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The development of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics, which requires that the interacting waves propagate in transparent volumes for distances much longer than their wavelength. Here we present experimental evidence that optical nonlinearities in doped semiconductors are due to free-electron and their efficiency could exceed by several orders of magnitude that of conventional dielectric nonlinearities. Our experimental findings are supported by comprehensive computational results based on the hydrodynamic modeling, which naturally includes nonlocal effects, of the free-electron dynamics in heavily doped semiconductors. By studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density, we discriminate between hydrodynamic and dielectric nonlinearities. As a result, the value of maximum nonlinear efficiency as well as its spectral location can now be controlled by tuning the doping level. Having employed the common material platform InGaAs/InP that supports integrated waveguides, our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits.

All-optical modulation yields the promise of high-speed information processing. In this frame, metasurfaces are rapidly gaining traction as ultrathin multifunctional platforms for light management. Among the featured functionalities, they enable light wavefront manipulation and, more recently, demonstrated the ability to perform light-by-light manipulation through nonlinear optical processes. Here, by employing a nonlinear periodic metasurface, we demonstrate all-optical routing of telecom photons upconverted to the visible range. This is achieved via the interference between two frequency-degenerate upconversion processes, namely third-harmonic and sum-frequency generation, stemming from the interaction of a pump pulse with its frequency-doubled replica. By tuning the relative phase and polarization between these two pump beams, and concurrently engineering the nonlinear emission of the individual elements of the metasurfaces (meta-atoms) along with its pitch, we route the upconverted signal among the diffraction orders of the metasurface with a modulation efficiency up to 90%. Thanks to the phase control and the ultrafast dynamics of the underlying nonlinear processes, free-space all-optical routing could be potentially performed at rates close to the employed optical frequencies divided by the quality factor of the optical resonances at play. Our approach adds a further twist to optical interferometry, which is a key-enabling technique in a wide range of applications, such as homodyne detection, radar interferometry, LiDAR technology, gravitational waves detection, and molecular photometry. In particular, the nonlinear character of light upconversion combined with phase sensitivity is extremely appealing for enhanced imaging and biosensing., Comment: 18 pages, 6 figures

Infrared (IR) nanospectroscopy by photothermal induced resonance (PTIR) is a novel experimental technique that combines the nanoscale resolution granted by atomic force microscopy (AFM) and the chemical labelling made possible by IR absorption spectroscopy. While the technique has developed enormously over the last decade from an experimental point of view, the theoretical modelling of the signal still varies significantly throughout the literature and misses a solid benchmark. Here, we report an analysis focused on the electromagnetic and thermal simulations of a PTIR experiment. Thanks to a control experiment where the signal is acquired as a function of the thickness of a polymer film and for different tip geometries, we find clear evidence that the interface thermal resistances play a key role in the determination of the measured signal and should therefore always be accounted for by any quantitative modelling.

Graphene is an ideal material for integrated nonlinear optics thanks to its strong light-matter interaction and large nonlinear optical susceptibility. Graphene has been used in optical modulators, saturable absorbers, nonlinear frequency converters, and broadband light emitters. For the latter application, a key requirement is the ability to control and engineer the emission wavelength and bandwidth, as well as the electronic temperature of graphene. Here, we demonstrate that the emission wavelength of graphene$'$ s broadband hot carrier photoluminescence can be tuned by integration on photonic cavities, while thermal management can be achieved by out-of-plane heat transfer to hexagonal boron nitride. Our results pave the way to graphene-based ultrafast broadband light emitters with tunable emission., Comment: 22 pages, 5 Figures

Photosensitive proteins embedded in the cell membrane (about 5 nm thickness) act as photoactivated proton pumps, ion gates, enzymes, or more generally, as initiators of stimuli for the cell activity. They are composed of a protein backbone and a covalently bound cofactor (e.g. the retinal chromophore in bacteriorhodopsin (BR), channel rhodopsin, and other opsins). The light-induced conformational changes of both the cofactor and the protein are at the basis of the physiological functions of photosensitive proteins. Despite the dramatic development of microscopy techniques, investigating conformational changes of proteins at the membrane monolayer level is still a big challenge. Techniques based on atomic force microscopy (AFM) can detect electric currents through protein monolayers and even molecular binding forces in single-protein molecules but not the conformational changes. For the latter, Fourier-transform infrared spectroscopy (FTIR) using difference-spectroscopy mode is typically employed, but it is performed on macroscopic liquid suspensions or thick films containing large amounts of purified photosensitive proteins. In this work, we develop AFM-assisted, tip-enhanced infrared difference-nanospectroscopy to investigate light-induced conformational changes of the bacteriorhodopsin mutant D96N in single submicrometric native purple membrane patches. We obtain a significant improvement compared with the signal-to-noise ratio of standard IR nanospectroscopy techniques by exploiting the field enhancement in the plasmonic nanogap that forms between a gold-coated AFM probe tip and an ultraflat gold surface, as further supported by electromagnetic and thermal simulations. IR difference-spectra in the 1450-1800 cm^{-1} range are recorded from individual patches as thin as 10 nm, with a diameter of less than 500 nm, well beyond the diffraction limit for FTIR microspectroscopy..., Comment: published under ACS AuthorChoice license

