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Dynamics of optically excited plasmonic nanoparticles are presently understood as a series of scattering events involving the initiation of nanoparticle breathing oscillations. According to established models, these are caused by statistical heat transfer from thermalized electrons to the lattice. An additional contribution by hot-electron pressure accounts for phase mismatches between theory and experimental observations. However, direct experimental studies resolving the breathing-oscillation excitation are still missing. We used optical transient-absorption spectroscopy and time-resolved single-particle X-ray diffractive imaging to access the electron system and lattice. The time-resolved single-particle imaging data provided structural information directly on the onset of the breathing oscillation and confirmed the need for an additional excitation mechanism for thermal expansion. We developed a new model that reproduces all of our experimental observations. We identified optically induced electron density gradients as the initial driving source.
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http://dx.doi.org/10.1021/acs.nanolett.3c00920 | DOI Listing |
ACS Appl Mater Interfaces
November 2024
Université Paris-Saclay, ENS Paris-Saclay, CNRS, CentraleSupélec, LuMIn, LuMIn, 91190 Gif-sur-Yvette, France.
Understanding the dynamics of electrical signals within neuronal assemblies is crucial to unraveling complex brain functions. Despite recent advances in employing optically active nanostructures in transmembrane potential sensing, there remains room for improvement in terms of response time and sensitivity. Here, we report the development of such a nanosensor capable of detecting electric fields with a submillisecond response time at the single-particle level.
View Article and Find Full Text PDFNanoscale
September 2024
School of Chemistry, University of Birmingham, Edgbaston, B15 2TT, UK.
Osmium(II) complexes have attractive properties for potential theranostic agents given their anticancer activitiy, their redox potentials favourable for biological transformations within cancer cells and their luminescence in the near infrared (NIR) region. To achieve localised detection and delivery, gold nanoparticles (AuNP) provide an attractive scaffold to attach multiple luminescent agents on a single particle and provide a multimodal platform for detection and loaclaised delivery. We have developed 13 nm and 25 nm AuNP decorated with an osmium complex based on 1,10-phenantholine and surface active bipyridine ligands, OsPhenSS for live cell imaging and singlet oxygen generation, notated as OsPhenSS·AuNP13 and OsPhenSS·AuNP25.
View Article and Find Full Text PDFCommun Biol
August 2024
Department of Chemistry and Chemical Biology, Cornell University, 14853, Ithaca, NY, USA.
Transglutaminase 2 (TG2) is a GTP-binding, protein-crosslinking enzyme that has been investigated as a therapeutic target for Celiac disease, neurological disorders, and aggressive cancers. TG2 has been suggested to adopt two conformational states that regulate its functions: a GTP-bound, closed conformation, and a calcium-bound, crosslinking-active open conformation. TG2 mutants that constitutively adopt an open conformation are cytotoxic to cancer cells.
View Article and Find Full Text PDFFront Mol Biosci
July 2024
LCLS, SLAC National Accelerator Laboratory, Stanford University, Palo Alto, CA, United States.
Molecules are essential building blocks of life and their different conformations (i.e., shapes) crucially determine the functional role that they play in living organisms.
View Article and Find Full Text PDFACS Nano
July 2024
Univ. Grenoble Alpes, CEA Grenoble, IRIG, MEM, NRX, 17 rue des Martyrs, F-38000 Grenoble, France.
Understanding the strain dynamic behavior of catalysts is crucial for the development of cost-effective, efficient, stable, and long-lasting catalysts. Using time-resolved Bragg coherent diffraction imaging at the fourth generation Extremely Brilliant Source of the European Synchrotron (ESRF-EBS), we achieved subsecond time resolution during chemical reactions. Upon investigation of Pt nanoparticles during CO oxidation, the three-dimensional strain profile highlights significant changes in the surface and subsurface regions, where localized strain is probed along the [111] direction.
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