Tomáš Neuman

Control and near-field detection of surface plasmon interference patterns.

The tailoring of electromagnetic near-field properties is the central task in the field of nanophotonics. In addition to 2D optics for optical nanocircuits, confined and enhanced electric fields are utilized in detection and sensing, photovoltaics, spatially localized spectroscopy (nanoimaging), as well as in nanolithography and nanomanipulation. For practical purposes, it is necessary to develop easy-to-use methods for controlling the electromagnetic near-field distribution. By imaging optical near-fields using a scanning near-field optical microscope, we demonstrate that surface plasmon polaritons propagating from slits along the metal-dielectric interface form tunable interference patterns. We present a simple way how to control the resulting interference patterns both by variation of the angle between two slits and, for a fixed slit geometry, by a proper combination of laser beam polarization and inhomogeneous far-field illumination of the structure. Thus the modulation period of interference patterns has become adjustable and new variable patterns consisting of stripelike and dotlike motifs have been achieved, respectively.

Real-Space Mapping of the Chiral Near-Field Distributions in Spiral Antennas and Planar Metasurfaces

Chiral antennas and metasurfaces can be designed to react differently to left- and right-handed circularly polarized light, which enables novel optical properties such as giant optical activity and negative refraction. Here, we demonstrate that the underlying chiral near-field distributions can be directly mapped with scattering-type scanning near-field optical microscopy employing circularly polarized illumination. We apply our technique to visualize, for the first time, the circular-polarization selective nanofocusing of infrared light in Archimedean spiral antennas, and explain this chiral optical effect by directional launching of traveling waves in analogy to antenna theory. Moreover, we near-field image single-layer rosette and asymmetric dipole-monopole metasurfaces and find negligible and strong chiral optical near-field contrast, respectively. Our technique paves the way for near-field characterization of optical chirality in metal nanostructures, which will be essential for the future development of chiral antennas and metasurfaces and their applications.

Coupling of Molecular Emitters and Plasmonic Cavities beyond the Point-Dipole Approximation

As the size of a molecular emitter becomes comparable to the dimensions of a nearby optical resonator, the standard approach that considers the emitter to be a point-like dipole breaks down. By adoption of a quantum description of the electronic transitions of organic molecular emitters, coupled to a plasmonic electromagnetic field, we are able to accurately calculate the position-dependent coupling strength between a plasmon and an emitter. The spatial distribution of excitonic and photonic quantum states is found to be a key aspect in determining the dynamics of molecular emission in ultrasmall cavities both in the weak and strong coupling regimes. Moreover, we show that the extreme localization of plasmonic fields leads to the selection rule breaking of molecular excitations.

Surface-Enhanced Molecular Electron Energy Loss Spectroscopy

Electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM) is becoming an important technique in spatially resolved spectral characterization of optical and vibrational properties of matter at the nanoscale. EELS has played a significant role in understanding localized polaritonic excitations in nanoantennas and also allows for studying molecular excitations in nanoconfined samples. Here we theoretically describe the interaction of a localized electron beam with molecule-covered polaritonic nanoantennas, and propose the concept of surface-enhanced molecular EELS exploiting the electromagnetic coupling between the nanoantenna and the molecular sample. Particularly, we study plasmonic and infrared phononic antennas covered by molecular layers, exhibiting either an excitonic or vibrational response. We demonstrate that EEL spectra of these molecule-antenna coupled systems exhibit Fano-like or strong coupling features, similar to the ones observed in far-field optical and infrared spectroscopy. EELS offers the advantage to acquire spectral information with nanoscale spatial resolution, and importantly, to control the antenna-molecule coupling on demand. Considering ongoing instrumental developments, EELS in STEM shows the potential to become a powerful tool for fundamental studies of molecules that are naturally or intentionally located on nanostructures supporting localized plasmon or phonon polaritons. Surface-enhanced EELS might also enable STEM-EELS applications such as remote- and thus damage-free-sensing of the excitonic and vibrational response of molecules, quantum dots, or 2D materials.

Molecular optomechanical approach to surface-enhanced Raman scattering in plasmonic cavities

Recent advances on Surface Enhanced Raman Scattering (SERS) have led to a delicate control of the coupling between extremely-confined plasmonic resonances supported by metallic structures and the vibrational states of molecules. As a consequence, experiments have started to emerge that cannot be easily explained using standard models based on the classical enhancement of the plasmonic fields near smooth metallic systems[1,2].

Controlling molecular vibrations in resonant surface-enhanced Raman scattering

Plasmonic cavities are suitable platforms for studying the interaction of light and matter at the nanoscale. It has been demonstrated that plasmonic cavities are able to squeeze light into nanometer-sized volumes and thus open novel possibilities for studying the interaction of single molecules with light. For example, it has been recently shown that off-resonance Surface-Enhanced Raman Spectroscopy (SERS) can be described in the framework of cavity quantum electrodynamics (QED) and that molecular vibrations interacting with a plasmonic cavity mode represent a molecular optomechanical system [1-3].