Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8% expansion of the Au-Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1039/c4cp03301a | DOI Listing |
Nat Commun
January 2025
Department of Physics, ETH Zürich, Otto-Stern-Weg 1, 8093, Zürich, Switzerland.
Quantum magnetometers based on spin defects in solids enable sensitive imaging of various magnetic phenomena, such as ferro- and antiferromagnetism, superconductivity, and current-induced fields. Existing protocols primarily focus on static fields or narrow-band dynamical signals, and are optimized for high sensitivity rather than fast time resolution. Here, we report detection of fast signal transients, providing a perspective for investigating the rich dynamics of magnetic systems.
View Article and Find Full Text PDFSci 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 PDFJ Am Chem Soc
January 2025
Department of Chemistry and the Manitoba Institute for Materials, University of Manitoba, 144 Dysart Road, Winnipeg, Manitoba R3T 2N2, Canada.
The ability to manipulate excited-state decay cascades using molecular structure is essential to the application of abundant-metal photosensitizers and chromophores. Ligand design has yielded some spectacular results elongating charge-transfer excited state lifetimes of Fe(II) coordination complexes, but triplet metal-centered (MC) excited states─recently demonstrated to be critical to the photoactivity of isoelectronic Co(III) polypyridyls─have to date remained elusive, with temporally isolable examples limited to the picosecond regime. With this report, we show how strong-field donors and intramolecular π-stacking can conspire to stabilize a long-lived MC excited state for a remarkable 4.
View Article and Find Full Text PDFNat Commun
December 2024
Department of Chemical Engineering, Electrochemical Innovation Lab, University College London, London, UK.
High-temperature proton exchange membrane fuel cells (HT-PEMFCs) offer solutions to challenges intrinsic to low-temperature PEMFCs, such as complex water management, fuel inflexibility, and thermal integration. However, they are hindered by phosphoric acid (PA) leaching and catalyst migration, which destabilize the critical three-phase interface within the membrane electrode assembly (MEA). This study presents an innovative approach to enhance HT-PEMFC performance through membrane modification using picosecond laser scribing, which optimises the three-phase interface by forming a graphene-like structure that mitigates PA leaching.
View Article and Find Full Text PDFRev Sci Instrum
December 2024
Lawrence Livermore National Laboratory, Livermore, California 94550, USA.
Ultra-intense short-pulse lasers interacting with matter are capable of generating exceptionally bright secondary radiation sources. The short pulse duration (picoseconds to nanoseconds), small source size (sub-mm), and comparable high peak flux to conventional single particle sources make them an attractive source for radiography using a combination of particle species, known as multimodal imaging. Simultaneous x-ray and MeV neutron imaging of multi-material objects can yield unique advantages for material segmentation and identification within the full sample.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!