Review of Charged Particle Dynamics. Beam Optics and Focusing Systems Without Space Charge. Linear Beam Optics with Space Charge. Self-Consistent Theory of Beams. Emittance Variation. Beam Physics Research from 1993 to 2007. Appendices. List of Frequently Used Symbols. Bibliography. Index.

Theory and Design of Charged Particle Beams

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.

Mapping surface plasmons on a single metallic nanoparticle

2D layered materials (2DLMs) are a subject of intense research for a wide variety of applications (e.g., electronics, photonics, and optoelectronics) due to their unique physical properties. Most recently, increasing research efforts on 2DLMs are projected toward the nonlinear optical properties of 2DLMs, which are not only fascinating from the fundamental science point of view but also intriguing for various potential applications. Here, the current state of the art in the field of nonlinear optics based on 2DLMs and their hybrid structures (e.g., mixed-dimensional heterostructures, plasmonic structures, and silicon/fiber integrated structures) is reviewed. Several potential perspectives and possible future research directions of these promising nanomaterials for nonlinear optics are also presented.

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Nonlinear Optics with 2D Layered Materials.

Watching a single molecule move on its intrinsic timescale has been one of the central goals of modern nanoscience, and calls for measurements that combine ultrafast temporal resolution with atomic spatial resolution. Steady-state experiments access the requisite spatial scales, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution. But tracking the intrinsic dynamics of a single molecule directly in the time domain faces the challenge that interactions with the molecule must be confined to a femtosecond time window. For individual nanoparticles, such ultrafast temporal confinement has been demonstrated by combining scanning tunnelling microscopy with so-called lightwave electronics, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on timescales faster even than a single cycle of light. Here we build on ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state. It thereby removes a single electron from an individual pentacene molecule's highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record approximately 100-femtosecond snapshot images of the orbital structure with sub-angstrom spatial resolution, and to reveal, through pump/probe measurements, coherent molecular vibrations at terahertz frequencies directly in the time domain. We anticipate that the combination of lightwave electronics and the atomic resolution of our approach will open the door to visualizing ultrafast photochemistry and the operation of molecular electronics on the single-orbital scale.

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Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam.

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven 'quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

We study photon-induced scattering of swift electrons with confined light in an ultrafast transmission electron microscope. The fluence-dependent sideband population in the kinetic energy spectra evidences the quantum coherent manipulation of the electron momenta.

Quantum coherent interaction of electrons with optical near-fields in an ultrafast electron microscope

Photon-induced scattering of swift electrons with confined light is studied by ultrafast transmission electron microscopy (UTEM) and employed to locally map optical near-fields. Fluence-dependent kinetic energy spectra reveal quantum coherent scattering features.

Electron-light interaction in optical near-fields studied by ultrafast transmission electron microscopy

Ultrafast transmission electron microscopy (UTEM) is a rapidly developing technique which aims to elucidate laser-triggered ultrafast processes at the nanometer scale [1]. In UTEM, ultrafast imaging and spectroscopy with sub-picosecond temporal resolution is achieved by utilizing electron pulses in a stroboscopic laser-pump/electron-probe scheme (Fig 1a). The previously employed flat-surface photocathodes put a severe limit on the achievable spatial resolution due to their intrinsically large electron source size, demanding novel pulsed electron source concepts.

Jakob Schauss

Papers

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam.

Quantum coherent interaction of electrons with optical near-fields in an ultrafast electron microscope

Electron-light interaction in optical near-fields studied by ultrafast transmission electron microscopy

Ultrafast Transmission Electron Microscopy with nanoscale Photoemitters