Johannes Schötz

Attosecond physics at the nanoscale

Recently two emerging areas of research, attosecond and nanoscale physics, have started to come together. Attosecond physics deals with phenomena occurring when ultrashort laser pulses, with duration on the femto- and sub-femtosecond time scales, interact with atoms, molecules or solids. The laser-induced electron dynamics occurs natively on a timescale down to a few hundred or even tens of attoseconds (1 attosecond  =  1 as  =  10-18 s), which is comparable with the optical field. For comparison, the revolution of an electron on a 1s orbital of a hydrogen atom is  ∼152 as. On the other hand, the second branch involves the manipulation and engineering of mesoscopic systems, such as solids, metals and dielectrics, with nanometric precision. Although nano-engineering is a vast and well-established research field on its own, the merger with intense laser physics is relatively recent. In this report on progress we present a comprehensive experimental and theoretical overview of physics that takes place when short and intense laser pulses interact with nanosystems, such as metallic and dielectric nanostructures. In particular we elucidate how the spatially inhomogeneous laser induced fields at a nanometer scale modify the laser-driven electron dynamics. Consequently, this has important impact on pivotal processes such as above-threshold ionization and high-order harmonic generation. The deep understanding of the coupled dynamics between these spatially inhomogeneous fields and matter configures a promising way to new avenues of research and applications. Thanks to the maturity that attosecond physics has reached, together with the tremendous advance in material engineering and manipulation techniques, the age of atto-nanophysics has begun, but it is in the initial stage. We present thus some of the open questions, challenges and prospects for experimental confirmation of theoretical predictions, as well as experiments aimed at characterizing the induced fields and the unique electron dynamics initiated by them with high temporal and spatial resolution.

Attosecond nanoscale near-field sampling

The promise of ultrafast light-field-driven electronic nanocircuits has stimulated the development of the new research field of attosecond nanophysics. An essential prerequisite for advancing this new area is the ability to characterize optical near fields from light interaction with nanostructures, with sub-cycle resolution. Here we experimentally demonstrate attosecond near-field retrieval for a tapered gold nanowire. By comparison of the results to those obtained from noble gas experiments and trajectory simulations, the spectral response of the nanotaper near field arising from laser excitation can be extracted.

Intensity dependence of the attosecond control of the dissociative ionization of D2

Light-field driven electron localization in deuterium molecules in intense near single-cycle laser fields is studied as a function of the laser intensity. The emission of D+ ions from the dissociative ionization of D2 is interrogated with single-shot carrier–envelope phase (CEP)-tagged velocity map imaging. We explore the reaction for an intensity range of (1.0–2.8) × 1014 W cm−2, where laser-driven electron recollision leads to the population of excited states of D2+. Within this range we find the onset of dissociation from 3σ states of D2+ by comparing the experimental data to quantum dynamical simulations including the first eight states of D2+. We find that dissociation from the 3σ states yields D+ ions with kinetic energies above 8 eV. Electron localization in the dissociating molecule is identified through an asymmetry in the emission of D+ ions with respect to the laser polarization axis. The observed CEP-dependent asymmetry indicates two mechanisms for the population of 3σ states: (1) excitation by electron recollision to the lower excited states, followed by laser-field excitation to the 3σ states, dominating at low intensities, and (2) direct excitation to the 3σ states by electron recollision, playing a role at higher intensities.

Reconstruction of Nanoscale Near Fields by Attosecond Streaking

Recent advances in attosecond science in combination with the well-established techniques of nanofabrication have led to the new research field of attosecond nanophysics. One central goal is the characterization and manipulation of electromagnetic fields on the attosecond and nanometer scale. This has so far remained challenging both theoretically and experimentally. One major obstacle is the inhomogeneity of the electric fields. We present a general model below, which allows the description of attosecond streaking in near fields. It allows the classification into different regimes as well as the reconstruction of the electric fields at the surface. In addition, we discuss the case of parallel polarization of the streaking fields to the surface, which has so far not been considered for attosecond streaking from metallic surfaces. Finally, we review recent measurements of the electric field and response function of a gold nanotaper. Our results are highly relevant for future attosecond streaking experiments in inhomogeneous fields.

