Imaging and controlling plasmonic interference fields at buried interfaces

Capturing and controlling plasmons at buried interfaces with nanometre and femtosecond resolution has yet to be achieved and is critical for next generation plasmonic devices. Here we use light to excite plasmonic interference patterns at a buried metal-dielectric interface in a nanostructured thin film. Plasmons are launched from a photoexcited array of nanocavities and their propagation is followed via photon-induced near-field electron microscopy (PINEM). The resulting movie directly captures the plasmon dynamics, allowing quantification of their group velocity at similar to 0.3 times the speed of light, consistent with our theoretical predictions. Furthermore, we show that the light polarization and nanocavity design can be tailored to shape transient plasmonic gratings at the nanoscale. This work, demonstrating dynamical imaging with PINEM, paves the way for the femtosecond and nanometre visualization and control of plasmonic fields in advanced heterostructures based on novel two-dimensional materials such as graphene, MoS2, and ultrathin metal films.

Near-field imaging

Libo Yu

Bloch surface waves (BSWs) are surface electromagnetic waves excited at the interface between a truncated periodic dielectric multilayer and a surrounding medium. This particular solution to the Maxwell equations in stratified media has been known since the late 1970s. However, few studies have been conducted till now on the manipulation and control of BSW propagation over 2D surfaces of photonic structures. There are several advantages provided by BSW propagation on almost flat surfaces. Due to the use of dielectric materials, losses are very low, thus allowing the propagation of BSWs over long distances. Another advantage in using BSWs is the possibility of operating within a broad range of wavelengths by properly designing a suitable multilayered structure. Furthermore, since the maximum intensity associated with BSWs can be tuned on the surface, a strong field intensity increased by several orders of magnitude can be achieved and can thereby enhance the field close to the structure's surface. This tunable localized field confinement is particularly attractive in fluorescence biosensing. In the following, we will use an exemplary BSW-sustaining multilayer as a general platform suitable for manipulating and controlling BSW propagation on its surface in the spectral range of telecom wavelengths. Several 2D optical photonic devices can be implemented starting from an ultra-thin (~ λ /15) polymer layer spun on the multilayer, which can be subsequently shaped as desired. The presence of the polymer modifies the local effective refractive index, enabling a direct manipulation of the BSWs. We experimentally and theoretically demonstrate that BSWs can be diffracted, focused, coupled and made resonating by locally shaping the geometries of 2D photonic devices—such as lenses, prisms, gratings, bended waveguides and waveguide couplers—on the multilayer. One of the main advantages is that these 2D photonic devices can have arbitrary shapes, which are difficult to obtain in 3D. The strong point of the platform concept is that a thin-film multilayer enables standard-wafer-scale production. The top surface can be modified to customize a 2D micro-system by, e.g., e-beam writing, optical lithography, stamping or other replication techniques. Since a BSW can be considered as a 2D wave and it is bounded at the surface of the multilayer, near-field imaging is one of the preferred tools to directly monitor and characterize the near field produced on the structured multilayered surface mentioned above. A multi-heterodyne scanning near-field optical microscope (MH-SNOM) developed in our lab (EPFL-OPT) makes near-field characterization possible. The operation wavelength is in the near infrared range (1460 nm–1580 nm). A polarization-retrieval method is developed in this thesis to measure and characterize the near-field polarization response for arbitrary polarization- sensitive photonic nano-devices, such as photonic crystal microcavities, waveguides, thin films, nanoparticles, spiral gratings and other near-field polarization-sensitive imaging applications. Polarization retrieval is easily accessible in far-field microscopy, but is challenging for the near field. This is because when a SNOM probe interacts with the near field and scatters the signal to the far field, the near-field polarization may be considerably altered. In this thesis, the developed method uses an isotropic region in the vicinity of the nanostructure as a calibration area, whose known polarization properties provide a global criterion to calibrate and quantify the polarization distortion induced by the detection system. It is then applied on the field measured above the structure of interest to compensate and reconstruct its complex field response. We experimentally show the effectiveness of the method on a silicon form- birefringent grating (FBG) with significant polarization diversity. Three spatial dimensional near-field measurements are in agreement with theoretical predictions obtained with rigorous coupled-wave analysis (RCWA). Pseudo-far- field (~10λ away from the surface) measurements are performed to obtain the effective refractive index of the FBG, emphasizing the validity of the proposed method. This reconstruction algorithm makes the MH-SNOM a powerful tool to analyze concurrently the polarization-dependent near-field optical response of any nanostructures with subwavelength resolution as long as a calibration area is available in close proximity.

EPFL2013

Fast and ultrafast electron microscopies for skyrmions and plasmonics

Gabriele Berruto

In recent years, topology gained a central role in physics. We learnt that energetics could be often explained better by classes of objects defined by having qualitative differences. In today's jargon, we say they are topologically distinct. The process of creation and annihilation of physical objects with topological charge has peculiar aspects, because it cannot proceed by continuous deformations. The consequent protection of these physical states against internal and external perturbations can therefore be striking. In condensed matter, topologically-protected states are found in electronic systems in solids, spin textures, and particle or quasiparticle wave functions. Because of their general reluctance to change topological state,methods to manipulate their topological charge should be thoroughly designed. In this dissertation, I illustrate dynamical manipulation of a topological charge in two distinct -yet connected- research areas: nanoscopic spin textures and free electrons. In both cases, the manipulation is performed via the interaction of ultrashort light packets with the system under investigation. In the first, topologically nontrivial spin vortices, called skyrmions, are injected and controlled by the laser pulses. In FeGe, Bloch-type skyrmions are investigated via static, in-situ, and time-resolved Lorentz electronmicroscopy. Spin supercooling has been found responsible for the creation and stabilization of skyrmions in large regions of the phase diagram, controlling the amount of topological charge in the material. The cooling rate ensuing from the excitation of thematerial with strong laser pulses can reach tremendous values. This work enabled an estimate of the speed limit for laser-induced writing and erasing of such skyrmionic states. In the second case, circularly-polarized light is used to convert an electron plane wave into an electron vortex with nonzero topological charge. A chiral plasmon photoinduced at the edges of a nanohole in a metal transfers the vortex phase structure to the electron beam via stimulated plasmon absorption and emission. In a wider picture, the precise tailoring of the free electron wave function can be obtained by electron-photon inelastic scattering in proximity of a physical object, as extensively discussed in this thesis. The new awareness of our tools to control matter waves led to the implementation of an innovative type of time-domain holography, which can be used to image nanoscopic, propagating electromagnetic fields. Besides the single results exemplified in the different chapters, such as the topological-charge manipulation studies, this thesis contributes to the refinement of time-resolved microscopy with ultrafast electrons for the investigation of magnetic, electronic, and structural degrees of freedom. Ideas for further original experiments that could push the discussed physics to new boundaries are debated throughout the chapters.

EPFL2019

Peculiarities of second harmonic generation with chirped femtosecond pulses at high conversion efficiency

Pierre-Marc Jean Marie Dansette

Frequency doubling of an infrared laser radiation in non-linear optical crystals is a widely used technique to obtain light in the visible range. The second harmonic generation process is influenced by several well-known parameters. In this article we study the effect of group delay dispersion on the second harmonic generation process for femtosecond pulses. We show, both through simulation and experiments, that for certain parameters even a small amount of chirp can have a detrimental effect on the conversion efficiency as well as the second harmonic beam quality. We also check the effect of higher order dispersion. By properly accounting for those effects the crystal length and focusing conditions can be optimized to reach high conversion efficiency, while maintaining low sensitivity to chirp variations and good beam quality.