Spatio-temporal shaping of a free-electron wave function via coherent light-electron interaction

The past decade has witnessed a quantum revolution in the field of computation, communication and materials investigation. A similar revolution is also occurring for free-electron based techniques, where the classical treatment of a free electron as a point particle is being surpassed toward a deeper exploitation of its quantum nature. Adopting familiar concepts from quantum optics, several groups have demonstrated temporal and spatial shaping of a free-electron wave function, developing theoretical descriptions of light-modulated states, as well as predicting and confirming fascinating phenomena as attosecond self-compression and orbital angular momentum transfer from light to electrons. In this review, we revisit the milestones of this development and the several methods adopted for imprinting a time-varying phase modulation on an electron wave function using properly synthesized ultrafast light fields, making the electron an exquisitely selective probe of out-of-equilibrium phenomena in individual atomic/nanoscale systems. We discuss both longitudinal and transverse phase manipulation of free-electrons, where coherent quantized exchanges of energy, linear momentum and orbital angular momentum mediating the electron-light coupling are key in determining their spatio-temporal redistribution. Spatio-temporal phase shaping of matter waves provides new routes toward image-resolution enhancement, selective probing, dynamic control of materials, new quantum information methods, and exploration of electronic motions and nuclear phenomena. Emerging as a new field, electron wave function shaping allows adopting familiar quantum optics concepts in composite-particle experiments and paves the way for atomic, ionic and nuclear wave function engineering with perspective applications in atomic interferometry and direct control of nuclear processes.

Four-dimensional electron microscopy: Ultrafast imaging, diffraction and spectroscopy in materials science and biology

Giovanni Maria Vanacore

Understanding the ultrafast evolution of atomic and electronic rearrangements under nonequilibrium conditions in organic, inorganic and biological materials plays a fundamental role in deciphering the mechanism governing chemical and biological functions. With direct visualization, the technological development of future innovative devices on the nanoscale becomes feasible. Although an enormous effort has been devoted to the comprehension and improvement of these materials and devices, the capability of investigating their dynamic behavior is hindered by the difficulty of simultaneously studying their evolution in space and time at the appropriate scales. The traditional characterization techniques and the steady-state theoretical models are both not adequate for describing their nonequilibrium behavior. Instead, a novel approach for visualization of matter with high temporal and spatial resolutions, together with energy and momentum selection, is indispensable to fully exploit their potential. Four-dimensional electron microscopy (4D-EM) has been developed with the capability of performing time-resolved imaging, diffraction and electron-spectroscopy. The acquired and sufficient spatial, temporal, energy and momentum resolution, provide the real-time access to the dynamic behavior of surfaces, interfaces and nanosystems. In this review, after outlining the 4D-EM approach, which enables sub-nanometer spatial resolution and temporal speed of 10 orders of magnitude faster than previously possible, we address several recent applications in materials science and biology, highlighting for each case the challenges that had to be overcome, the main scientific contributions, and future trends in the field. The highly inter- and multi-disciplinary approach presented here will pave the way for an unprecedented insight into the nonequilibrium phenomena of advanced materials, and should play a decisive role in the rational design and engineering of future applications. (C) 2016 Elsevier Ltd. All rights reserved.

Elsevier Sci Ltd2016

Realization and study of InAs/GaAs quantum dot superluminescent diodes emitting at 1.3µm

