Andrea Konečná

Bio: Andrea Konečná is an academic researcher from ICFO – The Institute of Photonic Sciences. The author has contributed to research in topics: Plasmon & Electron. The author has an hindex of 10, co-authored 38 publications receiving 316 citations. Previous affiliations of Andrea Konečná include Donostia International Physics Center & University of the Basque Country.

Probing low-energy hyperbolic polaritons in van der Waals crystals with an electron microscope

Abstract: Van der Waals materials exhibit intriguing structural, electronic, and photonic properties. Electron energy loss spectroscopy within scanning transmission electron microscopy allows for nanoscale mapping of such properties. However, its detection is typically limited to energy losses in the eV range—too large for probing low-energy excitations such as phonons or mid-infrared plasmons. Here, we adapt a conventional instrument to probe energy loss down to 100 meV, and map phononic states in hexagonal boron nitride, a representative van der Waals material. The boron nitride spectra depend on the flake thickness and on the distance of the electron beam to the flake edges. To explain these observations, we developed a classical response theory that describes the interaction of fast electrons with (anisotropic) van der Waals slabs, revealing that the electron energy loss is dominated by excitation of hyperbolic phonon polaritons, and not of bulk phonons as often reported. Thus, our work is of fundamental importance for interpreting future low-energy loss spectra of van der Waals materials. Here the authors adapt a STEM-EELS system to probe energy loss down to 100 meV, and apply it to map phononic states in hexagonal boron nitride, revealing that the electron loss is dominated by hyperbolic phonon polaritons.

Vibrational Spectroscopy of Water with High Spatial Resolution

Abstract: The ability to examine the vibrational spectra of liquids with nanometer spatial resolution will greatly expand the potential to study liquids and liquid interfaces. In fact, the fundamental properties of water, including complexities in its phase diagram, electrochemistry, and bonding due to nanoscale confinement are current research topics. For any liquid, direct investigation of ordered liquid structures, interfacial double layers, and adsorbed species at liquid-solid interfaces are of interest. Here, a novel way of characterizing the vibrational properties of liquid water with high spatial resolution using transmission electron microscopy is reported. By encapsulating water between two sheets of boron nitride, the ability to capture vibrational spectra to quantify the structure of the liquid, its interaction with the liquid-cell surfaces, and the ability to identify isotopes including H2 O and D2 O using electron energy-loss spectroscopy is demonstrated. The electron microscope used here, equipped with a high-energy-resolution monochromator, is able to record vibrational spectra of liquids and molecules and is sensitive to surface and bulk morphological properties both at the nano- and micrometer scales. These results represent an important milestone for liquid and isotope-labeled materials characterization with high spatial resolution, combining nanoscale imaging with vibrational spectroscopy.

Electron Beam Aberration Correction Using Optical Near Fields.

Abstract: The interaction between free electrons and optical near fields is attracting increasing attention as a way to manipulate the electron wave function in space, time, and energy. Relying on currently attainable experimental capabilities, we design optical near-field plates to imprint a lateral phase on the electron wave function that can largely correct spherical aberration without the involvement of electric or magnetic lenses in the electron optics, and further generate on-demand lateral focal spot profiles. Our work introduces a disruptive and powerful approach toward aberration correction based on light-electron interactions that could lead to compact and versatile time-resolved free-electron microscopy and spectroscopy.

Surface-Enhanced Molecular Electron Energy Loss Spectroscopy.

Abstract: 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.

Cathodoluminescence Phase Extraction of the Coupling between Nanoparticles and Surface Plasmon Polaritons

Abstract: Nanoscale gaps between metals can strongly confine electromagnetic fields that enable efficient electromagnetic energy conversion and coupling to nanophotonic structures. In particular, the gap formed by depositing a metallic particle on a metallic substrate produces coupling of localized particle plasmons to propagating surface plasmon polaritons (SPPs). Understanding and controlling the phase of such coupling is essential for the design of devices relying on nanoparticles coupled through SPPs. Here we demonstrate the experimental visualization of the phase associated with the plasmonic field of metallic particle-surface composites through nanoscopically and spectroscopically resolved cathodoluminescence using a scanning transmission electron microscope. Specifically, we study the interference between the substrate transition radiation and the field resulting from out-coupling of SPP excitation, therefore giving rise to angle-, polarization-, and energy-dependent photon emission fringe patterns from which we extract phase information. Our methods should be readily applicable to more complex nanostructures, thus providing direct experimental insight into nanoplasmonic near-fields with potential applications in improving plasmon-based devices.

I and i

Abstract: There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality. Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

Principles Of Optics Electromagnetic Theory Of Propagation Interference And Diffraction Of Light

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Observation of Single Colloidal Platinum Nanocrystal Growth Trajectories

Abstract: It is conventionally assumed that the growth of monodisperse colloidal nanocrystals requires a temporally discrete nucleation followed by monomer attachment onto the existing nuclei. However, recent studies have reported violations of this classical growth model, and have suggested that inter-particle interactions are also involved during the growth. Mechanisms of nanocrystal growth still remain controversial. Using in situ transmission electron microscopy, we show that platinum nanocrystals can grow either by monomer attachment from solution onto the existing particles or by coalescence between the particles. Surprisingly, an initially broad size distribution of the nanocrystals can spontaneously narrow. We suggest that nanocrystals take different pathways of growth based on their size- and morphology-dependent internal energies. These observations are expected to be highly relevant for other nanocrystal systems.

Mapping surface plasmons on a single metallic nanoparticle

Abstract: Understanding how light interacts with matter at the nanometre scale is a fundamental issue in optoelectronics and nanophotonics. In particular, many applications (such as bio-sensing, cancer therapy and all-optical signal processing) rely on surface-bound optical excitations in metallic nanoparticles. However, so far no experimental technique has been capable of imaging localized optical excitations with sufficient resolution to reveal their dramatic spatial variation over one single nanoparticle. Here, we present a novel method applied on silver nanotriangles, achieving such resolution by recording maps of plasmons in the near-infrared/visible/ultraviolet domain using electron beams instead of photons. This method relies on the detection of plasmons as resonance peaks in the energy-loss spectra of subnanometre electron beams rastered on nanoparticles of well-defined geometrical parameters. This represents a significant improvement in the spatial resolution with which plasmonic modes can be imaged, and provides a powerful tool in the development of nanometre-level optics.