XH ~ 0.37 ± 0.03 indicating that the miscibility gap is narrowed for the nanoparticular system. With increasing temperature, X$_H$ decreases until no $β$-PdH phase is formed anymore at 500 K. At the same temperature, we studied the interaction of the Pd/sapphire model catalyst with MCH, both in the presence and in the absence of H$_2$. In the absence of H$_2$, carbon is formed and diffuses into the bulk yielding PdC$_x$ with a C concentration of around x ~ 0.05 ± 0.01. In the presence of H$_2$ in the gas phase, bulk carbon formation in the Pd/sapphire model catalyst is completely suppressed. These results show that Pd nanoparticles act as an adequate catalyst for the dehydrogenation of MCH