The high peak electric fields provided by single-cycle light pulses can be harnessed to manipulate and control charge motion in solid-state systems, resulting in electron emission out of metals and semiconductors [1][2][3][4][5][6] or high harmonics generation in dielectrics 7,8 . These processes are of a non-perturbative character and require precise reproducibility of the electric-field profile 9-14 . Here, we vary the carrier-envelope phase of 6-fs-long near-infrared pulses with pJ-level energy to control electronic transport in a laterally confined nanoantenna with an 8 nm gap. Peak current densities of 50 MA cm -2 are achieved, corresponding to the transfer of individual electrons in a half-cycle period of 2 fs. The observed behaviours are made possible by the strong distortion of the effective tunnelling barrier due to the extreme electric fields that the nanostructure provides and sustains under sub-cycle optical biasing. Operating at room temperature and in a standard atmosphere, the performed experiments demonstrate a robust class of nanoelectronic switches gated by phase-locked optical transients of minute energy content.Present-day high-frequency devices operate in the microwave range, but direct control of electron flow by the electric-field profile of few-cycle optical pulses has recently been demonstrated 12,15 . These experiments were based on strong perturbation of the electronic system in a dielectric material, resulting in a large incoherent background current. Nanoscale confinement of the region biased by the optical transient might avoid a significant influence of nonlinear conductivity in an insulating substrate and result in purely coherent tunnelling currents 16 that may be controlled by the precise shape of the electric field cycles. Our approach to reaching this goal is illustrated in the upper part of Fig. 1a. A single-cycle near-infrared pulse (left) is focused to a nanoscale junction of an electronic circuit (centre) with nonlinear and antisymmetric current-voltage (I-V) characteristics (right). An effective bias then arises when the exciting electric field is cosine-shaped (blue transient and blue dot in the I-V scheme) because its extremum occurs only for one polarity. Consequently, the symmetry of electronic transport is broken, even when integrating over the entire transient, and a net tunnelling current of electrons results through the potential barrier represented by the free-space gap (Fig. 1b,c). Our experiment favours tunnelling over other phenomena such as multiphoton ionization 4 by operating with ultrashort pulses and extreme nanoconfinement of the electric field. No background current exists when the control field is sineshaped (red transient and dot in the I-V characteristics, respectively), because positive and negative polarities now have precisely opposite effects. Consequently, the total current amplitude and direction may be set by varying the carrier-envelope phase (CEP), Δφ CEP , of the pulse. Owing to the single-cycle pulse duration, nanoscale constriction and fi...
Plasmonic nanoantennas are efficient devices to concentrate light in spatial regions much smaller than the wavelength. Only recently, their ability to manipulate photons also on a femtosecond time scale has been harnessed. Nevertheless, designing the dynamical properties of optical antennas has been difficult since the relevant microscopic processes governing their ultrafast response have remained unclear. Here, we exploit frequency-resolved optical gating to directly investigate plasmon response times of different antenna geometries resonant in the near-infrared. Third-harmonic imaging is used in parallel to spatially monitor the plasmonic mode patterns. We find that the few-femtosecond dynamics of these nanodevices is dominated by radiative damping. A high efficiency for nonlinear frequency conversion is directly linked to long plasmon damping times. This single parameter explains the counterintuitive result that rod-type nanoantennas with minimum volume generate by far the strongest third-harmonic emission as compared to the more bulky geometries of bow-tie-, elliptical-, or disk-shaped specimens.
We report on the generation of extreme ultraviolet radiation utilizing the plasmonic field enhancement in arrays of bow-tie gold optical antennae. Furthermore, their suitability to support high-order harmonic generation is examined by means of finite-difference time-domain calculations and experiments. Particular emphasis is paid to the thermal properties, which become significant at the employed peak intensities. A damage threshold depending on the antenna length is predicted and confirmed by our experimental findings. Moreover, the gas density in the vicinity of the antennae is characterized experimentally to determine the number of atoms contributing to the measured radiation, which is almost an order of magnitude larger than previously reported.
We investigate the multiphoton photoluminescence characteristics of gold nanoantennas fabricated from single crystals and polycrystalline films. By exciting these nanostructures with ultrashort pulses tunable in the near-infrared range, we observe distinct features in the broadband photoluminescence spectrum. By comparing antennas of different crystallinity and shape, we demonstrate that the nanoscopic geometry of plasmonic devices determines the shape of the emission spectra. Our findings rule out the contribution of the gold band structure in shaping the photoluminescence.
Fundamental interactions induced by lattice vibrations on ultrafast time scales have become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the terahertz-frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here we report on the generation and nonlinear propagation of giant (1 per cent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for unambiguous characterization of arbitrary ultrafast acoustic transients. The giant acoustic pulses experience substantial nonlinear reshaping after a propagation distance of only 100 nm in a crystalline gold layer. Excellent agreement with the Korteveg-de Vries model points to future quantitative nonlinear femtosecond terahertz-ultrasonics at the nano-scale in metals at room temperature.
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