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.

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.

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.

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.

Strong-Field Bloch Electron Interferometry for Band-Structure Retrieval.

When Bloch electrons in a solid are exposed to a strong optical field, they are coherently driven in their respective bands where they acquire a quantum phase as the imprint of the band shape. If an electron approaches an avoided crossing formed by two bands, it may be split by undergoing a Landau-Zener transition. We here employ subsequent Landau-Zener transitions to realize strong-field Bloch electron interferometry, allowing us to reveal band structure information. In particular, we measure the Fermi velocity (band slope) of graphene in the vicinity of the K points as (1.07±0.04) nm fs^{-1}. We expect strong-field Bloch electron interferometry for band structure retrieval to apply to a wide range of material systems and experimental conditions, making it suitable for studying transient changes in band structure with femtosecond temporal resolution at ambient conditions.

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.

Light-field-driven currents in graphene.

The ability to steer electrons using the strong electromagnetic field of light has opened up the possibility of controlling electron dynamics on the sub-femtosecond (less than 10-15 seconds) timescale. In dielectrics and semiconductors, various light-field-driven effects have been explored, including high-harmonic generation, sub-optical-cycle interband population transfer and the non-perturbative change of the transient polarizability. In contrast, much less is known about light-field-driven electron dynamics in narrow-bandgap systems or in conductors, in which screening due to free carriers or light absorption hinders the application of strong optical fields. Graphene is a promising platform with which to achieve light-field-driven control of electrons in a conducting material, because of its broadband and ultrafast optical response, weak screening and high damage threshold. Here we show that a current induced in monolayer graphene by two-cycle laser pulses is sensitive to the electric-field waveform, that is, to the exact shape of the optical carrier field of the pulse, which is controlled by the carrier-envelope phase, with a precision on the attosecond (10-18 seconds) timescale. Such a current, dependent on the carrier-envelope phase, shows a striking reversal of the direction of the current as a function of the driving field amplitude at about two volts per nanometre. This reversal indicates a transition of light-matter interaction from the weak-field (photon-driven) regime to the strong-field (light-field-driven) regime, where the intraband dynamics influence interband transitions. We show that in this strong-field regime the electron dynamics are governed by sub-optical-cycle Landau-Zener-Stückelberg interference, composed of coherent repeated Landau-Zener transitions on the femtosecond timescale. Furthermore, the influence of this sub-optical-cycle interference can be controlled with the laser polarization state. These coherent electron dynamics in graphene take place on a hitherto unexplored timescale, faster than electron-electron scattering (tens of femtoseconds) and electron-phonon scattering (hundreds of femtoseconds). We expect these results to have direct ramifications for band-structure tomography and light-field-driven petahertz electronics.

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.

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.

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.

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 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.

Attosecond control of electrons emitted from a nanoscale metal tip.

Attosecond science is based on steering electrons with the electric field of well controlled femtosecond laser pulses. It has led to the generation of extreme-ultraviolet pulses with a duration of less than 100 attoseconds (ref. 3; 1 as = 10(-18) s), to the measurement of intramolecular dynamics (by diffraction of an electron taken from the molecule under scrutiny) and to ultrafast electron holography. All these effects have been observed with atoms or molecules in the gas phase. Electrons liberated from solids by few-cycle laser pulses are also predicted to show a strong light-phase sensitivity, but only very small effects have been observed. Here we report that the spectra of electrons undergoing photoemission from a nanometre-scale tungsten tip show a dependence on the carrier-envelope phase of the laser, with a current modulation of up to 100 per cent. Depending on the carrier-envelope phase, electrons are emitted either from a single sub-500-attosecond interval of the 6-femtosecond laser pulse, or from two such intervals; the latter case leads to spectral interference. We also show that coherent elastic re-scattering of liberated electrons takes place at the metal surface. Owing to field enhancement at the tip, a simple laser oscillator reaches the peak electric field strengths required for attosecond experiments at 100-megahertz repetition rates, rendering complex amplified laser systems dispensable. Practically, this work represents a simple, extremely sensitive carrier-envelope phase sensor, which could be shrunk in volume to about one cubic centimetre. Our results indicate that the attosecond techniques developed with (and for) atoms and molecules can also be used with solids. In particular, we foresee subfemtosecond, subnanometre probing of collective electron dynamics (such as plasmon polaritons) in solid-state systems ranging in scale from mesoscopic solids to clusters and to single protruding atoms.

Transverse and longitudinal characterization of electron beams using interaction with optical near-fields.

We demonstrate an experimental technique for both transverse and longitudinal characterization of bunched femtosecond free electron beams. The operation principle is based on monitoring of the current of electrons that obtained an energy gain during the interaction with the synchronized optical near-field wave excited by femtosecond laser pulses. The synchronous accelerating/decelerating fields confined to the surface of a silicon nanostructure are characterized using a highly focused sub-relativistic electron beam. Here the transverse spatial resolution of 450 nm and femtosecond temporal resolution of 480 fs (sub-optical-cycle temporal regime is briefly discussed) achievable by this technique are demonstrated.

Two-Color Coherent Control of Femtosecond Above-Threshold Photoemission from a Tungsten Nanotip.

We demonstrate coherent control of multiphoton and above-threshold photoemission from a single solid-state nanoemitter driven by a fundamental and a weak second harmonic laser pulse. Depending on the relative phase of the two pulses, electron emission is modulated with a contrast of the oscillating current signal of up to 94%. Electron spectra reveal that all observed photon orders are affected simultaneously and similarly. We confirm that photoemission takes place within 10 fs. Accompanying simulations indicate that the current modulation with its large contrast results from two interfering quantum pathways leading to electron emission.