The generation and dynamics of plasmon-induced hot carriers in gold nanoparticles offer crucial insights into nonequilibrium states for energy applications, yet the underlying mechanisms remain experimentally elusive. Here, we leverage ultrafast X-ray absorption spectroscopy (XAS) to directly capture hot carrier dynamics with sub-50 fs temporal resolution, providing clear evidence of plasmon decay mechanisms. We observe the sequential processes of Landau damping (~25 fs) and hot carrier thermalization (~1.5 ps), identifying hot carrier formation as a significant decay pathway. Energy distribution measurements reveal carriers in non-Fermi-Dirac states persisting beyond 500 fs and observe electron populations exceeding single-photon excitation energy, indicating the role of an Auger heating mechanism alongside traditional impact excitation. These findings deepen the understanding of hot carrier behavior under localized surface plasmon resonance, offering valuable implications for applications in photocatalysis, photovoltaics, and phototherapy. This work establishes a methodological framework for studying hot carrier dynamics, opening avenues for optimizing energy transfer processes in nanoscale plasmonic systems.
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http://dx.doi.org/10.1038/s41467-025-57657-1 | DOI Listing |
ACS Nano
March 2025
Department of Chemistry Education, Korea National University of Education (KNUE), Chungbuk 28173, Republic of Korea.
Hot carriers, generated through nonadiabatic energy dissipation during exothermic catalytic reactions, play a pivotal role in enhancing catalytic performance. Upon generation, hot electrons typically reside in the sp-band above the Fermi level, while hot holes are formed in the -band below the Fermi level, following the energy distribution of the metal's electronic structure. However, it has been technically challenging to simultaneously capture and understand the flow of these two opposite charges during chemical reactions.
View Article and Find Full Text PDFJ Colloid Interface Sci
March 2025
National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, East China University of Science and Technology, Shanghai 200237, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200237, China. Electronic address:
Fe-based metal-organic frameworks (Fe-MOFs) have been extensively studied as fascinating photocatalysts due to their tunable structure and appealing light response. However, the application of traditional three-dimensional (3D) Fe-MOFs is limited by rapid carrier recombination and inaccessible active sites. In this work, a novel two-dimensional (2D) Bi decorated Fe-MOFs nanosheet photocatalyst was constructed, which exhibits significantly enhanced solar-driven photocatalytic activity due to the synergistic effect of localized surface plasmon resonance (LSPR) and surface high-density exposed metal active sites.
View Article and Find Full Text PDFSci Adv
March 2025
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Yuseong-Gu, Daejeon 34141, Republic of Korea.
While energetic plasmonic hot carriers in nonthermal equilibrium states have pushed the limits of energy conversion efficiency in plasmon-driven photocatalysts and optoelectronics, the acceleration of plasmonic hot-hole flux remains a challenge. Here, we demonstrate an approach to control the generation and injection nature of plasmonic hot holes released from Au nanomesh/p-type GaN (p-GaN) Schottky architecture by modulating polarity of p-GaN. This polarity modulation enhances the flux of hot holes into the plasmonic platform, thereby accelerating Landau damping stemming from increased effective heat capacity of hot electrons in the metallic nanomaterial.
View Article and Find Full Text PDFNat Commun
March 2025
Institute of Physical Chemistry, Polish Academy of Sciences, Warsaw, Poland.
The generation and dynamics of plasmon-induced hot carriers in gold nanoparticles offer crucial insights into nonequilibrium states for energy applications, yet the underlying mechanisms remain experimentally elusive. Here, we leverage ultrafast X-ray absorption spectroscopy (XAS) to directly capture hot carrier dynamics with sub-50 fs temporal resolution, providing clear evidence of plasmon decay mechanisms. We observe the sequential processes of Landau damping (~25 fs) and hot carrier thermalization (~1.
View Article and Find Full Text PDFPLoS One
March 2025
Advanced Manufacturing Alliance, Energy and Resources Institute, Charles Darwin University, Darwin, Australia.
Nickel aluminium bronze (NAB) alloys are known for their excellent strength and corrosion resistance, making them suitable for maritime and industrial applications. NAB is producible by Powder Metallurgy (PM) but typically requires high compaction pressure. The objective of this study is to investigate the manufacturing of NAB using the cold spray additive manufacturing (AM) process and to compare its properties to those produced by traditional methods such as casting and PM.
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