Attosecond-controlled photoemission from metal nanowire tips in the few-electron regime

Metal nanotip photoemitters have proven to be versatile in fundamental nanoplasmonics research and applications, including, e.g., the generation of ultrafast electron pulses, the adiabatic focusing of plasmons, and as light-triggered electron sources for microscopy. Here, we report the generation of high energy photoelectrons (up to 160 eV) in photoemission from single-crystalline nanowire tips in few-cycle, 750-nm laser fields at peak intensities of (2-7.3) × 1012 W/cm2. Recording the carrier-envelope phase (CEP)-dependent photoemission from the nanowire tips allows us to identify rescattering contributions and also permits us to determine the high-energy cutoff of the electron spectra as a function of laser intensity. So far these types of experiments from metal nanotips have been limited to an emission regime with less than one electron per pulse. We detect up to 13 e/shot and given the limited detection efficiency, we expect up to a few ten times more electrons being emitted from the nanowire. Within ...

Optical Control of Young’s Type Double-slit Interferometer for Laser-induced Electron Emission from a Nano-tip

Interference experiments with electrons in a vacuum can illuminate both the quantum and the nanoscale nature of the underlying physics. An interference experiment requires two coherent waves, which can be generated by splitting a single coherent wave using a double slit. If the slit-edge separation is larger than the coherence width at the slit, no interference appears. Here we employed variations in surface barrier at the apex of a tungsten nano-tip as slits and achieved an optically controlled double slit, where the separation and opening-and-closing of the two slits can be controlled by respectively adjusting the intensity and polarization of ultrashort laser pulses. Using this technique, we have demonstrated interference between two electron waves emitted from the tip apex, where interference has never been observed prior to this technique because of the large slit-edge separation. Our findings pave the way towards simple time-resolved electron holography on e.g. molecular adsorbates employing just a nano-tip and a screen.

Sub-cycle steering of the deprotonation of acetylene by intense few-cycle mid-infrared laser fields

Directional breaking of the C-H/C-D molecular bond is manipulated in acetylene (C2H2) and deuterated acetylene (C2D2) by waveform controlled few-cycle mid-infrared laser pulses with a central wavelength around 1.6 μm at an intensity of about 8 × 1013 W/cm2. The directionality of the deprotonation of acetylene is controlled by changing the carrier-envelope phase (CEP). The CEP-control can be attributed to the laser-induced superposition of vibrational modes, which is sensitive to the sub-cycle evolution of the laser waveform. Our experiments and simulations indicate that near-resonant, intense mid-infrared pulses permit a higher degree of control of the directionality of the reaction compared to those obtained in near-infrared fields, in particular for the deuterated species.

Optimization of a nanotip on a surface for the ultrafast probing of propagating surface plasmons

We theoretically analyze a method for characterizing propagating surface plasmon polaritons (SPPs) on a thin gold film. The SPPs are excited by few-cycle near-infrared pulses using Kretschmann coupling, and a nanotip is used as a local field sensor. This geometry removes the influence of the incident excitation laser from the near fields, and enhances the plasmon electric field strength. Using finite-difference-time-domain studies we show that the geometry can be used to measure SPP waveforms as a function of propagation distance. The effects of the nanotip shape and material on the field enhancement and plasmonic response are discussed.

High power CEP-stable 2 μm source based on fiber-laser seeded Innoslab with 100-kHz to 1-MHz repetition rate

Intense laser fields with controlled waveform are an important tool in strong-field and attosecond physics. Mid-inirared laser systems based on difference frequency generation (DFG) provide passively carrier-envelope phase (CEP) stable femtosecond pulses [1]. As Mid-IR generation is inherently inefficient, systems based on optical parametric amplification (OPA) and DFG are either limited by the peak power [2] or repetition rate [3].

Photoemission from Nanomaterials in Strong Few-Cycle Laser Fields

The application of ultra-short waveform-controlled laser fields to nanostructured materials enables the generation of localized near-fields with well-defined spatiotemporal field evolution. The optical fields that can be tailored on sub-wavelength spatial and attosecond temporal scales have a high potential for the control of ultrafast processes at the nanoscale, with important implications for laser-driven electron acceleration, extreme ultraviolet (XUV) light generation, and nanoscale electronics operating at optical frequencies.