Projecting picosecond lattice dynamics through x-ray topography

A method for time-resolved x-ray diffraction studies has been demonstrated. As a test case, coherent acoustic phonon propagation into crystalline InSb is observed using a laser plasma x-ray source. An extended x-ray topogram of the semiconductor's surface was projected onto a high spatial resolution x-ray detector and acoustic phonons were excited by rapidly heating the crystal's surface with a femtosecond laser pulse. A correlation between the spatial position on the x-ray detector and the time of arrival of the laser pulse was encoded into the experimental geometry by tilting the incident laser pulse with an optical grating. This approach enabled a temporal window of 200 ps to be sampled in a single topogram, thereby negating the disadvantages of pulse-to-pulse fluctuations in the intensity and spectrum of the laser-plasma source. (C) 2002 American Institute of Physics

Time-resolved X-ray diffraction studies of phonons and phase transitions

This thesis summarizes work in which time-resolved X-ray diffraction has been used to probe crystalline materials, thereby revealing the dynamics of phonons and phase transitions. X-ray diffraction is the standard tool in investigations of structure on the atomic scale. It has been used for a long time, and has successfully helped scientists to find the structure of a wide range of materials. The use of ultrafast time-resolved X-ray diffraction is a strongly emerging field which is still under development. Impulsive strain pulses, or coherent acoustic phonons, have been probed using optical techniques for at least two decades. Yet, optical pulses can only probe the surface of a semiconductor. X-rays penetrate deeper and can follow the phonons as they propagate into the sample. Real time studies of phase transitions have also been conducted using optical methods. These measurements are indirect in the sense that they probe the susceptibility change of the sample rather than the positions of the atoms. Again, time-resolved X-ray diffraction can give new insights into the field by probing the structural changes directly. This thesis focuses mainly on experimental work in which time-resolved X-ray diffraction has been used to probe phonons or samples undergoing phase transitions. A brief theoretical background will also be given, as well as a description of beamline D611 at MAX-lab, a synchrotron beamline for time-resolved X-ray diffraction measurements which has been developed during the work for this thesis

Studies of resolidification of non-thermally molten InSb using time-resolved X-ray diffraction

We have used time-resolved X-ray diffraction to monitor the resolidification process of molten InSb. Melting was induced by an ultra-short laser pulse and the measurement conducted in a high-repetition-rate multishot experiment. The method gives direct information about the nature of the transient regrowth and permanently damaged layers. It does not rely on models based on surface reflectivity or second harmonic generation (SHG). The measured resolidification process has been modeled with a 1-D thermodynamic heat-conduction model. Important parameters like sample temperature, melting depth and amorphous surface layer thickness come directly out of the data, while mosaicity of the sample and free carrier density can be quantified by comparing with models. Melt depths up to 80 nm have been observed and regrowth velocities in the range 2-8 m/s have been measured

Time resolved X-ray diffraction and non-thermal inelastic X-ray scattering

Atomic processes like e.g. molecular vibrations, chemical reactions or phase transitions happen on picosecond down to femtosecond time scales. Novel pulsed X-ray sources or alternatively ultrafast X-ray detectors allow the investigation of these processes in real time. A powerful tool for the investigation of the dynamics in crystalline materials is time resolved X-ray diffraction (TRXD). As an example the authors present the measurement of "phonon branch folding" in a GaSb/InAs superlattice by means of TRXD. In the second part we look forward to the near future of TRXD. X-ray scattering from coherent acoustic and optical phonons has recently become describable within the framework of dynamical diffraction theory. This theory provides the means for the detailed modeling of how various lattice dynamical processes manifest themselves in the diffracted X-ray signal. Simulations are presented showing the effects of coherent acoustic and optical phonons on the rocking curve of quartz (010

Picosecond x-ray studies of coherent folded acoustic phonons in a periodic semiconductor heterostructure

Zone folded coherent acoustic phonons were generated in a multilayered GaSb/InAs epitaxial heterostructure via rapid heating by femtosecond laser pulses. These phonons were probed by means of ultrafast x-ray diffraction. Phonons both from the fundamental acoustic branch and the first back-folded branch were detected. This represents the first clear evidence for phonon branch folding based directly on the atomic motion to which x-ray diffraction is sensitive. From a comparison of the measured phonon-modulated x-ray reflectivity with simulations, evidence was found for a reduction of the laser penetration depth. This reduction can be explained by the self-modulation of the absorption index due to photogenerated free carriers

Opportunities and challenges using short-pulse X-ray sources.

