Integrated photonics enables continuous-beam electron phase modulation

Integrated photonics facilitates extensive control over fundamental light-matter interactions in manifold quantum systems including atoms(1), trapped ions(2,3), quantum dots(4) and defect centres(5). Ultrafast electron microscopy has recently made free-electron beams the subject of laser-based quantum manipulation and characterization(6-11), enabling the observation of free-electron quantum walks(12-14), attosecond electron pulses(10,15-17) and holographic electromagnetic imaging(18). Chip-based photonics(19,20) promises unique applications in nanoscale quantum control and sensing but remains to be realized in electron microscopy. Here we merge integrated photonics with electron microscopy, demonstrating coherent phase modulation of a continuous electron beam using a silicon nitride microresonator. The high-finesse (Q(0) approximate to 10(6)) cavity enhancement and a waveguide designed for phase matching lead to efficient electron-light scattering at extremely low, continuous-wave optical powers. Specifically, we fully deplete the initial electron state at a cavity-coupled power of only 5.35 microwatts and generate >500 electron energy sidebands for several milliwatts. Moreover, we probe unidirectional intracavity fields with microelectronvolt resolution in electron-energy-gain spectroscopy(21). The fibre-coupled photonic structures feature single-optical-mode electron-light interaction with full control over the input and output light. This approach establishes a versatile and highly efficient framework for enhanced electron beam control in the context of laser phase plates(22), beam modulators and continuous-wave attosecond pulse trains(23), resonantly enhanced spectroscopy(24-26) and dielectric laser acceleration(19,20,27). Our work introduces a universal platform for exploring free-electron quantum optics(28-31), with potential future developments in strong coupling, local quantum probing and electron-photon entanglement.

Optically active quantum dots in bottom-up nanowires

Yannik Fontana

This thesis is dedicated to the discovery and progressive study of quantum emitters embedded in the shell of coaxial gallium arsenide/ aluminum gallium arsenide nanowires. The bottom-up core/shell nanowires were grown in a molecular beam epitaxy machine. During the shell growth, diffusion-driven phenomena lead to segregation effects. Gallium-rich regions are formed at the nanoscopic scale. The observation has been made that the reduced dimensionality of these regions provides true tridimensional confinement for the carriers. The recombination spectra of the electrons with the holes in what was coined shell quantum dots (shell-QDs) thus appear as sets of narrow, intense peaks. The formation of shell quantum dots is taking place on a large range of growth temperatures and nominal alloy fractions, giving freedom to engineer the growth process. The shell thickness plays an important role in the quantum dot density and total ensemble spectrum. In addition, the adjunction of an aluminum arsenide predeposition layer increasing the local curvature has been seen to foster the quantum dots formation. Single emitter spectroscopy reveals the few-particles electronic structure of quantum dots, with systematic signatures for the different degrees of occupation of the quantum dot. The shape anisotropy of the quantum dots leads to observable spin-spin interactions, which lift the degeneracy of the exciton level (one hole and one electron). Generally undesirable, this effect allows here to find that the orientation of the quantum dots in the nanowire is not hard-wired to the growth direction or to the nanowire long axis. This observation is confirmed by magneto-photoluminescence experiments. The energetic splitting and shift of the spin sublevels when an external magnetic field is applied also confirms the small size of the quantum dots. It is found that for GaAs in the strong confinement regime, the Landé coefficients of the electron and hole take opposite signs and are dependent on the angle at which the field is applied. These effects allow to tune the exciton composite Landé coefficient and could be used to reduce the splitting between the exciton spin sublevels or create optically degenerate coupled systems. Finally, the sub-nanosecond dynamics happening in the quantum dots are probed with time-correlated photon counting. It is shown that the carriers in the shell are quickly captured by the quantum dots. In addition, it is proposed that the electron population is reduced due to diffusion-assisted mechanisms or through electron-donor recombination.

