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Marco Kloos

Publications and source records attributed to Marco Kloos.

3 recordsLinked to original sources

Time Resolved Study of Laser Induced Ultrafast Alloying Processes in Au/Pd Core Shell Nanorods

Femtosecond laser-induced alloying presents a novel approach to modifying bimetallic systems. Visualizing ultrafast processes during laser-induced alloying is essential to uncover fundamental mechanisms associated with phase transformations, which enables precise control over material composition and structure at the atomic level. In this study, we investigated the ultrafast dynamics of laser-induced alloying of Au/Pd core-shell nanorods using a time-resolved X-ray diffraction technique at an X-ray free-electron laser facility, capturing the structural evolution from picoseconds to microsecond timescales. We found that a laser fluence threshold of ~ 48 mJ/cm2 with 800 nm excitation is sufficient for melting and subsequent alloy formation. Above this threshold, the formation of Au1.51Pd0.49 was observed, and we found that alloying is not a single-step phenomenon; instead, it is a dynamic process involving interdiffusion.

cond-mat.mtrl-sci

3D-Printed Sheet Jet for Stable Megahertz Liquid Sample Delivery at X-ray Free Electron Lasers

X-ray Free Electron Lasers (XFELs) can probe chemical and biological reactions as they unfold with unprecedented spatial and temporal resolution. A principal challenge in this pursuit is the delivery of samples to the X-ray interaction point in a way that produces data of the highest possible quality and efficiency. This is hampered by constraints posed by the light source and operation within a beamline environment. For liquid samples, the solution typically involves a high-speed liquid jet, capable of keeping up with the rate of X-ray pulses. However, conventional jets are not ideal because of radiation-induced explosions of the jet, as well as their cylindrical geometry combined with the X-ray pointing instability of many beamlines causes the interaction volume to differ for every pulse. This complicates data analysis and contributes to measurement errors. An alternative geometry is a liquid sheet jet which, with its constant thickness over large areas, eliminates the X-ray pointing related problems. Since liquid sheets can be made very thin, the radiation-induced explosion is reduced, boosting their stability. They are especially attractive for experiments which benefit from small interaction volumes such as fluctuation X-ray scattering and several types of spectroscopy. Although they have seen increasing use for soft X-ray applications in recent years, there has not yet been wide-scale adoption at XFELs. Here, we demonstrate liquid sheet jet sample injection at the European XFEL. We evaluate several aspects of its performance relative to a conventional liquid jet including thickness profile, stability, and radiation-induced explosion dynamics at high repetition rates. The sheet jet exhibits superior performance across these critical experimental parameters. Its minute thickness also suggests ultrafast single-particle solution scattering is a possibility.

physics.ins-det

Three-dimensional view of ultrafast dynamics in photoexcited bacteriorhodopsin

Bacteriorhodopsin (bR) is a light-driven proton pump. We use time-resolved crystallography at an X-ray free-electron laser to follow the structural changes in multiphoton-excited bR from 250 femtoseconds to 10 picoseconds. Quantum chemistry and ultrafast spectroscopy allow identifying a sequential two-photon absorption process, leading to excitation of a tryptophan residue flanking the retinal chromophore, as a first manifestation of multi-photon effects. We resolve distinct stages in the structural dynamics of the all-trans retinal in photoexcited bR to a highly twisted 13-cis conformation. Other active site sub-picosecond rearrangements include correlated vibrational motions of the electronically excited retinal chromophore, the surrounding amino acids and water molecules as well as their hydrogen bonding network. These results show that this extended photo-active network forms an electronically and vibrationally coupled system in bR, and most likely in all retinal proteins.

physics.bio-ph