A Gold Needle Tip Array Ultrafast Electron Source with High Beam Quality.

Electron sources are crucial elements in diverse applications such as electron microscopes, synchrotrons, and free-electron lasers. Nanometer-sharp needle tips are electron emitters with the highest beam quality, yet for a single needle the current is limited. Combining the emission of multiple needles promises large current yields while preserving the individual emitters' favorable properties. We present an ultrafast electron source consisting of a lithographically fabricated array of sharp gold tips illuminated with 25 fs laser pulses. The source provides up to 2000 electrons per pulse for moderate laser peak intensities of 1011 W/cm2 and a narrow energy width of 0.5 ± 0.05 eV at low current. The electron beam has a well-behaved Gaussian profile and is highly collimated, yielding a small normalized emittance on the order of nm·rad. These properties are well suited for applications requiring both high current and spatial resolution, such as free-electron light sources and chip-based particle accelerators.

Weak measurements and quantum-to-classical transitions in free electron-photon interactions.

How does the quantum-to-classical transition of measurement occur? This question is vital for both foundations and applications of quantum mechanics. Here, we develop a new measurement-based framework for characterizing the classical and quantum free electron-photon interactions and then experimentally test it. We first analyze the transition from projective to weak measurement in generic light-matter interactions and show that any classical electron-laser-beam interaction can be represented as an outcome of weak measurement. In particular, the appearance of classical point-particle acceleration is an example of an amplified weak value resulting from weak measurement. A universal factor, [Formula: see text], quantifies the measurement regimes and their transition from quantum to classical, where [Formula: see text] corresponds to the ratio between the electron wavepacket size and the optical wavelength. This measurement-based formulation is experimentally verified in both limits of photon-induced near-field electron microscopy and the classical acceleration regime using a DLA. Our results shed new light on the transition from quantum to classical electrodynamics, enabling us to employ the essence of the wave-particle duality of both light and electrons in quantum measurement for exploring and applying many quantum and classical light-matter interactions.

Optical measurement of the work function and the field reduction factor of metallic needle tips.

Quintessential parameters for needle tip-based electron sources are the work function, the tip apex radius, and the field reduction factor. They determine the static emission properties and strongly influence laser-triggered photoemission experiments at these needle tips. We present a simple method based on photoemission with two different commonly available continuous-wave laser diodes to determine both parameters in situ. We demonstrate our technique at tungsten needle tips. In a first application, use the method to in situ monitor changes of the emitter caused by illumination with strong femtosecond laser pulses. After illumination, we observe an increase in the work function caused by laser-induced changes to the apex of the tip. These changes are reversible upon field evaporation and are accompanied by a change in the spatial electron emission distribution. We believe that this simple in situ work function determination technique is applicable to any metal and in many experimental settings.

Coherent nanophotonic electron accelerator.

Particle accelerators are essential tools in a variety of areas of industry, science and medicine1-4. Typically, the footprint of these machines starts at a few square metres for medical applications and reaches the size of large research centres. Acceleration of electrons with the help of laser light inside of a photonic nanostructure represents a microscopic alternative with potentially orders-of-magnitude decrease in cost and size5-16. Despite large efforts in research on dielectric laser acceleration17,18, including complex electron phase space control with optical forces19-21, noteworthy energy gains have not been shown so far. Here we demonstrate a scalable nanophotonic electron accelerator that coherently combines particle acceleration and transverse beam confinement, and accelerates and guides electrons over a considerable distance of 500 µm in a just 225-nm-wide channel. We observe a maximum coherent energy gain of 12.3 keV, equalling a substantial 43% energy increase of the initial 28.4 keV to 40.7 keV. We expect this work to lead directly to the advent of nanophotonic accelerators offering high acceleration gradients up to the GeV m-1 range utilizing high-damage-threshold dielectric materials22 at minimal size requirements14. These on-chip particle accelerators will enable transformative applications in medicine, industry, materials research and science14,23,24.

Highly Localized Optical Field Enhancement at Neon Ion Sputtered Tungsten Nanotips.

We present laser-driven rescattering of electrons at a nanometric protrusion (nanotip), which is fabricated with an in situ neon ion sputtering technique applied to a tungsten needle tip. Electron energy spectra obtained before and after the sputtering show rescattering features, such as a plateau and high-energy cutoff. Extracting the optical near-field enhancement in both cases, we observe a strong increase of more than 2-fold for the nanotip. Accompanying finite-difference time-domain (FDTD) simulations show a good match with the experimentally extracted near-field strengths. Additionally, high electric field localization for the nanotip is found. The combination of transmission electron microscope imaging of such nanotips and the determination of the near-field enhancement by electron rescattering represent a full characterization of the electric near-field of these intriguing electron emitters. Ultimately, nanotips as small as single nanometers can be produced, which is of utmost interest for electron diffraction experiments and low-emittance electron sources.

