73 research outputs found
Understanding Hot-Electron Generation and Plasmon Relaxation in Metal Nanocrystals: Quantum and Classical Mechanisms
Generation of energetic (hot) electrons is an intrinsic property of any
plasmonic nanostructure under illumination. Simultaneously, a striking
advantage of metal nanocrystals over semiconductors lies in their very large
absorption cross sections. Therefore, metal nanostructures with strong and
tailored plasmonic resonances are very attractive for photocatalytic
applications. However, the central questions regarding plasmonic hot electrons
are how to quantify and extract the optically-excited energetic electrons in a
nanocrystal. We develop a theory describing the generation rates and the
energy-distributions of hot electrons in nanocrystals with various geometries.
In our theory, hot electrons are generated owing to surfaces and hot spots. The
formalism predicts that large optically-excited nanocrystals show the
excitation of mostly low-energy Drude electrons, whereas plasmons in small
nanocrystals involve mostly hot electrons. The energy distributions of
electrons in an optically-excited nanocrystal show how the quantum many-body
state in small particles evolves towards the classical state described by the
Drude model when increasing nanocrystal size. We show that the rate of surface
decay of plasmons in nanocrystals is directly related to the rate of generation
of hot electrons. Based on a detailed many-body theory involving kinetic
coefficients, we formulate a simple scheme describing the plasmon's dephasing.
In most nanocrystals, the main decay mechanism of a plasmon is the Drude
friction-like process and the secondary path comes from generation of hot
electrons due to surfaces and electromagnetic hot spots. This latter path
strongly depends on the size, shape and material of the nanocrystal,
correspondingly affecting its efficiency of hot-electron production. The
results in the paper can be used to guide the design of plasmonic nanomaterials
for photochemistry and photodetectors.Comment: 90 pages, 21 figures, including Supplementary Informatio
What's so Hot about Electrons in Metal Nanoparticles?
Metal nanoparticles are excellent light absorbers. The absorption processes
create highly excited electron-hole pairs and recently there has been interest
in harnessing these hot charge carriers for photocatalysis and solar energy
conversion applications. The goal of this Perspectives article is to describe
the dynamics and energy distribution of the charge carriers produced by photon
absorption, and the implications for the photocatalysis mechanism. We will also
discuss how spectroscopy can be used to provide insight into the coupling
between plasmons and molecular resonances. In particular, the analysis shows
that the choice of material and shape of the nanocrystal can play a crucial
role in hot electron generation and coupling between plasmons and molecular
transitions. The detection and even calculation of many-body hot-electron
processes in the plasmonic systems with continuous spectra of electrons and
short lifetimes are challenging, but at the same time very interesting from the
point of view of both potential applications and fundamental physics. We
propose that developing an understanding of these processes will provide a
pathway for improving the efficiency of plasmon-induced photocatalysis.Comment: To be published in ACS Energy. 41 pages and 8 figures, including
Supplementary Informatio
On the age of the hominid fossils at the Sima de los Huesos, Sierra de Atapuerca, Spain: paleomagnetic evidence
We report new paleomagnetic data for the Middle Pleistocene hominid-bearing strata in the Sima de los Huesos, North Spain. Sediments (brown muds with human and bear fossils and the underlying sterile clayey and sandy unit) preserve both normal and reversed magnetic components. The sterile unit has exclusively reversed magnetization, dating back to the Matuyama Chron, and thus is Lower Pleistocene in age. The overlying fossiliferous muds have a dominant normal magnetization that overprints a partially resolved reversed magnetization. These data are compatible with one of the reversal events that occurred during the Brunhes Chron. Combined with the existing U-series dates and evidence from the macro- and microfauna, these paleomagnetic results suggest an age of the hominid fossils between 325 to 205 ka, whereas the underlying sand and silts are older than 780 ka.This research was supported by DGES grants PB96-0815 and PB96-1026-C03, and by the Unidad Asociada CSIC-UCM.Peer reviewe
Mode specific dynamics for the acoustic vibrations of a gold nanoplate
The vibrational modes of semiconductor and metal nanostructures occur in the MHz to GHz frequency range, depending on dimensions. These modes are at the heart of nano-optomechanical devices, and understanding how they dissipate energy is important for applications of the devices. In this paper ultrafast transient absorption microscopy has been used to examine the breathing modes of a single gold nanoplate, where up to four overtones were observed. Analysis of the frequencies and amplitudes of the modes using a simple continuum mechanics model shows that the system behaves as a free plate, even though it is deposited onto a surface with no special preparation. The overtones decay faster than the fundamental mode, which is not predicted by continuum mechanics calculations of mode damping due to radiation of sound waves. Possible reasons for this effect include frequency dependent thermoelastic effects in the nanoplate, and/or flow of acoustic energy out of the excitation region
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