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Register a new userFemtosecond phase-resolved microscopy of plasmon dynamics in individual gold nanospheres
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The selective optical detection of individual metallic nanoparticles (NPs) with high spatial and temporal resolution is a challenging endeavour, yet is key to the understanding of their optical response and their exploitation in applications from miniaturised optoelectronics and sensors to medical diagnostics and therapeutics. However, only few reports on ultrafast pump-probe spectroscopy on single small metallic NPs are available to date. Here, we demonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy in heterodyne detection to resolve for the first time the ultrafast changes of real and imaginary part of the dielectric function of single small (<40nm) spherical gold NPs. The results are quantitatively described via the transient electron temperature and density in gold considering both intraband and interband transitions at the surface plasmon resonance. This novel microscopy technique enables background-free detection of the complex susceptibility change even in highly scattering environments and can be readily applied to any metal nanostructure.
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We show that a dimer made of two gold nanospheres exhibits a remarkable efficiency for second-harmonic generation under femtosecond optical excitation. The detectable nonlinear emission for the given particle size and excitation wavelength arises when the two nanoparticles are as close as possible to contact, as in situ controlled and measured using the tip of an atomic force microscope. The excitation wavelength dependence of the second-harmonic signal supports a coupled plasmon resonance origin with radiation from the dimer gap. This nanometer-size light source might be used for high-resolution near-field optical microscopy.
We demonstrate that nanocavity plasmons generated a few nanometers away from a molecule can induce molecular motion. For this, we study the well-known rapid shuttling motion of zinc phthalocyanine molecules adsorbed on ultrathin NaCl films by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced light emission. Comparing spatially resolved single-molecule luminescence spectra from molecules anchored to a step edge with isolated molecules adsorbed on the free surface, we found that the azimuthal modulation of the Lamb shift is diminished in case of the latter. This is evidence that the rapid shuttling motion is remotely induced by plasmon-exciton coupling. Plasmon-induced molecular motion may open an interesting playground to bridge the nanoscopic and mesoscopic worlds by combining molecular machines with nanoplasmonics to control directed motion of single molecules without the need for local probes.
Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single femtosecond laser pulses. We find that the energy transfer from the fs laser pulse to the nanoparticles is limited by the Rayleigh scattering cross section, which in combination with the light absorption of the supporting substrate and protective layers determines the increase in the nanoparticle temperature. We investigate individual Co nanoparticles (8 to 20 nm in size) as a prototypical model system, using x-ray photoemission electron microscopy and scanning electron microscopy upon excitation with single femtosecond laser pulses of varying intensity and polarization. In agreement with calculations, we find no deterministic or stochastic reversal of the magnetization in the nanoparticles up to intensities where ultrafast demagnetization or all-optical switching is typically reported in thin films. Instead, at higher fluences, the laser pulse excitation leads to photo-chemical reactions of the nanoparticles with the protective layer, which results in an irreversible change in the magnetic properties. Based on our findings, we discuss the conditions required for achieving laser-induced switching in isolated nanomagnets.
The motion of electrons in or near solids, liquids and gases can be tracked by forcing their ejection with attosecond x-ray pulses, derived from femtosecond lasers. The momentum of these emitted electrons carries the imprint of the electronic state. Aberration corrected transmission electron microscopes have observed individual atoms, and have sufficient energy sensitivity to quantify atom bonding and electronic configurations. Recent developments in ultrafast electron microscopy and diffraction indicate that spatial and temporal information can be collected simultaneously. In the present work, we push the capability of femtosecond transmission electron microscopy (fs-TEM) towards that of the state of the art in ultrafast lasers and electron microscopes. This is anticipated to facilitate unprecedented elucidation of physical, chemical and biological structural dynamics on electronic time and length scales. The fs-TEM numerically studied employs a nanotip source, electrostatic acceleration to 70 keV, magnetic lens beam transport and focusing, a condenser-objective around the sample and a terahertz temporal compressor, including space charge effects during propagation. With electron emission equivalent to a 20 fs laser pulse, we find a spatial resolution below 10 nm and a temporal resolution of below 10 fs will be feasible for pulses comprised of on average 20 electrons. The influence of a transverse electric field at the sample is modelled, indicating that a field of 1 V/$mu$m can be resolved.
We report a simple, rapid, and quantitative wide-field technique to measure the optical extinction $sigma_{rm ext}$ and scattering $sigma_{rm sca}$ cross-section of single nanoparticles using wide-field microscopy enabling simultaneous acquisition of hundreds of nanoparticles for statistical analysis. As a proof of principle, we measured nominally spherical gold nanoparticles of 40,nm and 100,nm diameter and found mean values and standard deviations of $sigma_{rm ext}$ and $sigma_{rm sca}$ consistent with previous literature. Switching from unpolarized to linearly polarized excitation, we measured $sigma_{rm ext}$ as a function of the polarization direction, and used it to characterize the asphericity of the nanoparticles. The method can be implemented cost-effectively on any conventional wide-field microscope and is applicable to any nanoparticles.
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