Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas.

The optimization of nonlinear optical processes on the nanoscale is a crucial step for the integration of complex functionalities into compact photonic devices and metasurfaces. In such systems, photon upconversion can be achieved with higher efficiencies via third-order processes, such as third-harmonic generation (THG), thanks to the resonantly enhanced volume currents. Conversely, second-order processes, such as second-harmonic generation (SHG), are often inhibited by the symmetry of metal lattices and of common nanoantenna geometries. SHG and THG processes in plasmonic nanostructures are generally treated independently because they typically represent small perturbations in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold for plasmon-enhanced nonlinear optics by providing evidence of a sum-frequency generation (SFG) process seeded by SHG, which sizably contributes to the overall THG yield. We address this mechanism by unveiling a characteristic fingerprint in the polarization state of the THG emission from gold noncentrosymmetric nanoantennas, which directly reflects the asymmetric distribution of second-harmonic fields within the structure and does not depend on the model one employs to describe photon upconversion. We suggest that such cascaded processes may also appear for structures that exhibit only moderate SHG yields. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows us to gain further insight into the physics of plasmon-enhanced nonlinear optical processes. This could be crucial in the realization of nanoscale elements for photon conversion and manipulation operating at room temperature.

Nonclassical Optical Properties of Mesoscopic Gold.

Gold nanostructures have important applications in nanoelectronics, nano-optics, and in precision metrology due to their intriguing optoelectronic properties. These properties are governed by the bulk band structure but to some extent 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.

Reversible Mapping and Sorting the Spin of Photons on the Nanoscale: A Spin-Optical Nanodevice.

The photon spin is an important resource for quantum information processing as is the electron spin in spintronics. However, for subwavelength confined optical excitations, polarization as a global property of a mode cannot be defined. Here, we show that any polarization state of a plane-wave photon can reversibly be mapped to a pseudospin embodied by the two fundamental modes of a subwavelength plasmonic two-wire transmission line. We design a device in which this pseudospin evolves in a well-defined fashion throughout the device reminiscent of the evolution of photon polarization in a birefringent medium and the behavior of electron spins in the channel of a spin field-effect transistor. The significance of this pseudospin is enriched by the fact that it is subject to spin-orbit locking. Combined with optically active materials to exert external control over the pseudospin precession, our findings could enable spin-optical transistors, that is, the routing and processing of quantum information with light on a subwavelength scale.

Electromechanically Tunable Suspended Optical Nanoantenna.

Coupling mechanical degrees of freedom with plasmonic resonances has potential applications in optomechanics, sensing, and active plasmonics. Here we demonstrate a suspended two-wire plasmonic nanoantenna acting like a nanoelectrometer. The antenna wires are supported and electrically connected via thin leads without disturbing the antenna resonance. As a voltage is applied, equal charges are induced on both antenna wires. The resulting equilibrium between the repulsive Coulomb force and the restoring elastic bending force enables us to precisely control the gap size. As a result the resonance wavelength and the field enhancement of the suspended optical nanoantenna can be reversibly tuned. Our experiments highlight the potential to realize large bandwidth optical nanoelectromechanical systems.

Mode matching in multiresonant plasmonic nanoantennas for enhanced second harmonic generation.

Boosting nonlinear frequency conversion in extremely confined volumes remains a challenge in nano-optics research, but can enable applications in nanomedicine, photocatalysis and background-free biosensing. To obtain brighter nonlinear nanoscale sources, approaches that enhance the electromagnetic field intensity and counter the lack of phase matching in nanoplasmonic systems are often employed. However, the high degree of symmetry in the crystalline structure of plasmonic materials (metals in particular) and in nanoantenna designs strongly quenches second harmonic generation. Here, we describe doubly-resonant single-crystalline gold nanostructures with no axial symmetry displaying spatial mode overlap at both the excitation and second harmonic wavelengths. The combination of these features allows the attainment of a nonlinear coefficient for second harmonic generation of ∼5 × 10(-10) W(-1), enabling a second harmonic photon yield higher than 3 × 10(6) photons per second. Theoretical estimations point toward the use of our nonlinear plasmonic nanoantennas as efficient platforms for label-free molecular sensing.

Atomic-scale confinement of resonant optical fields.

In the presence of matter, there is no fundamental limit preventing confinement of visible light even down to atomic scales. Achieving such confinement and the corresponding resonant intensity enhancement inevitably requires simultaneous control over atomic-scale details of material structures and over the optical modes that such structures support. By means of self-assembly we have obtained side-by-side aligned gold nanorod dimers with robust atomically defined gaps reaching below 0.5 nm. The existence of atomically confined light fields in these gaps is demonstrated by observing extreme Coulomb splitting of corresponding symmetric and antisymmetric dimer eigenmodes of more than 800 meV in white-light scattering experiments. Our results open new perspectives for atomically resolved spectroscopic imaging, deeply nonlinear optics, ultrasensing, cavity optomechanics, as well as for the realization of novel quantum-optical devices.

Electrically connected resonant optical antennas.

Electrically connected resonant optical antennas hold promise for the realization of highly efficient nanoscale electro-plasmonic devices that rely on a combination of electric fields and local near-field intensity enhancement. Here we demonstrate the feasibility of such a concept by attaching leads to the arms of a two-wire antenna at positions of minimal near-field intensity with negligible influence on the antenna resonance. White-light scattering experiments in accordance with simulations show that the optical tunability of connected antennas is fully retained. Analysis of the electric properties demonstrates that in the antenna gaps direct current (DC) electric fields of 10(8) V/m can consistently be achieved and maintained over extended periods of time without noticeable damage.