arXiv subjects

René Kullock

Publications and source records attributed to René Kullock.

5 recordsLinked to original sources

arXiv2023

Controlling field asymmetry in nanoscale gaps for second harmonic generation

Plasmonic dimer antennas create strong field enhancement by squeezing light into a nanoscale gap. These optical hotspots are highly attractive for boosting nonlinear processes, such as harmonic generation, photoelectron emission, and ultrafast electron transport. Alongside large field enhancement, such phenomena often require control over the field asymmetry in the hotspot, which is challenging considering the nanometer length scales. Here, by means of strongly enhanced second harmonic generation, we demonstrate unprecedented control over the field distribution in a hotspot by systematically introducing geometrical asymmetry to the antenna gap. We use focused helium ion beam milling of mono-crystalline gold to realize asymmetric-gap dimer antennas in which an ultra-sharp tip with 3 nm apex radius faces a flat counterpart, conserving the bonding antenna mode and the concomitant field enhancement at the fundamental frequency. By decreasing the tip opening angle, we are able to systematically increase both field enhancement and asymmetry, thus enhancing second harmonic radiation to the far-field, which is nearly completely suppressed for equivalent symmetric dimer antennas. Combining these findings with second harmonic radiation patterns as well as quantitative nonlinear simulations, we further obtain remarkably detailed insights into the mechanism of second harmonic generation at the nanoscale. Our results open new opportunities for the realization of novel nonlinear nanoscale systems, where the control over local field asymmetry in combination with large field enhancement is essential to create nonreciprocal functionalities.

physics.optics↗

arXiv2022

Tunable nano-plasmonic photodetectors

Visible and infrared photons can be detected with a broadband response via the internal photoeffect. By using plasmonic nanostructures, i.e. nanoantennas, wavelength selectivity can be introduced to such detectors through geometry-dependent resonances. Also, additional functionality, like electronic responsivity switching and polarization detection have been realized. However, previous devices consisted of large arrays of nanostructures to achieve detectable photocurrents. Here we show that this concept can be scaled down to a single antenna level, resulting in detector dimensions well below the resonance wavelength of the device. Our design consists of a single electrically-connected plasmonic nanoantenna covered with a wide-bandgap semiconductor allowing broadband photodetection in the VIS/NIR via injection of hot carriers. We demonstrate electrical switching of the color sensitivity as well as polarization detection. Our results hold promise for the realization of ultra small, highly integratable photodetectors with advanced functionality.

physics.optics↗

arXiv2019

Nonclassical optical properties of mesoscopic gold

Gold nanostructures have important applications in nanoelectronics, nano-optics as well as in precision metrology due to their intriguing opto-electronic properties. These properties are governed by the bulk band structure but to some extend are tunable via geometrical resonances. Here we show that the band structure of gold itself exhibits significant size-dependent changes already for mesoscopic critical dimensions below 30 nm. To suppress the effects of geometrical resonances and grain boundaries, we prepared atomically flat ultrathin films of various thicknesses by utilizing large chemically grown single-crystalline gold platelets. We experimentally probe thickness-dependent changes of the band structure by means of two-photon photoluminescence and observe a surprising 100-fold increase of the nonlinear signal when the gold film thickness is reduced below 30 nm allowing us to optically resolve single-unit-cell steps. The effect is well explained by density functional calculations of the thickness-dependent 2D band structure of gold.

physics.optics↗

arXiv2015

Single-crystalline gold microplates grown on substrates by solution-phase synthesis

Chemically synthesized single-crystalline gold microplates have been attracting increasing interests because of their potential as high-quality gold films for nanotechnology. We present the growth of tens of nanometer thick and tens of micrometer large single-crystalline gold plates directly on solid substrates by solution-phase synthesis. Compared to microplates deposited on substrates from dispersion phase, substrate-grown plates exhibit significantly higher quality by avoiding severe small-particle contamination and aggregation. Substrate-grown gold plates also open new perspec-tives to study the growth mechanism via intermittent growth and observation cycles of a large number of individual plates. Growth models are proposed to interpret the evolution of thickness, area and shape of plates. It is found that the plate surface remains smooth after regrowth, implying the application of regrowth for producing giant plates as well as unique single-crystalline nano-structures.

cond-mat.mtrl-sci↗

arXiv2015

Electrically-driven optical antennas

Unlike radiowave antennas, optical nanoantennas so far cannot be fed by electrical generators. Instead, they are driven by light or via optically active materials in their proximity. Here, we demonstrate direct electrical driving of an optical nanoantenna featuring an atomic-scale feed gap. Upon applying a voltage, quantum tunneling of electrons across the feed gap creates broadband quantum shot noise. Its optical frequency components are efficiently converted into photons by the antenna. We demonstrate that the properties of the emitted photons are fully controlled by the antenna architecture, and that the antenna improves the quantum efficiency by up to two orders of magnitude with respect to a non-resonant reference system. Our work represents a new paradigm for interfacing electrons and photons at the nanometer scale, e.g. for on-chip wireless data communication, electrically driven single- and multiphoton sources, as well as for background-free linear and nonlinear spectroscopy and sensing with nanometer resolution.

physics.optics↗