Recent efforts in the field of surface-enhanced spectroscopies have focused on the paradigm of superchirality, entailing the engineering of the local electromagnetic fields to boost the enantiospecific interaction between light and chiral molecules. In this framework, approaches based on both metallic and dielectric nanostructures have been proposed and have also recently been extended to vibrational circular dichroism in the mid-infrared. In this work, we design, fabricate and characterize arrays of chiral plasmonic slits featuring enhanced chiral fields in the mid-infrared. We exploit collective lattice resonances to further enhance the local intensity and to generate sharp features in the circular dichroism spectra of the platform. Such features are ideally suited to test the superchiral coupling with the vibrational resonances of chiral molecules.

We introduce the use of superchiral surface waves for the all-optical separation of chiral compounds. Using a combination of electrodynamics modeling and analytical techniques, we show that the proposed approach provides chiral optical forces two orders of magnitude larger than those obtained with circularly polarized plane waves. Superchiral surface waves allow for enantiomer separation on spatial, temporal and size scales than would not be achievable with alternative techniques, thus representing a viable route towards all-optical enantiomer separation.

The optimization of nonlinear optical processes at the nanoscale is a crucial step for the development of nanoscale photon sources for quantum-optical networks. The development of innovative plasmonic nanoantenna designs and hybrid nanostructures to enhance optical nonlinearities in very small volumes represents one of the most promising routes. In such systems, the upconversion of photons can be achieved with high 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, since they both represent a small perturbation in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold in general, by providing evidence of a cascaded process in THG, which is fueled by SHG and sizably contributes to the overall yield. We address this mechanism by unveiling an anomalous fingerprint in the polarization state of the nonlinear emission from non-centrosymmetric gold nanoantennas and point out that such cascaded processes may also appear for structures that exhibit only moderate SHG yields - signifying its general relevance in plasmon-enhanced nonlinear optics. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows gaining further insight on 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., Comment: 25 pages, 4 figures

We demonstrate third harmonic generation in plasmonic antennas made of highly doped germanium and designed to be resonant in the mid infrared. Owing to the near-field enhancement, the result is an ultrafast, sub-diffraction, coherent light source tunable between 3 and 5 micrometer wavelength on a silicon substrate. To observe nonlinearity in this challenging spectral region, a high-power femtosecond laser system equipped with parametric frequency conversion in combination with an all-reflective confocal microscope setup is employed. We show spatially resolved maps of the linear scattering cross section and the nonlinear emission of single isolated antenna structures. A clear third order power dependence as well as the mid-infrared emission spectra prove the nonlinear nature of the light emission. Simulations support the observed resonance length of the double rod antenna and demonstrate that the field enhancement inside the antenna material is responsible for the nonlinear frequency mixing.

It has been recently suggested that the nonlinear optical processes in plasmonic nanoantennas allow for a substantial boost in the sensitivity of plasmonic sensing platforms. Here we present a sensing device based on an array of non-centrosymmetric plasmonic nanoantennas featuring enhanced second harmonic generation (SHG) integrated in a microfluidic chip. We evaluate its sensitivity both in the linear and nonlinear regime using a figure of merit (FOM = $(\Delta I/I)/\Delta n$) that accounts for the relative change in the measured intensity, \textit{I}, against the variation of the environmental refractive index \textit{n}. While the signal-to-noise ratio achieved in both regimes allows the detection of a minimum refractive index variation $\Delta n_{min} \approx 10^{-3}$, the platform operation in the nonlinear regime features a sensitivity (i.e. the FOM) that is at least 3 times higher than the linear one. Thanks to the surface sensitivity of plasmon-enhanced SHG, our results show that the development of such SHG sensing platforms with sensitivity performances exceeding those of their linear counterparts is within reach., Comment: 19 Pages, 5 Figures

