Near- and far-field study of polarization-dependent surface plasmon resonance in bowtie nano-aperture arrays.

Bowtie nano-apertures can confine light into deep subwavelength volumes with extreme field enhancement, making them a useful tool for various applications such as optical trapping, deep subwavelength imaging, nanolithography, and sensors. However, the correlation between the near- and far-field properties of bowtie nano-aperture arrays has yet to be fully explored. In this study, we experimentally investigated the polarization-dependent surface plasmon resonance in bowtie nano-aperture arrays using both optical transmission spectroscopy and photoemission electron microscopy. The experimental results reveal a nonlinear redshift in the transmission spectra as the gap size of the bowtie nanoaperture decreases for vertically polarized light, while the transmission spectra remain unchanged with different gap sizes for horizontally polarized light. To elucidate the underlying mechanisms, we present simulated charge and current distributions, revealing how the electrons respond to light and generate the plasmonic fields. These near-field distributions were verified by photoemission electron microscopy. This study provides a comprehensive understanding of the plasmonic properties of bowtie nano-aperture, enabling their further applications, one of which is the optical switching of the resonance wavelength in the widely used visible spectral region without changing the geometry of the nanostructure.

Low chromatic Fresnel lens for broadband attosecond XUV pulse applications.

Fresnel zone plates show a great potential in achieving high spatial resolution imaging or focusing for XUV and soft/hard X-ray radiation, however they are usually strictly monochromatic due to strong chromatic dispersion and thus do not support broad radiation spectra, preventing their application to attosecond XUV pulses. Here we report on the design and theoretical simulations based on the design of an achromatic hybrid optics combining both, a refractive and diffractive lens in one optical element. We are able to show by calculation that the chromatic dispersion along the optical axis can be greatly reduced compared to a standard Fresnel zone plate while preserving the temporal structure of the attosecond XUV pulses at focus.

Generation of circularly polarized high harmonic radiation using a transmission multilayer quarter waveplate.

High harmonic radiation is meanwhile nearly extensively used for the spectroscopic investigation of electron dynamics with ultimate time resolution. The majority of high harmonic beamlines provide linearly polarized radiation created in a gas target. However, circular polarization greatly extends the spectroscopic possibilities for high harmonics, especially in the analysis of samples with chirality or prominent spin polarization. We produced a free-standing multilayer foil as a transmission EUV quarter waveplate and applied it for the first time to high harmonic radiation. We measured a broadband (4.6 eV FWHM) ellipticity of 75% at 66 eV photon energy with a transmission efficiency of 5%. The helicity is switchable and the ellipticity can be adjusted to lower values by angle tuning. As a single element it can be easily integrated in any existing harmonic beamline without major changes.

High-order femtosecond vortices up to the 30th order generated from a powerful mode-locked Hermite-Gaussian laser.

Femtosecond vortex beams are of great scientific and practical interest because of their unique phase properties in both the longitudinal and transverse modes, enabling multi-dimensional quantum control of light fields. Until now, generating femtosecond vortex beams for applications that simultaneously require ultrashort pulse duration, high power, high vortex order, and a low cost and compact laser source has been very challenging due to the limitations of available generation methods. Here, we present a compact apparatus that generates powerful high-order femtosecond vortex pulses via astigmatic mode conversion from a mode-locked Hermite-Gaussian Yb:KGW laser oscillator in a hybrid scheme using both the translation-based off-axis pumping and the angle-based non-collinear pumping techniques. This hybrid scheme enables the generation of femtosecond vortices with a continuously tunable vortex order from the 1st up to the 30th order, which is the highest order obtained from any femtosecond vortex laser source based on a mode-locked oscillator. The average powers and pulse durations of all resulting vortex pulses are several hundred milliwatts and <650 fs, respectively. In particular, 424-fs 11th-order vortex pulses have been achieved with an average power of 1.6 W, several times more powerful than state-of-the-art oscillator-based femtosecond vortex sources.