Marco Rossetti

A quantum dot is a semiconductor nanostructure that confines the motion of conduction band electrons and valence band holes in all three spatial directions, thus creating fully discrete energy levels. The confinement in the InAs/GaAs material system is generated by the bandgap difference for the two materials (∼ 0.4 eV for InAs, and ∼ 1.4 eV for GaAs) which provides a minimum of potential energy for both electrons and holes inside the InAs nanoparticle. The appearance of new nanoscale effects modifies the electro-optical properties of such a system which makes possible the improvement of existing device performance or even fascinating novel device applications. For the creation of coherent structures with very high purity and high density, as it is required for application in light emitting devices, self-assembling is a very important pathway. The quantum dot creation mostly relies on the relaxation of the strain accumulated during the growth of lattice mismatched materials, which happens in a non-equlibrium condition. This results in a statistical distribution of all the parameters characterizing the InAs nanocrystals as size, composition and strain, whose direct manifestation is the inhomogeneously broadened light emission deriving from quantum dot ensembles. At the dawning of the quantum dot development the broadening was considered as a limiting factor for application in semiconductor lasers. Today, it is considered favorably for all the applications where a broad gain spectrum is required as optical amplifiers, monolithic and external-cavity tunable lasers, and superluminescent diodes. The objective of this thesis is the application of InAs/GaAs self-assembled quantum dots to the active region of high power and broad-band superluminescent diodes emitting in the 1.3 μm wavelength region. Superluminescent diodes are edge-emitting semiconductor light sources based on the amplification of spontaneous emission along a waveguide where optical gain is achieved through current injection. They combine the high power and brightness of laser diodes with the low coherence of LEDs. The latter is a fundamental feature for the application in optical coherence tomography medical imaging, where the image resolution is related to the spectral bandwidth of the light source used. The achievement of bandwidths larger than 100 nm are demonstrated in this work through the optimization of molecular beam epitaxy growth conditions. This may be done optimizing the statistical size-dispersion of the dot ensemble, or through the use of different dot layers emitting at slightly different wavelengths. The large bandwidth emission is obtained also due to the peculiar energy structure of this material, for which a multi-state emission appears under particular injection conditions. As a term of comparison, best commercial single-chip superluminescent diodes for the imaging application at 1.3 μm show bandwidths around 60 nm. Moreover, the discrete nature of the energy levels in InAs quantum dots together with the implementation of a GaAs-based technology can be beneficial for the device temperature stability (the competing technology, based on InP, suffers from strong thermal degradation). The analysis and understanding of the device temperature characteristics will be detailed in the last chapter of the manuscript. Even though standard devices show an important temperature dependence, a better stability may be achieved through the use of p-doped active regions. In the last few years quantum dot devices have shown outstanding properties if compared to the competing quantum well technology. Low threshold currents, high temperature stability and low chirp in lasers, large bandwidths and low gain saturation in amplifiers have been demonstrated. However, in spite of the large interest among the scientific community, many of the microscopic processes at the origin of the electro-optical characteristics of this material are not completely understood yet. The physics of the quantum dot active material, will be modeled in this work through the use of systems of rate equations with different complexity depending on the system they are applied to. We will provide a mean-field rate equation model allowing to get insights about carrier dynamics in QD lasers. Also, we will develop two different traveling-wave rate equation models, one for the modeling of the L-I characteristics and the other for the modeling of the spectral characteristics of quantum dot superluminescent diodes. Considering the carrier and photon density distributions across the device cavity is essential in superluminescent diodes, where the high single pass gain results in large non-homogeneities of photon and carrier distributions. The work is motivated by an industrial cooperation with EXALOS AG, a leading company in the development, manufacturing, and sales of broadband superluminescent diodes.

EPFL2007

Attosecond coherent control of free-electron wave functions using semi-infinite light fields

Brett Eugene Barwick, Gabriele Berruto, Fabrizio Carbone, Ido Kaminer, Ivan Madan, Enrico Pomarico, Giovanni Maria Vanacore

Light–electron interaction is the seminal ingredient in free-electron lasers and dynamical investigation of matter. Pushing the coherent control of electrons by light to the attosecond timescale and below would enable unprecedented applications in quantum circuits and exploration of electronic motions and nuclear phenomena. Here we demonstrate attosecond coherent manipulation of a free-electron wave function, and show that it can be pushed down to the zeptosecond regime. We make a relativistic single-electron wavepacket interact in free-space with a semi-infinite light field generated by two light pulses reflected from a mirror and delayed by fractions of the optical cycle. The amplitude and phase of the resulting electron–state coherent oscillations are mapped in energy-momentum space via momentum-resolved ultrafast electron spectroscopy. The experimental results are in full agreement with our analytical theory, which predicts access to the zeptosecond timescale by adopting semi-infinite X-ray pulses.