Imaging the field inside nanophotonic accelerators.

Controlling optical fields on the subwavelength scale is at the core of nanophotonics. Laser-driven nanophotonic particle accelerators promise a compact alternative to conventional radiofrequency-based accelerators. Efficient electron acceleration in nanophotonic devices critically depends on achieving nanometer control of the internal optical nearfield. However, these nearfields have so far been inaccessible due to the complexity of the devices and their geometrical constraints, hampering the design of future nanophotonic accelerators. Here we image the field distribution inside a nanophotonic accelerator, for which we developed a technique for frequency-tunable deep-subwavelength resolution of nearfields based on photon-induced nearfield electron-microscopy. Our experiments, complemented by 3D simulations, unveil surprising deviations in two leading nanophotonic accelerator designs, showing complex field distributions related to intricate 3D features in the device and its fabrication tolerances. We envision an extension of our method for full 3D field tomography, which is key for the future design of highly efficient nanophotonic devices.

Tracing attosecond electron emission from a nanometric metal tip.

Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in d.c. operation1,2 to petahertz vacuum electronics in laser-driven operation3-8. In the latter process, the electron wavepacket undergoes semiclassical dynamics9,10 in the strong oscillating laser field, similar to strong-field and attosecond physics in the gas phase11,12. There, the subcycle electron dynamics has been determined with a stunning precision of tens of attoseconds13-15, but at solids the quantum dynamics including the emission time window has so far not been measured. Here we show that two-colour modulation spectroscopy of backscattering electrons16 uncovers the suboptical-cycle strong-field emission dynamics from nanostructures, with attosecond precision. In our experiment, photoelectron spectra of electrons emitted from a sharp metallic tip are measured as function of the relative phase between the two colours. Projecting the solution of the time-dependent Schrödinger equation onto classical trajectories relates phase-dependent signatures in the spectra to the emission dynamics and yields an emission duration of 710 ± 30 attoseconds by matching the quantum model to the experiment. Our results open the door to the quantitative timing and precise active control of strong-field photoemission from solid state and other systems and have direct ramifications for diverse fields such as ultrafast electron sources17, quantum degeneracy studies and sub-Poissonian electron beams18-21, nanoplasmonics22 and petahertz electronics23.

Light-field control of real and virtual charge carriers.

Light-driven electronic excitation is a cornerstone for energy and information transfer. In the interaction of intense and ultrafast light fields with solids, electrons may be excited irreversibly, or transiently during illumination only. As the transient electron population cannot be observed after the light pulse is gone, it is referred to as virtual, whereas the population that remains excited is called real1-4. Virtual charge carriers have recently been associated with high-harmonic generation and transient absorption5-8, but photocurrent generation may stem from real as well as virtual charge carriers9-14. However, a link between the generation of the carrier types and their importance for observables of technological relevance is missing. Here we show that real and virtual charge carriers can be excited and disentangled in the optical generation of currents in a gold-graphene-gold heterostructure using few-cycle laser pulses. Depending on the waveform used for photoexcitation, real carriers receive net momentum and propagate to the gold electrodes, whereas virtual carriers generate a polarization response read out at the gold-graphene interfaces. On the basis of these insights, we further demonstrate a proof of concept of a logic gate for future lightwave electronics. Our results offer a direct means to monitor and excite real and virtual charge carriers. Individual control over each type of carrier will markedly increase the integrated-circuit design space and bring petahertz signal processing closer to reality15,16.

Inverse-Designed Narrowband THz Radiator for Ultrarelativistic Electrons.

THz radiation finds various applications in science and technology. Pump-probe experiments at free-electron lasers typically rely on THz radiation generated by optical rectification of ultrafast laser pulses in electro-optic crystals. A compact and cost-efficient alternative is offered by the Smith-Purcell effect: a charged particle beam passes a periodic structure and generates synchronous radiation. Here, we employ the technique of photonic inverse design to optimize a structure for Smith-Purcell radiation at a single wavelength from ultrarelativistic electrons. The resulting design is highly resonant and emits narrowbandly. Experiments with a 3D-printed model for a wavelength of 900 µm show coherent enhancement. The versatility of inverse design offers a simple adaption of the structure to other electron energies or radiation wavelengths. This approach could advance beam-based THz generation for a wide range of applications.

Diamond-based dielectric laser acceleration.

