Tom T. A. Lummen

Simultaneous observation of the quantization and the interference pattern of a plasmonic near-field.

Surface plasmon polaritons can confine electromagnetic fields in subwavelength spaces and are of interest for photonics, optical data storage devices and biosensing applications. In analogy to photons, they exhibit wave–particle duality, whose different aspects have recently been observed in separate tailored experiments. Here we demonstrate the ability of ultrafast transmission electron microscopy to simultaneously image both the spatial interference and the quantization of such confined plasmonic fields. Our experiments are accomplished by spatiotemporally overlapping electron and light pulses on a single nanowire suspended on a graphene film. The resulting energy exchange between single electrons and the quanta of the photoinduced near-field is imaged synchronously with its spatial interference pattern. This methodology enables the control and visualization of plasmonic fields at the nanoscale, providing a promising tool for understanding the fundamental properties of confined electromagnetic fields and the development of advanced photonic circuits.

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 ∼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.

Emergent Low-Symmetry Phases and Large Property Enhancements in Ferroelectric KNbO3 Bulk Crystals

The design of new or enhanced functionality in materials is traditionally viewed as requiring the discovery of new chemical compositions through synthesis. Large property enhancements may however also be hidden within already well-known materials, when their structural symmetry is deviated from equilibrium through a small local strain or field. Here, the discovery of enhanced material properties associated with a new metastable phase of monoclinic symmetry within bulk KNbO3 is reported. This phase is found to coexist with the nominal orthorhombic phase at room temperature, and is both induced by and stabilized with local strains generated by a network of ferroelectric domain walls. While the local microstructural shear strain involved is only ≈0.017%, the concurrent symmetry reduction results in an optical second harmonic generation response that is over 550% higher at room temperature. Moreover, the meandering walls of the low-symmetry domains also exhibit enhanced electrical conductivity on the order of 1 S m-1 . This discovery reveals a potential new route to local engineering of significant property enhancements and conductivity through symmetry lowering in ferroelectric crystals.

Ultrafast imaging of plasmons in a transmission electron microscope

Miniaturized plasmonic and photonic integrated circuits are generally considered as the core of future generations of optoelectronic devices, due to their potential to bridge the size-compatibility gap between photonics and electronics. However, as the nanoscale is approached in increasingly small plasmonic and photonic systems, experimentally observing their behavior involves ever more stringent requirements in terms of both temporal and spatial resolution. This talk focuses on the use of time-resolved Photon-Induced Near-Field Electron Microscopy (PINEM) to study the excitation, propagation, (self-)interference and dynamics of surface plasmon polaritons (SPPs) in various plasmonic nanostructures with both nanometer and ultrafast resolution in a transmission electron microscope. Using this field-ofview technique, we directly show how photo-excited plasmonic interference patterns are controlled through the combination of excitation polarization and nanostructure geometry. Moreover, we capture the propagation of the photoinduced self-interfering plasmonic wave, clearly demonstrating the effects of axial confinement in nanostructured plasmonic thin film stacks.

Symmetry disquisition on theTiOXphase diagram(X=Br,Cl)

The sequence of phase transitions and the symmetry of, in particular, the low temperature incommensurate and spin-Peierls phases of the quasi-one-dimensional inorganic spin-Peierls system TiOX (X=Br and Cl) have been studied using inelastic light scattering experiments. The anomalous first-order character of the transition to the spin-Peierls phase is found to be a consequence of the different symmetries of the incommensurate and spin-Peierls (P2(1)/m) phases. The pressure dependence of the lowest transition temperature strongly suggests that magnetic interchain interactions play an important role in the formation of the spin-Peierls and the incommensurate phases. Finally, a comparison of Raman data on VOCl to the TiOX spectra shows that the high energy scattering previously observed has a phononic origin.