Arthur Losquin

Unveiling Nanometer Scale Extinction and Scattering Phenomena through Combined Electron Energy Loss Spectroscopy and Cathodoluminescence Measurements

Plasmon modes of the exact same individual gold nanoprisms are investigated through combined nanometer-resolved electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) measurements. We show that CL only probes the radiative modes, in contrast to EELS, which additionally reveals dark modes. The combination of both techniques on the same particles thus provides complementary information and also demonstrates that although the radiative modes give rise to very similar spatial distributions when probed by EELS or CL, their resonant energies appear to be different. We trace this phenomenon back to plasmon dissipation, which affects in different ways the plasmon signatures probed by these techniques. Our experiments are in agreement with electromagnetic numerical simulations and can be further interpreted within the framework of a quasistatic analytical model. We therefore demonstrate that CL and EELS are closely related to optical scattering and extinction, respectively, with the addition of nanometer spatial resolution.

Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna

The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.

Direct subwavelength imaging and control of near-field localization in individual silver nanocubes

We demonstrate the control of near-field localization within individual silver nanocubes through photoemission electron microscopy combined with broadband, few-cycle laser pulses. We find that the near-field is concentrated at the corners of the cubes, and that it can be efficiently localized to different individual corners depending on the polarization of the incoming light. The experimental results are confirmed by finite-difference time-domain simulations, which also provide an intuitive picture of polarization dependent near-field localization in nanocubes.

Size and shape dependent few-cycle near-field dynamics of bowtie nanoantennas

Metal nanostructures can transfer electromagnetic energy from femtosecond laser pulses to the near-field down to spatial scales well below the optical diffraction limit. By combining few-femtosecond laser pulses with photoemission electron microscopy, we study the dynamics of the induced few-cycle near-field in individual bowtie nanoantennas. We investigate how the dynamics depend on antenna size and exact bowtie shape resulting from fabrication. Different dynamics are, as expected, measured for antennas of different sizes. However, we also detect comparable dynamics differences between individual antennas of similar size. With Finite-difference time-domain simulations we show that these dynamics differences between similarly sized antennas can be due to small lateral shape variations generally induced during the fabrication.

Spatial Control of Multiphoton Electron Excitations in InAs Nanowires by Varying Crystal Phase and Light Polarization

We demonstrate the control of multiphoton electron excitations in InAs nanowires (NWs) by altering the crystal structure and the light polarization. Using few-cycle, near-infrared laser pulses from an optical parametric chirped-pulse amplification system, we induce multiphoton electron excitations in InAs nanowires with controlled wurtzite (WZ) and zincblende (ZB) segments. With a photoemission electron microscope, we show that we can selectively induce multiphoton electron emission from WZ or ZB segments of the same wire by varying the light polarization. Developing ab initio GW calculations of first to third order multiphoton excitations and using finite-difference time-domain simulations, we explain the experimental findings: While the electric-field enhancement due to the semiconductor/vacuum interface has a similar effect for all NW segments, the second and third order multiphoton transitions in the band structure of WZ InAs are highly anisotropic in contrast to ZB InAs. As the crystal phase of NWs can be precisely and reliably tailored, our findings open up for new semiconductor optoelectronics with controllable nanoscale emission of electrons through vacuum or dielectric barriers.

Compact 200 kHz HHG source driven by a few-cycle OPCPA

We present a compact HHG source driven by a few-cycle, few μJ, 200 kHz OPCPA system. Efficient harmonics are generated from Neon, Argon and Krypton with conversion efficiency of 4.0×10⁻⁸, 1.2×10⁻⁶ and 4.1×10⁻⁶, respectively.

How Dark Are Radial Breathing Modes in Plasmonic Nanodisks

Due to a vanishing dipole moment, radial breathing modes in small flat plasmonic nanoparticles do not couple to light and have to be probed with a near-field source, as in electron energy loss spectroscopy (EELS). With increasing particle size, retardation gives rise to light coupling, enabling probing breathing modes optically or by cathodoluminescence (CL). Here, we investigate single silver nanodisks with diameters of 150–500 nm by EELS and CL in an electron microscope and quantify the EELS/CL ratio, which corresponds to the ratio of full to radiative damping of the breathing mode. For the investigated diameter range, we find the CL signal to increase by about 1 order of magnitude, in agreement with numerical simulations. Due to reciprocity, our findings corroborate former optical experiments and enable a quantitative understanding of the light coupling of dark plasmonic modes.