The demand for single photon sources at $\lambda~=~1.54~\mu$m, which follows from the consistent development of quantum networks based on commercial optical fibers, makes Er:O$_x$ centers in Si still a viable resource thanks to the optical transition of $Er^{3+}~:~^4I_{13/2}~\rightarrow~^4I_{15/2}$. Yet, to date, the implementation of such system remains hindered by its extremely low emission rate. In this Letter, we explore the room-temperature photoluminescence (PL) at the telecomm wavelength of very low implantation doses of $Er:O_x$ in $Si$. The emitted photons, excited by a $\lambda~=~792~nm$ laser in both large areas and confined dots of diameter down to $5~\mu$m, are collected by an inverted confocal microscope. The lower-bound number of detectable emission centers within our diffraction-limited illumination spot is estimated to be down to about 10$^4$, corresponding to an emission rate per individual ion of about $4~\times~10^{3}$ photons/s., Comment: 13 pages, 4 figures

We present a novel chiral sensing platform that combines a one-dimensional photonic crystal design with a birefringent surface defect. The platform sustains simultaneous transverse electric and transverse magnetic surface modes, which are exploited to generate chiral surface waves. The present design provides homogeneous and superchiral fields of both handednesses over arbitrarily large areas in a wide spectral range, resulting in the enhancement of the circular dichroism signal by two orders of magnitude, thus paving the road toward the successful combination of surface-enhanced spectroscopies and electromagnetic superchirality., Comment: Added references. Corrected typos. Included new design for broadband chiral surface waves

We study the local field enhancement properties of self-similar nanolenses and compare the obtained results with the performance of standard dimer nanoantennas. We report that, despite the additional structural complexity, self-similar nanolenses are unable to provide significant improvements over the field enhancement performance of standard plasmonic dimers.

Impulsive interband excitation with femtosecond near-infrared pulses establishes a plasma response in intrinsic germanium structures fabricated on a silicon substrate. This direct approach activates the plasmonic resonance of the Ge structures and enables their use as optical antennas up to the mid-infrared spectral range. The optical switching lasts for hundreds of picoseconds until charge recombination red-shifts the plasma frequency. The full behavior of the structures is modeled by the electrodynamic response established by an electron-hole plasma in a regular array of antennas.

Heavily-doped semiconductor films are very promising for application in mid-infrared plasmonic devices because the real part of their dielectric function is negative and broadly tunable in this wavelength range. In this work we investigate heavily n-type doped germanium epilayers grown on different substrates, in-situ doped in the $10^{17}$ to $10^{19}$ cm$^{-3}$ range, by infrared spectroscopy, first principle calculations, pump-probe spectroscopy and dc transport measurements to determine the relation between plasma edge and carrier density and to quantify mid-infrared plasmon losses. We demonstrate that the unscreened plasma frequency can be tuned in the 400 - 4800 cm$^{-1}$ range and that the average electron scattering rate, dominated by scattering with optical phonons and charged impurities, increases almost linearly with frequency. We also found weak dependence of losses and tunability on the crystal defect density, on the inactivated dopant density and on the temperature down to 10 K. In films where the plasma was optically activated by pumping in the near-infrared, we found weak but significant dependence of relaxation times on the static doping level of the film. Our results suggest that plasmon decay times in the several-picosecond range can be obtained in n-type germanium thin films grown on silicon substrates hence allowing for underdamped mid-infrared plasma oscillations at room temperature., Comment: 18 pages, 10 figures

The n-type Ge-on-Si epitaxial material platform enables a novel paradigm for plasmonics in the mid-infrared, prompting the future development of lab-on-a-chip and subwavelength vibrational spectroscopic sensors. In order to exploit this material, through proper electrodynamic design, it is mandatory to retrieve the dielectric constants of the thin Ge epilayers with high precision due to the difference from bulk Ge crystals. Here we discuss the procedure we have employed to extract the real and imaginary part of the dielectric constants from normal incidence reflectance measurements, by combining the standard multilayer fitting procedure based on the Drude model with Kramers-Kronig transformations of absolute reflectance data in the zero-transmission range of the thin film., Comment: Infrared, Millimeter, and Terahertz waves (IRMMW-THz), 2014 39th International Conference on

We discuss the possibility of enhancing the chiroptical response from molecules uniformly distributed around nanostructures that sustain localized plasmon resonances. We demonstrate that the average optical chirality in the near field of any plasmonic nanostrucure cannot be significantly higher than that in a plane wave. This conclusion stems from the quasi-static nature of the nanoparticle-enhanced electromagnetic fields and from the fact that, at optical frequencies, the magnetic response of matter is much weaker than the electric one.