The field of dielectric laser accelerators (DLA) garnered a considerable interest in the past six years as it offers novel opportunities in accelerator science and potentially transformative applications. Currently, the most widespread approach considers silicon-based structures due to their low absorption and high refractive index in the infrared spectral region and the well-developed silicon processing technology. In this paper we investigate a diamond as an alternative to silicon, mainly due to its considerably higher damage threshold. In particular, we find that our diamond grating allows a three times higher acceleration gradient (60 MeV/m) compared to silicon gratings designed for a similar electron energy. Using more complex geometries, GeV/m acceleration gradients are within reach for subrelativistic electrons.

Electronic Coherence and Coherent Dephasing in the Optical Control of Electrons in Graphene.

Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure a lower bound of the electronic coherence time of 22 ± 4 fs in graphene. The photocurrent is ideally suited to measure electronic coherence, as it is a direct result of coherent quantum-path interference, controlled by the delay between two ultrashort two-color laser pulses. The maximum delay for which interference between the population amplitude injected by the first pulse interferes with that generated by the second pulse determines the electronic coherence time. In particular, numerical simulations reveal that the experimental data yields a lower bound on the electronic coherence time, masked by coherent dephasing due to the broadband absorption in graphene. We expect that our results will significantly advance the understanding of coherent quantum control in solid-state systems ranging from excitation with weak fields to strongly driven systems.

Imprinting the quantum statistics of photons on free electrons.

The interaction between free electrons and light stands at the base of both classical and quantum physics, with applications in free-electron acceleration, radiation sources, and electron microscopy. Yet to this day, all experiments involving free-electron­light interactions are fully explained by describing the light as a classical wave. We observed quantum statistics effects of photons on free-electron­light interactions. We demonstrate interactions that pass continuously from Poissonian to super-Poissonian and up to thermal statistics, revealing a transition from quantum walk to classical random walk on the free-electron energy ladder. The electron walker serves as the probe in nondestructive quantum detection, measuring the second-order photon-correlation g(2)(0) and higher-orders g(n)(0). Unlike conventional quantum-optical detectors, the electron can perform both quantum weak measurements and projective measurements by evolving into an entangled joint state with the photons. These findings inspire hitherto inaccessible concepts in quantum optics, including free-electron­based ultrafast quantum tomography of light.

Quantum Interference Visibility Spectroscopy in Two-Color Photoemission from Tungsten Needle Tips.

When two-color femtosecond laser pulses interact with matter, electrons can be emitted through various multiphoton excitation pathways. Quantum interference between these pathways gives rise to a strong oscillation of the photoemitted electron current, experimentally characterized by its visibility. In this Letter, we demonstrate the two-color visibility spectroscopy of multiphoton photoemissions from a solid-state nanoemitter. We investigate the quantum pathway interference visibility over an almost octave-spanning wavelength range of the fundamental (ω) femtosecond laser pulses and their second harmonic (2ω). The photoemissions show a high visibility of 90% ± 5%, with a remarkably constant distribution. Furthermore, by varying the relative intensity ratio of the two colors, we find that we can vary the visibility between 0% and close to 100%. A simple but highly insightful theoretical model allows us to explain all observations, with excellent quantitative agreements. We expect this work to be universal to all kinds of photo-driven quantum interference, including quantum control in physics, chemistry, and quantum engineering.

Charged particle guiding and beam splitting with auto-ponderomotive potentials on a chip.

Electron and ion beams are indispensable tools in numerous fields of science and technology, ranging from radiation therapy to microscopy and lithography. Advanced beam control facilitates new functionalities. Here, we report the guiding and splitting of charged particle beams using ponderomotive forces created by the motion of charged particles through electrostatic optics printed on planar substrates. Shape and strength of the potential can be locally tailored by the lithographically produced electrodes' layout and the applied voltages, enabling the control of charged particle beams within precisely engineered effective potentials. We demonstrate guiding of electrons and ions for a large range of energies (from 20 to 5000 eV) and masses (from 5 · 10-4 to 131 atomic mass units) as well as electron beam splitting for energies up to the keV regime as a proof-of-concept for more complex beam manipulation.

Carrier-envelope-phase-stable soliton-based pulse compression to 4.4 fs and ultraviolet generation at the 800 kHz repetition rate.

In this Letter, we report the generation of a femtosecond supercontinuum extending from the ultraviolet to the near-infrared spectrum and detection of its carrier-envelope-phase (CEP) variation by f-to-2f interferometry. The spectrum is generated in a gas-filled hollow-core photonic crystal fiber, where soliton dynamics allows the CEP-stable self-compression of the optical parametric chirped-pulse amplifier pump pulses at 800 nm to a duration of 1.7 optical cycles, followed by dispersive wave emission. The source provides up to 1 µJ of pulse energy at the 800 kHz repetition rate, resulting in 0.8 W of average power, and it can be extremely useful, for example in strong-field physics, pump-probe measurements, and ultraviolet frequency comb metrology.