EPFL2015

Nanoparticle sensitisation of solid-state nanocrystalline solar cell

Robert Plass

Over the past fifteen years dye-sensitised nanocrystalline solar cells have been the subject of intense research and development efforts. These systems provide a technically and economically credible alternative to classical p-n junction solar cells, reaching over 10 % certified efficiency under standard solar illumination conditions (AM 1.5, 1000 W/m2). Recently, the liquid electrolyte, commonly used in these dye-sensitised solar cells, could successfully be replaced by a novel solid hole-conducting material (spiro-OMeTAD). The absence of volatile solvents and corrosive components like iodine presents a clear advantage of these solid-state devices over their photoelectrochemical counterparts. Yet, their maximum overall efficiency of about 3 % clearly lacks behind the performance features of classical dye-sensitized solar cells. The objective of this work is the replacement of the usually used sensitiser (transition metal complexes and organic dyes) by quantum-dots. It was motivated by the possibility to achieve panchromatic light absorption due to the size-dependent properties of the quantum-dots. Some studies have been published using quantum-dots of inorganic low-bandgap semiconductors as sensitisers for mesoporous wide bandgap semiconductor electrodes in conjunction with liquid electrolytes. These systems often suffer from corrosion and photo-corrosion mainly due to the aggressive nature of the electrolyte employed. Solid-state organic-inorganic heterojunctions might provide the desired environment for quantum-dot sensitisation, as the environment is much less aggressive. A large variety of inorganic quantum-dot materials like PbS, CdS, PbSe and CdSe were scrutinized for their use as sensitisers. All particles were synthesised in situ on the TiO2 surface using two different techniques: dip-coating and chemical bath deposition. Lead sulphide was the most investigated due to its superior photovoltaic characteristics. High Resolution Transmission Electron Microscopy (HRTEM) of PbS sensitised TiO2 electrodes fabricated via dip-coating clearly showed the distinct particles on the surface of the semiconductor. The electron transfer dynamics following optical excitation of quantum-dot sensitized TiO2/spiro-OMeTAD heterojunctions were thoroughly studied. Fluorescence spectroscopy was used to prove the possible electron injection from the PbS into the TiO2. Nanosecond laser spectroscopy was applied to monitor the interfacial recombination of the injected electron and the oxidised hole-conductor. Femtosecond laser spectroscopy allowed measuring the ultra-fast kinetics in the system, including electron trapping, exciton recombination and PbS regeneration. An overall efficiency of 0.5 % at 0.1 sun (AM 1.5) has been reached with such systems. Chemical bath deposition (CBD) of PbS leads to the formation of a layer rather than distinct particles on the TiO2. Solar cells fabricated via CBD exhibited open-circuit voltages which were generally 100 mV higher then those of comparable devices made via dip-coating. The PbS layer acts as blocking layer, hindering the contact between TiO2 and the hole-conductor. This technique allowed achieving devices highly linear with respect to the illumination power. Different strategies were pursued to impede interfacial recombination, among which the introduction of self-assembled monolayers at the interface between the organic and inorganic phases was proven to be the most efficient. Nanosecond laser spectroscopy showed a strong decrease of the interfacial recombination kinetic rates in the presence of hexadecylmalonic acid or decylphosphonic acid monolayers. Short-circuit currents could be raised by a factor two to four using such type of molecules. The overall efficiency of the device could be strongly increased, reaching 1 % at 0.1 Sun (AM 1.5). CBD was also used to deposit PbSe and CdSe layers at the surface of TiO2. Fluorescence spectroscopy was used to probe electron injection from CdSe quantum dots to TiO2. Generally it was observed that metal sulfides were more efficient in sensitizing TiO2/OMeTAD heterojunctions then the respective selenides.

EPFL2004

Scanning near-field infrared microscopy and spectromicroscopy applied to nano-systems and cells

Dusan Vobornik

This thesis further explores the possibilities of scanning near-field optical microscopy (SNOM) in both materials and life sciences. Two experimental SNOM setups were developed: one designed for infrared spectroscopy applications and the other for the imaging of fluorescently labeled samples. The results of the experiments that were conducted with both setups are presented and analyzed in this thesis. Diffraction limits the resolution of lens-based microscopes to a value close to that of the wavelength of the light that is used to illuminate the samples. SNOM instruments overcome this limit by probing the near-field light — the light that remains within close vicinity of the sample and decays exponentially away from it. The SNOM concept and instrumental design are described. A comparison of SNOM with other novel microscopies (electron, atomic force, and scanning tunneling microscopies) outlines the main advantages of SNOM — the sole optical microscopy technique with a nanometer resolution. Aperture-based infrared SNOM (IR-SNOM), performed in the spectroscopic mode using the Vanderbilt University free electron laser, recently started delivering spatially resolved information on the distribution of chemical species and on other laterally fluctuating properties. The IR-SNOM combines the IR spectroscopy's chemical specificity and the SNOM's high optical and topographical resolutions. The IR-SNOM experimental setup is described in detail and results from the study of cells, boron nitride and lithium fluoride thin films are presented and analyzed. They demonstrate the great potential of this new technique. An overview of the development of IR-SNOM, as well as a consideration of its future possibilities are presented. The newly built SNOM instrument at EPFL was used for experiments that are complementary to the aforementioned IR-SNOM experiments. Specifically, the new SNOM enabled the study of fluorescently marked samples. Images of fluorescently labeled cells and carbon nanotubes are presented and analyzed. The results further demonstrate the exciting possibilities of SNOM.

EPFL2005