Murat Sivis

Nanostructure-enhanced atomic line emission

Arising from S. Kim et al. 453, 757–760 (2008)10.1038/nature07012; Kim et al. replyPlasmonic nanostructures offer unique possibilities for enhancing linear and nonlinear optical processes. Recently, Kim et al. reported nanostructure-enhanced high harmonic generation (HHG). Here, using nearly identical conditions, we demonstrate extreme-ultraviolet (EUV) emission from gas-exposed nanostructures, but come to entirely different conclusions: instead of HHG, we observe line emission of neutral and ionized gas atoms. We also discuss fundamental physical aspects limiting nanostructure-based HHG.

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam

We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9Å focused beam diameter, 200fs pulse duration and 0.6eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams.

Generation and bistability of a waveguide nanoplasma observed by enhanced extreme-ultraviolet fluorescence.

We present a study of the highly nonlinear optical excitation of noble gases in tapered hollow waveguides using few-femtosecond laser pulses. The local plasmonic field enhancement induces the generation of a nanometric plasma, resulting in incoherent extreme-ultraviolet fluorescence from optical transitions of neutral and ionized xenon, argon, and neon. Despite sufficient intensity in the waveguide, high-order harmonic generation is not observed. The fluorescent emission exhibits a strong bistability manifest as an intensity hysteresis, giving strong indications for multistep collisional excitations.

Tailored semiconductors for high-harmonic optoelectronics

Hitting the highs in solid state The ability to generate high harmonics of optical frequencies through the nonlinear interaction between intense light pulses and gas atoms has opened up the area of ultrafast optics and spectroscopy. Sivis et al. now show that high harmonics can also be generated with a solid-state sample. They used nanofabricated structured targets of ZnO and varied the chemical composition of the sample to demonstrate that (modest) high harmonics can be generated as the light interacts with the target materials. The results present the possibility of developing solid-state ultrafast optical devices. Science, this issue p. 303 Nanofabricated structures and chemical composition can tune the generation of high harmonics from solid-state targets. The advent of high-harmonic generation in gases 30 years ago set the foundation for attosecond science and facilitated ultrafast spectroscopy in atoms, molecules, and solids. We explore high-harmonic generation in the solid state by means of nanostructured and ion-implanted semiconductors. We use wavelength-selective microscopic imaging to map enhanced harmonic emission and show that the generation medium and the driving field can be locally tailored in solids by modifying the chemical composition and morphology. This enables the control of high-harmonic technology within precisely engineered solid targets. We demonstrate customized high-harmonic wave fields with wavelengths down to 225 nanometers (ninth-harmonic order of 2-micrometer laser pulses) and present an integrated Fresnel zone plate target in silicon, which leads to diffraction-limited self-focusing of the generated harmonics down to 1-micrometer spot sizes.

An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

Nanoscale magnetic imaging using circularly polarized high-harmonic radiation

We introduce laboratory-scale magneto-optical imaging with sub–50-nm resolution using high-harmonic radiation. This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the exceptional coherence of high harmonics, this approach will facilitate quantitative, element-specific, and spatially resolved studies of ultrafast magnetization dynamics, advancing both fundamental and applied aspects of nanoscale magnetism.

Phase ordering of charge density waves traced by ultrafast low-energy electron diffraction

A tracing of the phase-ordering kinetics of a charge density wave system demonstrates the potential of ultrafast low-energy electron diffraction for studying phase transitions and ordering phenomena at surfaces and in low-dimensional systems.

Coherent diffractive imaging beyond the projection approximation: waveguiding at extreme ultraviolet wavelengths

We study extreme-ultraviolet wave propagation within optically thick nanostructures by means of high-resolution coherent diffractive imaging using high-harmonic radiation. Exit waves from different objects are reconstructed by phase retrieval algorithms, and are shown to be dominated by waveguiding within the sample. The experiments provide a direct visualization of extreme-ultraviolet guided modes, and demonstrate that multiple scattering is a generic feature in extruded nanoscale geometries. The observations are successfully reproduced in numerical and semi-analytical simulations.

Nanotip-based photoelectron microgun for ultrafast LEED

We present the design and fabrication of a micrometer-scale electron gun for the implementation of ultrafast low-energy electron diffraction from surfaces. A multi-step process involving photolithography and focused-ion-beam nanostructuring is used to assemble and electrically contact the photoelectron gun, which consists of a nanotip photocathode in a Schottky geometry and an einzel lens for beam collimation. We characterize the low-energy electron pulses by a transient electric field effect and achieve pulse durations of 1.3 ps at an electron energy of 80 eV. First diffraction images in a backscattering geometry (at 50 eV electron energy) are shown.

Polarization contrast of nanoscale waveguides in high harmonic imaging

The optical polarization response of a structured material is one of its most significant properties, carrying information about microscopic anisotropies as well as chiral features and spin orientations. Polarization analysis is therefore a key element of imaging and spectroscopy techniques throughout the entire spectrum. In the case of extreme ultraviolet (EUV) radiation, however, both the preparation and detection of well-defined polarization states remain challenging. As a result, polarization-sensitive EUV microscopy based on table-top sources has not yet been realized, despite its great potential, for example, in nanoscale magnetic imaging. Here, we demonstrate polarization contrast in coherent diffractive imaging using high harmonic radiation and investigate the polarization properties of nanoscale transmission waveguides. We quantify the achievable polarization extinction ratio for different waveguide geometries and wavelengths. Our results demonstrate the utility of slab waveguides for efficient EUV polarization control and illustrate the importance of considering polarization contrast in the imaging of nanoscale structures.