Generation of 1.5 cycle pulses at 780 nm at oscillator repetition rates with stable carrier-envelope phase.

We demonstrate a spectral broadening and compression setup for carrier-envelope phase (CEP) stable sub-10-fs Ti:sapphire oscillator pulses resulting in 3.9 fs pulses spectrally centered at 780 nm. Pulses from the oscillator with 2 nJ energy are launched into a 1 mm long all-normal dispersive solid-core photonic crystal fiber and spectrally broadened to more than one octave. Subsequent pulse compression is achieved with a phase-only 4f pulse shaper. Second harmonic frequency resolved optical gating with a ptychographic reconstruction algorithm is used to obtain the spectral phase, which is fed back as a phase mask to the shaper display for pulse compression. The compressed pulses are CEP stable with a long term standard deviation of 0.23 rad for the CEP noise and 0.32 rad for the integrated rms phase jitter. The high total throughput of 15% results in a remaining pulse energy of about 300 pJ at 80 MHz repetition rate. With these parameters and the ability to tailor the spectral phase, the system is well suited for waveform sensitive photoemission experiments with needle tips or nanostructures and can be easily adapted to other sub-10 fs ultra-broadband Ti:sapphire oscillators.

Dielectric laser electron acceleration in a dual pillar grating with a distributed Bragg reflector.

We report on the efficacy of a novel design for dielectric laser accelerators by adding a distributed Bragg reflector (DBR) to a dual pillar grating accelerating structure. This mimics a double-sided laser illumination, resulting in an enhanced longitudinal electric field while reducing the deflecting transverse effects when compared to single-sided illumination. We improve the coupling efficiency of the incident electric field into the accelerating mode by 57%. The 12 µm long structures accelerate sub-relativistic 28 keV electrons with gradients of up to 200 MeV/m in theory and 133 MeV/m in practice. This Letter shows how lithographically produced nano-structures help to make novel laser accelerators more efficient.

Generation and Characterization of Attosecond Microbunched Electron Pulse Trains via Dielectric Laser Acceleration.

Dielectric laser acceleration is a versatile scheme to accelerate and control electrons with the help of femtosecond laser pulses in nanophotonic structures. We demonstrate here the generation of a train of electron pulses with individual pulse durations as short as 270±80 attoseconds (FWHM), measured in an indirect fashion, based on two subsequent dielectric laser interaction regions connected by a free-space electron drift section, all on a single photonic chip. In the first interaction region (the modulator), an energy modulation is imprinted on the electron pulse. During free propagation, this energy modulation evolves into a charge density modulation, which we probe in the second interaction region (the analyzer). These results will lead to new ways of probing ultrafast dynamics in matter and are essential for future laser-based particle accelerators on a photonic chip.

Alternating-Phase Focusing for Dielectric-Laser Acceleration.

The concept of dielectric-laser acceleration provides the highest gradients among breakdown-limited (nonplasma) particle accelerators. However, stable beam transport and staging have not been shown experimentally yet. We present a scheme that confines the beam longitudinally and in one transverse direction. Confinement in the other direction is obtained by a single conventional quadrupole magnet. Within the small aperture of 420 nm we find the matched distributions, which allow an optimized injection into pure transport, bunching, and accelerating structures. The combination of these resembles the photonics analogue of the radio frequency quadrupole, but since our setup is entirely two dimensional, it can be manufactured on a microchip by lithographic techniques. This is a crucial step towards relativistic electrons in the MeV range from low-cost, handheld devices and connects the two fields of attosecond physics and accelerator physics.

Coherent Electron Trajectory Control in Graphene.

We investigate coherent electron dynamics in graphene, interacting with the electric field waveform of two orthogonally polarized, few-cycle laser pulses. Recently, we demonstrated that linearly polarized driving pulses lead to sub-optical-cycle Landau-Zener quantum path interference by virtue of the combination of intraband motion and interband transition [Higuchi et al., Nature 550, 224 (2017)NATUAS0028-083610.1038/nature23900]. Here we introduce a pulsed control laser beam, orthogonally polarized to the driving pulses, and observe the ensuing electron dynamics. The relative delay between the two pulses is a tuning parameter to control the electron trajectory, now in a complex fashion exploring the full two-dimensional reciprocal space in graphene. Depending on the relative phase, the electron trajectory in the reciprocal space can, e.g., be deformed to suppress the quantum path interference resulting from the driving laser pulse. Intriguingly, this strong-field-based complex matter wave manipulation in a two-dimensional conductor is driven by a high repetition rate laser oscillator, rendering unnecessary complex and expensive amplified laser systems.