Complete characterization of ultrafast optical fields by phase-preserving nonlinear autocorrelation.

Nonlinear autocorrelation was one of the earliest and simplest tools for obtaining partial temporal information about an ultrashort optical pulse by gating it with itself. However, since the spectral phase is lost in a conventional autocorrelation measurement, it is insufficient for a full characterization of an ultrafast electric field, requiring additional spectral information for phase retrieval. Here, we show that introducing an intensity asymmetry into a conventional nonlinear interferometric autocorrelation preserves some spectral phase information within the autocorrelation signal, which enables the full reconstruction of the original electric field, including the direction of time, using only a spectrally integrating detector. We call this technique Phase-Enabled Nonlinear Gating with Unbalanced Intensity (PENGUIN). It can be applied to almost any existing nonlinear interferometric autocorrelator, making it capable of complete optical field characterization and thus providing an inexpensive and less complex alternative to methods relying on spectral measurements, such as frequency-resolved optical gating (FROG) or spectral phase interferometry for direct electric-field reconstruction (SPIDER). More importantly, PENGUIN allows the precise characterization of ultrafast fields in non-radiative (e.g., plasmonic) nonlinear optical interactions where spectral information is inaccessible. We demonstrate this novel technique through simulations and experimentally by measuring the electric field of ~6-fs laser pulses from a Ti:sapphire oscillator. The results are validated by comparison with the well-established FROG method.

Time of flight-photoemission electron microscope for ultrahigh spatiotemporal probing of nanoplasmonic optical fields.

Nanoplasmonic excitations as generated by few-cycle laser pulses on metal nanostructures undergo ultrafast dynamics with timescales as short as a few hundred attoseconds (1 as = 10(-18) s). So far, the spatiotemporal dynamics of optical fields localized on the nanoscale (nanoplasmonic field) have been hidden from direct access in the real space and time domain. An approach which combines photoelectron emission microscopy and attosecond streaking spectroscopy and which provides direct and non-invasive access to the nanoplasmonic field with nanometer-scale spatial resolution and temporal resolution of the order of 100 as has been proposed (Stockman et al 2007 Nat. Photon. 1 539). To implement this approach, a time of flight-photoemission electron microscope (TOF-PEEM) with ∼25 nm spatial and ∼50 meV energy resolution, which has the potential to detect a nanoplasmonic field with nanometer spatial and attosecond temporal resolution, has been developed and characterized using a 400 nm/60 ps pulsed diode laser. The first experimental results obtained using this newly developed TOF-PEEM in a two-photon photoemission mode with a polycrystalline Cu sample and an Ag microstructure film show that the yield and the kinetic energy of the emitted photoelectrons are strongly affected by the nanolocalized plasmonic field.

Interferometric time- and energy-resolved photoemission electron microscopy for few-femtosecond nanoplasmonic dynamics.

We report a time-resolved normal-incidence photoemission electron microscope with an imaging time-of-flight detector using ∼7-fs near-infrared laser pulses and a phase-stabilized interferometer for studying ultrafast nanoplasmonic dynamics via nonlinear photoemission from metallic nanostructures. The interferometer's stability (35 ± 6 as root-mean-square from 0.2 Hz to 40 kHz) as well as on-line characterization of the driving laser field, which is a requirement for nanoplasmonic near-field reconstruction, is discussed in detail. We observed strong field enhancement and few-femtosecond localized surface plasmon lifetimes at a monolayer of self-assembled gold nanospheres with ∼40 nm diameter and ∼2 nm interparticle distance. A wide range of plasmon resonance frequencies could be simultaneously detected in the time domain at different nanospheres, which are distinguishable already within the first optical cycle or as close as about ±1 fs around time-zero. Energy-resolved imaging (microspectroscopy) additionally revealed spectral broadening due to strong-field or space charge effects. These results provide a clear path toward visualizing optically excited nanoplasmonic near-fields at ultimate spatiotemporal resolution.