Jörg Robin

Ultrafast Electron Emission from a Sharp Metal Nanotaper Driven by Adiabatic Nanofocusing of Surface Plasmons

We report photoelectron emission from the apex of a sharp gold nanotaper illuminated via grating coupling at a distance of 50 μm from the emission site with few-cycle near-infrared laser pulses. We find a fifty-fold increase in electron yield over that for direct apex illumination. Spatial localization of the electron emission to a nanometer-sized region is demonstrated by point-projection microscopic imaging of a silver nanowire. Our results reveal negligible plasmon-induced electron emission from the taper shaft and thus efficient nanofocusing of few-cycle plasmon wavepackets. This novel, remotely driven emission scheme offers a particularly compact source of ultrashort electron pulses of immediate interest for miniaturized electron microscopy and diffraction schemes with ultrahigh time resolution.

Differential Nanosecond Protein Dynamics in Homologous Calcium Sensors.

Shaping the temporal response of photoreceptors is facilitated by a well-balanced second messenger cascade, in which two neuronal Ca(2+)-sensor proteins operate in a sequential relay mechanism. Although they share structurally similar sensing units, they differentially activate the same target protein. Here, as a prototypical case in Ca(2+)-mediated signal processing, we investigate differential cellular responsiveness in protein conformational dynamics on a nanosecond time scale. For this, we have site-specifically labeled cysteine residues in guanylate cyclase-activating protein GCAP1 by the fluorescent dye Alexa647 and probed its local environment via time-resolved fluorescence spectroscopy. Fluorescence lifetime and rotational anisotropy measurements reveal a distinct structural movement of the polypeptide chain around position 106 upon release of Ca(2+). This is supported by analyzing the diffusional dye motion in a wobbling-in-a-cone model and by molecular dynamics simulations. We conclude that GCAP1 and its cellular cognate GCAP2 operate by distinctly different switching mechanisms despite their high structural homology.

High passive CEP stability from a few-cycle, tunable NOPA-DFG system for observation of CEP-effects in photoemission

The investigation of fundamental mechanisms taking place on a femtosecond time scale is enabled by ultrafast pulsed laser sources. Here, the control of pulse duration, center wavelength, and especially the carrier-envelope phase has been shown to be of essential importance for coherent control of high harmonic generation and attosecond physics and, more recently, also for electron photoemission from metallic nanostructures. In this paper we demonstrate the realization of a source of 2-cycle laser pulses tunable between 1.2 and 2.1 μm, and with intrinsic CEP stability. The latter is guaranteed by difference frequency generation between the output pulse trains of two noncollinear optical parametric amplifier stages that share the same CEP variations. The CEP stability is better than 50 mrad over 20 minutes, when averaging over 100 pulses. We demonstrate the good CEP stability by measuring kinetic energy spectra of photoemitted electrons from a single metal nanostructure and by observing a clear variation of the electron yield with the CEP.

Ultrafast coherent dynamics of Rydberg electrons bound in the image potential near a single metallic nano-object (Presentation Recording)

Image potential states are well established surface states of metallic films [1]. For a single metallic nanostructure these surface states can be localized in the near-field arising from illumination by a strong laser field. Thus single metallic nanostructures offer the unique possibility to study quantum systems with both high spatial and ultrafast temporal resolution. Here, we investigate the dynamics of Rydberg states localized to a sharp metallic nanotaper. For this purpose we realized a laser system delivering few-cycle pulses tunable over a wide wavelength range [2]. Pulses from a regenerative titanium:sapphire amplifier generate a white light continuum, from which both a proportion in the visible and in the infrared are amplified in two non-collinear optical parametric amplification (NOPA) stages. Difference frequency generation (DFG) of both stages provides pulses in the near-infrared. With a precisely delayed sequence of few-cycle pulses centered around 600 nm (NOPA#1 output) and 1600 nm (DFG output) we illuminate the apex of a sharply etched gold tip. Varying the delay we observe an exponential decay of photoemitted electrons with a distinctly asymmetric decay length on both sides, indicating the population of different states. Superimposed on the decay is a clearly discernible quantum beat pattern with a period of <50 fs, which arises from the motion of Rydberg photoelectrons bound within their own image potential. These results therefore constitute a step towards controlling single electron wavepackets released from a gold tip opening up fascinating perspectives for applications in ultrafast electron microscopy [3]. [1] Hofer, U. et al. Science 277, 1480 (1997) [2] Vogelsang, J., Robin J. et al. Opt. Express 22, 25295 (2014) [3] Petek, H. et al. ACS Nano 8, 5 (2014)

Controlling the Motion of Strong-Field, Few-Cycle Photoemitted Electrons in the Near-Field of a Sharp Metal Tip

The real-time probing of electron motion in solid nanostructures or the visualization of nanoplasmonic field dynamics may come into reach using electron pulses generated by strong-field tunneling from sharp gold tips irradiated by few-cycle laser pulses. The acceleration of the ultrashort electron wavepackets in the near field of the sharp gold tips introduces new possibilities of steering and control of electron wavepackets by light, which is expected to pave the way towards such ultrafast probing. Here we discuss the motion of these highly accelerated electrons in the near-field and demonstrate how the carrier-envelope phase admits a new control mechanism for their motion.