Unveiling Nanometric Plasmons Optical Properties With Advanced Electron Spectroscopy in the Scanning Transmission Electron Microscope

Since the pioneering work of Yamamoto and co-workers [1], the use of electron spectroscopy such as Cathodoluminescence (CL) and Electron Energy Loss Spectroscopy (EELS) in a Scanning (Transmission) Electron Microscope (STEM) has considerably helped improving our understanding of the optical properties of metallic nanoparticles. The resemblance of spectroscopic signals between electron and optical techniques leads to the intuition that both types of excitations (optical and electronic) give very similar information, an idea theoretically discussed quite early [2,3].

Spatiotemporal imaging of few‐cycle nanoplasmonic fields using photoemission electron microscopy

Surface plasmons are capable of concentrating light on both a nanometre spatial and femtosecond temporal scale, thus serving as a basis for nanotechnology at optical frequencies. However, the simultaneously small and fast nature of surface plasmons leads to new challenges for spatiotemporal characterization of the electric fields. An especially successful method for this purpose is photoemission electron microscopy (PEEM) in combination with ultrashort laser pulses. This method uses the high spatial resolution offered by electron microscopy together with the temporal resolution offered by femtosecond laser technology. By combining PEEM with state-of-the-art sources of ultrashort bursts of light, we have contributed to two pathways towards the ultimate goal: the full spatiotemporal reconstruction of the surface electric field at arbitrary nanostructures. The first approach is based on extending interferometric time-resolved PEEM (ITR-PEEM) [1] to the few light cycle regime by using two synchronized pulses from an ultra-broadband oscillator. Because the photon energy (1.2-2.0 eV) is well below the material work function, photoemission occurs through a multiphoton process. The measurement is performed by scanning the delay between two identical, sub-6 fs pulses and measuring the local photoemission intensity (Fig. 1a). We have applied this method to a variety of nanostructures, including rice-shaped silver particles, nanocubes, and gold bow-tie nanoantennas. As an example, results from the rice-shaped silver nanoparticles are shown in Fig. 1. We excited multipolar surface plasmons at grazing incidence, and imaged the photoelectrons emitted from the two ends of the nanoparticle (Fig. 1b). Upon scanning the delay between the two pulses, the interference fringes measured from the two ends of the nanoparticle are shifted with respect to each other (Fig. 1c). We show that these shifts correspond to locally different instantaneous frequencies of the near-field within the same nanoparticle, and that these differences occur due to a combination of retardation effects and the excitation of multiple surface plasmon modes [2]. The second approach is based on using high-order harmonic generation (HHG) to produce attosecond pulses in the extreme ultraviolet (XUV) region. Attosecond XUV pulses have been proposed to enable a direct spatiotemporal measurement of nanoplasmonic fields with a temporal resolution down to 100 as [3]. However, PEEM imaging using HHG light sources has turned out to be a major challenge due to numerous issues such as space charge effects, chromatic aberration, and poor image contrast [4-6]. To address these issues, we perform HHG using a new optical parametric chirped pulse amplification system delivering 7 fs pulses at 200 kHz repetition rate. We show how the XUV pulses generated by this system allow for PEEM imaging with both higher resolution and shorter acquisition times. For comparison, Fig. 2 shows PEEM images of silver nanowires on a gold substrate, imaged using high-order harmonics at 1 kHz repetition rate (Fig. 2a, acquisition time is 400 s) and at 200 kHz repetition rate (Fig. 2b, acquisition time is 30 s). The image quality is clearly improved (Fig. 2c). We also show how the higher repetition rate allows for PEEM imaging using only primary (“true”) photoelectrons, whereas previous studies have acquired images using secondary electrons [4-6]. Keywords: photoemission electron microscopy; ultrafast plasmonics