Nonlinear Light Generation in Localized Fields Using Gases and Tailored Solids

n Chap. 18, we demonstrated polarization-sensitive imaging at extreme-ultraviolet (EUV) wavelengths using a gas-phase high-harmonic generation (HHG) source. In a related project, we have investigated new types of gas-phase and solid-state EUV light sources employing field localization in plasmonic nanostructures and structured targets. Whereas our first results indicate that strong field confinement leads to exceedingly inefficient high-harmonic generation in gas-phase targets, for solid-state media efficient high-harmonic generation is possible in localized fields. The latter has great ramifications for new types of high-harmonic generation experiments and technological developments. Therefore, our research efforts aim in two directions: firstly, the development of new types of solid-state sources for high-harmonic generation and, secondly, the application of locally generated solid-state high-harmonic signals for spectroscopy and imaging

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

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

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

Controlling free electrons with optical whispering-gallery modes

Free-electron beams are versatile probes of microscopic structure and composition1,2, and have revolutionized atomic-scale imaging in several fields, from solid-state physics to structural biology3. Over the past decade, the manipulation and interaction of electrons with optical fields have enabled considerable progress in imaging methods4, near-field electron acceleration5,6, and four-dimensional microscopy techniques with high temporal and spatial resolution7. However, electron beams typically couple only weakly to optical excitations, and emerging applications in electron control and sensing8,9,10,11 require large enhancements using tailored fields and interactions. Here we couple a free-electron beam to a travelling-wave resonant cavity mode. The enhanced interaction with the optical whispering-gallery modes of dielectric microresonators induces a strong phase modulation on co-propagating electrons, which leads to a spectral broadening of 700 electronvolts, corresponding to the absorption and emission of hundreds of photons. By mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the lifetime of the the microresonator following a femtosecond excitation and observe the spectral response of the cavity. The natural matching of free electrons to these quintessential optical modes could enable the application of integrated photonics technology in electron microscopy, with broad implications for attosecond structuring, probing quantum emitters and possible electron–light entanglement

Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields

The interplay between free electrons, light, and matter offers unique prospects for space, time, and energy resolved optical material characterization, structured light generation, and quantum information processing. Here, we study the nanoscale features of spontaneous and stimulated electron–photon interactions mediated by localized surface plasmon resonances at the tips of a gold nanostar using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Supported by numerical electromagnetic boundary-element method (BEM) calculations, we show that the different coupling mechanisms probed by EELS, CL, and PINEM feature the same spatial dependence on the electric field distribution of the tip modes. However, the electron–photon interaction strength is found to vary with the incident electron velocity, as determined by the spatial Fourier transform of the electric near-field component parallel to the electron trajectory. For the tightly confined plasmonic tip resonances, our calculations suggest an optimum coupling velocity at electron energies as low as a few keV. Our results are discussed in the context of more complex geometries supporting multiple modes with spatial and spectral overlap. We provide fundamental insights into spontaneous and stimulated electron-light-matter interactions with key implications for research on (quantum) coherent optical phenomena at the nanoscale

Nanoscale magnetic imaging using circularly polarized 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