Electron microscopy methods for space-, energy-, and time-resolved plasmonics

Nanoscale plasmonic systems combine the advantages of optical frequencies with those of small spatial scales, circumventing the limitations of conventional photonic systems by exploiting the strong field confinement of surface plasmons. As a result of this miniaturization to the nanoscale, electron microscopy techniques are the natural investigative methods of choice. Recent years have seen the development of a number of electron microscopy techniques that combine the use of electrons and photons to enable unprecedented views of surface plasmons in terms of combined spatial, energy, and time resolution. This review aims to provide a comparative survey of these different approaches from an experimental viewpoint by outlining their respective experimental domains of suitability and highlighting their complementary strengths and limitations as applied to plasmonics in particular

Seeing And Measuring In Colours: Electron Microscopy And Spectroscopies Applied To Nano-optics

Over the past ten years, Scanning Transmission Electron Microscopes (STEM) fitted with Electron Energy Loss Spectroscopy (EELS) and/or Cathodoluminescence (CL) spectroscopy have demonstrated to be essential tools for probing the optical properties of nano-objects at sub-wavelength scales. Thanks to the possibility of measuring them at a nanometer scale in parallel to the determination of the structure and morphology of the object of interest, new challenging experimental and theoretical horizons have been unveiled. As regards optical properties of metallic nanoparticles, surface plasmons have been mapped at a scale unimaginable only a few years ago, while the relationship between the energy levels and the size of semiconducting nanostructures a few atomic layers thick could directly be measured. 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Experimental evidence of nanometer-scale confinement of plasmonic eigenmodes responsible for hot spots in random metallic films

International audienceWe report on the identification and nanometer scale characterization over a large energy range of random, disorder-driven, surface plasmons in silver semicontinuous films embedded in silicon nitride. By performing spatially resolved electron energy loss spectroscopy experiments, we experimentally demonstrate that these plasmons eigenmodes arise when the films become fractal, leading to the emergence of strong electrical fields (" hot spots ") localized over few nanometers. We show that disorder-driven surface plasmons strongly depart from those usually found in nanoparticles, being strongly confined and randomly and densely distributed in space and energy. Beyond that, we show that they have no obvious relation with the local morphology of the films, in stark contrast with surface plasmon eigenmodes of nanoparticles

Stimulated electron energy loss and gain in an electron microscope without a pulsed electron gun

FAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOWe report on a novel way of performing stimulated electron energy-loss and energy-gain spectroscopy (sEELS/sEEGS) experiments that does not require a pulsed gun. In this scheme, a regular scanning transmission electron microscope (STEM) equipped with a conventional continuous electron gun is fitted with a modified EELS detector and a light injector in the object chamber. The modification of the EELS detector allows one to expose the EELS camera during tunable time intervals that can be synchronized with nanosecond laser pulses hitting the sample, therefore allowing us to collect only those electrons that have interacted with the sample under light irradiation. Using similar to 5 ns laser pulses of similar to 2 eV photon energy on various plasmonic silver samples, we obtain evidence of sEELS/sEEGS through the emergence of up to two loss and gain peaks in the spectra at +/- 2 and +/- 4 eV. Because this approach does not involve any modification of the gun, our method retains the original performances of the microscope in terms of energy resolution and spectral imaging with and without light injection. Compared to pulsed-gun techniques, our method is mainly limited to a perturbative regime (typically no more that one gain event per incident electron), which allows us to observe resonant effects, in particular when the plasmon energy of a silver nanostructure matches the laser photon energy. In this situation, EELS and EEGS signals are enhanced in proportion to n + 1 and n, respectively, where n is the average plasmon population due to the external illumination. The n term is associated with stimulated loss and gain processes, and the term of 1 corresponds to conventional (spontaneous) loss. The EELS part of the spectrum is therefore an incoherent superposition of spontaneous and stimulated EEL events. This is confirmed by a proper quantum-mechanical description of the electron/light/plasmon system incorporating light-plasmon and plasmon-electron interactions, as well as inelastic plasmon decay.203SI4451FAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOFAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULO2014/23399-92017/00259-5MK wants to thank F. Houdellier and A. Arbouet for fruitful discussions. This work has received support from the National Agency for Research under the program of future investment TEMPOS-CHROMATEM with the Reference No. ANR-10-EQPX-50 and FEMTOTEM ANR-14-CE26-0013. FJGA acknowledges support from ERC (Advanced Grant 789104-eNANO) and the Spanish MINECO (MAT2017-88492-R and SEV2015-0522). LFZ and YA acknowledges support from FAPESP (grants 2014/23399-9 and 2017/00259-5)

Few-cycle high-repetition rate OPCPA for multiphoton PEEM towards atto-PEEM

We present a few-cycle high-repetition rate optical parametric amplifier for multiphoton PEEM experiments on semiconductor nanowires. This parametric amplifier is also used for the generation of high-order harmonics at 200kHz for future atto-PEEM experiments

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