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Non-linear enhancement of ultrafast X-ray diffraction through transient resonances.
Nat Commun
January 2025
SLAC National Accelerator Laboratory, Stanford PULSE Institute, Menlo Park, CA, USA.
Diffraction-before-destruction imaging with ultrashort X-ray pulses can visualize non-equilibrium processes, such as chemical reactions, with sub-femtosecond precision in the native environment. Here, a nanospecimen diffracts a single X-ray flash before it disintegrates. The sample structure can be reconstructed from the coherent diffraction image (CDI).
View Article and Find Full Text PDFOrganic Spacers Modulated Low Dose X-Ray Detection in Hybrid Halide 2D Perovskites: Unveiling Exciton Dynamics.
Small
January 2025
Department of Physics, Indian Institute of Technology Roorkee, Roorkee, 247667, India.
In this study, we investigate how modulating organic spacers in perovskites influences their X-ray detection performance and reveal the mechanism of low-dose detection with high sensitivity using femtosecond-transient absorption spectroscopy (fs-TAS). Particularly, we employ N,N,N',N'-tetramethyl-1,4-phenylenediammonium (TMPDA) and N,N-dimethylphenylene-p-diammonium (DPDA) as organic spacers to synthesize 2D perovskite single crystals (SCs). We find that DPDA-based SCs exhibit reduced interplanar spacing between inorganic layers, leading to increased lattice packing.
View Article and Find Full Text PDFConvergent-beam attosecond x-ray crystallography.
Struct Dyn
January 2025
Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany.
Sub-ångström spatial resolution of electron density coupled with sub-femtosecond to few-femtosecond temporal resolution is required to directly observe the dynamics of the electronic structure of a molecule after photoinitiation or some other ultrafast perturbation, such as by soft X-rays. Meeting this challenge, pushing the field of quantum crystallography to attosecond timescales, would bring insights into how the electronic and nuclear degrees of freedom couple, enable the study of quantum coherences involved in molecular dynamics, and ultimately enable these dynamics to be controlled. Here, we propose to reach this realm by employing convergent-beam x-ray crystallography with high-power attosecond pulses from a hard-x-ray free-electron laser.
View Article and Find Full Text PDFRevealing the reaction path of UVC bond rupture in cyclic disulfides with ultrafast x-ray scattering.
Sci Adv
January 2025
Department of Chemistry, Brown University, Providence, RI, USA.
Disulfide bonds are ubiquitous molecular motifs that influence the tertiary structure and biological functions of many proteins. Yet, it is well known that the disulfide bond is photolabile when exposed to ultraviolet C (UVC) radiation. The deep-UV-induced S─S bond fragmentation kinetics on very fast timescales are especially pivotal to fully understand the photostability and photodamage repair mechanisms in proteins.
View Article and Find Full Text PDFExploring the reaction dynamics of alanine racemase using serial femtosecond crystallography.
Sci Rep
December 2024
Department of Life Sciences, Pohang University of Science and Technology, Pohang, 37673, Kyungbook, Republic of Korea.
Alanine racemase (Alr) catalyzes the pyridoxal 5'-phosphate (PLP)-dependent racemization between L- and D-alanine in bacteria. Owing to the potential interest in targeting Alr for antibacterial drug development, several studies have determined the structures of Alr from different species, proposing models for the reaction mechanism. Insights into its reaction dynamics may be conducive to a better understanding of the Alr reaction mechanism.
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