Free-electron lasers will change the way we carry out time-resolved X-ray experiments. At present date, we use laser-produced plasma sources or synchrotron radiation. Laser-produced plasma sources have short pulses, but unfortunately large pulse-to-pulse fluctuations and large divergence. Synchrotron radiation from third generation source provide collimated and stable beams, but unfortunately long pulses. This means that either the time-resolution is limited to 100 ps or rather complex set-ups involving slicing or streak cameras are needed. Hard X-ray free-electron lasers will combine the best properties of present-day sources and increase the number of photons by many orders of magnitude. Already today, a precursor to the free-electron lasers has been built at Stanford Linear Accelerator Centre (SLAC). The Sub-Picosecond Photon Source (SPPS) has already shown the opportunities and challenges of using short-pulse X-ray sources

Lipid Nanoparticles Deliver the Therapeutic VEGFA mRNA In Vitro and In Vivo and Transform Extracellular Vesicles for Their Functional Extensions

Lipid nanoparticles (LNPs) are currently used to transport functional mRNAs, such as COVID-19 mRNA vaccines. The delivery of angiogenic molecules, such as therapeutic VEGF-A mRNA, to ischemic tissues for producing new blood vessels is an emerging strategy for the treatment of cardiovascular diseases. Here, the authors deliver VEGF-A mRNA via LNPs and study stoichiometric quantification of their uptake kinetics and how the transport of exogenous LNP-mRNAs between cells is functionally extended by cells’ own vehicles called extracellular vesicles (EVs). The results show that cellular uptake of LNPs and their mRNA molecules occurs quickly, and that the translation of exogenously delivered mRNA begins immediately. Following the VEGF-A mRNA delivery to cells via LNPs, a fraction of internalized VEGF-A mRNA is secreted via EVs. The overexpressed VEGF-A mRNA is detected in EVs secreted from three different cell types. Additionally, RNA-Seq analysis reveals that as cells’ response to LNP-VEGF-A mRNA treatment, several overexpressed proangiogenic transcripts are packaged into EVs. EVs are further deployed to deliver VEGF-A mRNA in vitro and in vivo. Upon equal amount of VEGF-A mRNA delivery via three EV types or LNPs in vitro, EVs from cardiac progenitor cells are the most efficient in promoting angiogenesis per amount of VEGF-A protein produced. Intravenous administration of luciferase mRNA shows that EVs could distribute translatable mRNA to different organs with the highest amounts of luciferase detected in the liver. Direct injections of VEGF-A mRNA (via EVs or LNPs) into mice heart result in locally produced VEGF-A protein without spillover to liver and circulation. In addition, EVs from cardiac progenitor cells cause minimal production of inflammatory cytokines in cardiac tissue compared with all other treatment types. Collectively, the data demonstrate that LNPs transform EVs as functional extensions to distribute therapeutic mRNA between cells, where EVs deliver this mRNA differently than LNPs. CC BY 4.0© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.E-mail: [email protected] authors acknowledge the support from the National Genomics Infrastructure in Stockholm funded by Science for Life (SciLife) Laboratory, the Knut and Alice Wallenberg Foundation and the Swedish Research Council, and SNIC/Uppsala Multidisciplinary Center for Advanced Computational Science for assistance with massively parallel sequencing and access to the UPPMAX computational infrastructure. Moreover, the authors acknowledge Mr. Mario Soriano Navarro at the Responsable Servicio Microscopía Electrónica, Valencia Spain, for technical assistance. This work was supported by grants from the Swedish Foundation of Strategic Research (Stiftelsen för strategisk forskning: SSF) in the Industrial Research Centre, FoRmulaEx - Nucleotide Functional Drug Delivery (Grant ID: IRC15-0065), the Swedish research council (VR, Grant ID: 2020-01316), and the Swedish governmental agency for innovation systems (VINNOVA, Grant ID: 2017-02960). This research was also funded by the Systems Biology Research Centre at the University of Skövde under grants from the Knowledge Foundation (Grant ID: 20160330).</p