53 research outputs found
Spatially dependent Rabi oscillations: an approach to sub-diffraction-limited CARS microscopy
We present a theoretical investigation of coherent anti-Stokes Raman
scattering (CARS) that is modulated by periodically depleting the ground state
population through Rabi oscillations driven by an additional control laser. We
find that such a process generates optical sidebands in the CARS spectrum and
that the frequency of the sidebands depends on the intensity of the control
laser light field. We show that analyzing the sideband frequency upon scanning
the beams across the sample allows one to spatially resolve emitter positions
where a spatial resolution of 65 nm, which is well below the diffraction-limit,
can be obtained
Observing charge separation in nanoantennas via ultrafast point-projection electron microscopy
Observing the motion of electrons on their natural nanometer length and femtosecond time scales is a fundamental goal of and an open challenge for contemporary ultrafast science. At present, optical techniques and electron microscopy mostly provide either ultrahigh temporal or spatial resolution, and microscopy techniques with combined space-time resolution require further development. In this study, we create an ultrafast electron source via plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used in an optical pump—electron probe experiment to study ultrafast photoemissions from a
nanometer-sized plasmonic antenna. We probe the real space motion of the photoemitted electrons with a 20-nm spatial resolution and a 25-fs time resolution and reveal the deflection of probe electrons by residual holes in the metal. This is a step toward time-resolved microscopy of electronic motion in nanostructures
Long-lived electron emission reveals localized plasmon modes in disordered nanosponge antennas
We report long-lived, highly spatially localized plasmon states on the surface of nanoporous gold nanoparticles-nanosponges-with high excitation efficiency. It is well known that disorder on the nanometer scale, particularly in two-dimensional systems, can lead to plasmon localization and large field enhancements, which can, in turn, be used to enhance nonlinear optical effects and to study and exploit quantum optical processes. Here, we introduce promising, three-dimensional model systems for light capture and plasmon localization as gold nanosponges that are formed by the dewetting of gold/ silver bilayers and dealloying. We study light-induced electron emission from single nanosponges, a nonlinear process with exponents of n approximate to 5...7, using ultrashort laser pulse excitation to achieve femtosecond time resolution. The long-lived electron emission process proves, in combination with optical extinction measurements and finite-difference time-domain calculations, the existence of localized modes with lifetimes of more than 20 fs. These electrons couple efficiently to the dipole antenna mode of each individual nanosponge, which in turn couples to the far-field. Thus, individual gold nanosponges are cheap and robust disordered nanoantennas with strong local resonances, and an ensemble of nanosponges constitutes a meta material with a strong polarization independent, nonlinear response over a wide frequency range
High passive CEP stability from a few-cycle, tunable NOPA-DFG system for observation of CEP-effects in photoemission
Ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering microscopy
We theoretically investigate ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. We propose a scheme based on ground-state depopulation, which is achieved via a control laser light field incident prior to the CARS excitation light fields. This ground-state depopulation results in a reduced CARS signal generation. With an appropriate choice of spatial beam profiles, the scheme can be used to increase the spatial resolution. Based on the density matrix formalism we calculate the CARS signal generation and find a CARS signal suppression by 75% due to ground-state depletion with a single control light field and by using two control light fields the CARS signal suppression can be enhanced to 94%. Additional control light fields will enhance the CARS suppression even further. In case of a single control light field we calculate resulting CARS images using a computer-generated test image including quantum and detector noise and show that the background from the limited CARS suppression can be removed by calculating difference images, yielding subdiffraction-limited resolution where the resolution achievable depends only on the intensity used
Carrier-envelope phase effects on the strong-field photoemission of electrons from metallic nanostructures
Sharp metallic nanotapers irradiated with few-cycle laser pulses are emerging
as a source of highly confined coherent electron wavepackets with attosecond
duration and strong directivity. The possibility to steer, control or switch
such electron wavepackets by light is expected to pave the way towards direct
visualization of nanoplasmonic field dynamics and real-time probing of electron
motion in solid state nanostructures. Such pulses can be generated by
strong-field induced tunneling and acceleration of electrons in the near-field
of sharp gold tapers within one half-cycle of the driving laser field. Here, we
show the effect of the carrier-envelope phase of the laser field on the
generation and motion of strong-field emitted electrons from such tips. This is
a step forward towards controlling the coherent electron motion in and around
metallic nanostructures on ultrashort length and time scales
Ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering microscopy
We theoretically investigate ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. We propose a scheme based on ground-state depopulation, which is achieved via a control laser light field incident prior to the CARS excitation light fields. This ground-state depopulation results in a reduced CARS signal generation. With an appropriate choice of spatial beam profiles, the scheme can be used to increase the spatial resolution. Based on the density matrix formalism we calculate the CARS signal generation and find a CARS signal suppression by 75% due to ground-state depletion with a single control light field and by using two control light fields the CARS signal suppression can be enhanced to 94%. Additional control light fields will enhance the CARS suppression even further. In case of a single control light field we calculate resulting CARS images using a computer-generated test image including quantum and detector noise and show that the background from the limited CARS suppression can be removed by calculating difference images, yielding subdiffraction-limited resolution where the resolution achievable depends only on the intensity used
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