14 research outputs found

    Wave-Mechanical Electron-Optical Modeling of Field-Emission Electron Sources

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    Electron source coherence has a very important influence on the imaging capabilities of modern electron microscopes. However, conventional electron source models that are based on geometrical electron optics implicitly assume that the emission from the source surface is fully incoherent, which can complicate the treatment of highly coherent field-emission sources. In an attempt to treat the wave-optical properties of electron sources, models inspired by light optics treatments of (partially) coherent sources, which assume a planar source and free wave propagation, have been developed. In this case the underlying assumptions are problematic, because the source surface of a field emitter can have a radius of curvature on the nanometer scale, and the emitted electrons are accelerated by a strong, inhomogeneous electrostatic field following emission. We introduce a model based on wave-mechanical electron optics that draws on a quantum mechanical description of electron emission and propagation to obtain a physically consistent treatment of the wave-mechanical properties of electron sources. We apply the model to investigate spatial resolution limits in low-energy electron holography and microscopy, where it is shown that aberrations and coherence properties of the electron source are crucial and interrelated. The wave-mechanical electron-optical model can, furthermore, be readily generalized to assess and improve electron source performance in other scenarios and techniques where spatial and temporal coherence, and electron-optical aberrations, are relevant

    Femtosecond Thermal and Nonthermal Hot Electron Tunneling Inside a Photoexcited Tunnel Junction

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    Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photo-assisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transient thermalized electron distribution, but the tunneling of thermalized hot electrons on time scales faster than electron-lattice equilibration is not well understood. Here, we investigate ultrafast electronic heating and transient thermionic tunneling inside a metallic photoexcited tunnel junction and its role in the generation of ultrafast photocurrents in STM. Phase-resolved sampling of broadband THz pulses via the THz-field-induced modulation of ultrafast photocurrents allows us to probe the electronic temperature evolution inside the STM tip, and to observe the competition between instantaneous and delayed tunneling due to nonthermal and thermal hot electron distributions in real time. Our results reveal the pronounced nonthermal character of photo-induced hot electron tunneling, and provide a detailed microscopic understanding of hot electron dynamics inside a laser-excited tunnel junction

    Ultrafast rotational motions of supported nanoclusters probed by electron diffraction

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    In crystals, microscopic energy flow is governed by electronic and vibrational excitations. In nanoscale materials, however, translations and rotations of entire nanoparticles represent additional fundamental excitations. The observation of such motions is elusive as most ultrafast techniques are insensitive to motions of the phonons’ frame of reference. Here, we study heterostructures of size-selected Au nanoclusters with partial (111) orientation on few-layer graphite with femtosecond electron diffraction. We demonstrate that ultrafast, constrained rotations of nanoclusters, so-called librations, in photo-induced non-equilibrium conditions can be observed separately from vibrational structural dynamics. Molecular dynamics and electron diffraction simulations provide quantitative understanding on librations-induced deviations from the conventional temperature dependence of diffraction patterns. We find that nanocluster librations with a period of ∼20 picoseconds are triggered quasi-impulsively by graphene flexural motions. These ultrafast structural dynamics modulate the Au/C interface and hence are expected to play a key role in energy- and mass-transport at the nanoscale

    Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

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    Citation: Savelyev, E., Boll, R., Bomme, C., Schirmel, N., Redlin, H., Erk, B., . . . Rolles, D. (2017). Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser. New Journal of Physics, 19, 13. doi:10.1088/1367-2630/aa652dIn pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene (C6H3F2I) molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. Wediscuss in detail the necessary data analysis steps and describe the origin of the timedependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment

    Quantitative sampling of femtosecond THz voltage pulses and hot electron dynamics in an STM junction

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    We demonstrate phase-resolved detection of femtosecond voltage transients in a scanning tunneling microscope induced by ultrabroadband THz pulses from a spintronic emitter, and probe hot electron dynamics inside the photoexcited junction on the nano-femtoscale

    Orthostatic hypotension in older persons: a diagnostic algorithm

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    Orthostatic hypotension (OH) is a frequent phenomenon in older persons and usually has a multifactorial origin. When the diagnosis is suspected, the work-up should initially be directed at the most prevalent causes. This clinical algorithm may be a useful tool in the diagnostic proces

    Multiple-orbital effects in laser-induced electron diffraction of aligned molecules

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    Photoelectron angular distributions (PADs) resulting from 800 and 1300 nm strong-field ionization of impulsively aligned CF3I molecules were analyzed using time-dependent density functional theory (TDDFT). The normalized difference between the PADs for aligned and antialigned molecules displays large modulations in the high-energy recollision plateau that are assigned to the diffraction of backscattered photoelectrons. The TDDFT calculations reveal that, in spite of their 2.6 eV energy difference, ionization from the HOMO-1 orbital contributes to the diffraction pattern on the same footing as ionization from the doubly degenerate HOMO orbital
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