Boosting nonlinear frequency conversion in extremely confined volumes remains a key challenge in nano-optics, nanomedicine, photocatalysis, and background-free biosensing. To this aim, field enhancements in plasmonic nanostructures are often exploited to effectively compensate for the lack of phase-matching at the nanoscale. Second harmonic generation (SHG) is, however, strongly quenched by the high degree of symmetry in plasmonic materials at the atomic scale and in nanoantenna designs. Here, we devise a plasmonic nanoantenna lacking axial symmetry, which exhibits spatial and frequency mode overlap at both the excitation and the SHG wavelengths. The effective combination of these features in a single device allows obtaining unprecedented SHG conversion efficiency. Our results shed new light on the optimization of SHG at the nanoscale, paving the way to new classes of nanoscale coherent light sources and molecular sensing devices based on nonlinear plasmonic platforms., Comment: 14 pages, 4 figures

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 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 anti-symmetric 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, ultra-sensing, cavity optomechanics as well as for the realization of novel quantum-optical devices.

Nanoantennas for visible and infrared radiation can strongly enhance the interaction of light with nanoscale matter by their ability to efficiently link propagating and spatially localized optical fields. This ability unlocks an enormous potential for applications ranging from nanoscale optical microscopy and spectroscopy over solar energy conversion, integrated optical nanocircuitry, opto-electronics and density-ofstates engineering to ultra-sensing as well as enhancement of optical nonlinearities. Here we review the current understanding of optical antennas based on the background of both well-developed radiowave antenna engineering and the emerging field of plasmonics. In particular, we address the plasmonic behavior that emerges due to the very high optical frequencies involved and the limitations in the choice of antenna materials and geometrical parameters imposed by nanofabrication. Finally, we give a brief account of the current status of the field and the major established and emerging lines of investigation in this vivid area of research., Comment: Review article with 76 pages, 21 figures

Deep subwavelength integration of high-definition plasmonic nanostructures is of key importance for the development of future optical nanocircuitry for high-speed communication, quantum computation and lab-on-a-chip applications. So far the experimental realization of proposed extended plasmonic networks consisting of multiple functional elements remains challenging, mainly due to the multi-crystallinity of commonly used thermally evaporated gold layers. Resulting structural imperfections in individual circuit elements will drastically reduce the yield of functional integrated nanocircuits. Here we demonstrate the use of very large (>100 micron^2) but thin (<80 nm) chemically grown single-crystalline gold flakes, which, after immobilization, serve as an ideal basis for focused-ion beam milling and other top-down nanofabrication techniques on any desired substrate. Using this methodology we obtain high-definition ultrasmooth gold nanostructures with superior optical properties and reproducible nano-sized features over micrometer length scales. Our approach provides a possible solution to overcome the current fabrication bottleneck and to realize high-definition plasmonic nanocircuitry., Comment: 28 pages, 14 figures, including Supporting Information (11 pages, 10 figures)

The number of eigenmodes in plasmonic nanostructures increases with complexity due to mode hybridization, raising the need for efficient mode characterization and selection. Here we experimentally demonstrate direct imaging and selective excitation of the bonding and antibonding plasmon mode in symmetric dipole nanoantennas using confocal two-photon photoluminescence mapping. Excitation of a high-quality-factor antibonding resonance manifests itself as a two-lobed pattern instead of the single spot observed for the broad bonding resonance, in accordance with numerical simulations. The two-lobed pattern is observed due to the fact that excitation of the antibonding mode is forbidden for symmetric excitation at the feedgap, while concomitantly the mode energy splitting is large enough to suppress excitation of the bonding mode. The controlled excitation of modes in strongly coupled plasmonic nanostructures is mandatory for efficient sensors, in coherent control as well as for implementing well-defined functionalities in complex plasmonic devices., Comment: 11 pages, 5 figures, 1 supplementary information

An experimentally realizable prototype nanophotonic circuit consisting of a receiving and an emitting nano antenna connected by a two-wire optical transmission line is studied using finite-difference time- and frequency-domain simulations. To optimize the coupling between nanophotonic circuit elements we apply impedance matching concepts in analogy to radio frequency technology. We show that the degree of impedance matching, and in particular the impedance of the transmitting nano antenna, can be inferred from the experimentally accessible standing wave pattern on the transmission line. We demonstrate the possibility of matching the nano antenna impedance to the transmission line characteristic impedance by variations of the antenna length and width realizable by modern microfabrication techniques. The radiation efficiency of the transmitting antenna also depends on its geometry but is independent of the degree of impedance matching. Our systems approach to nanophotonics provides the basis for realizing general nanophotonic circuits and a large variety of derived novel devices.

By exploiting photo-induced reorientation in azo-polymer thin films, we demonstrate all-optical polarization-encoded information storage with a scanning near-field optical microscope. In the writing routine, 5-level bits are created by associating different bit values to different birefringence directions, induced in the polymer after illumination with linearly polarized light. The reading routine is then performed by implementing polarization-modulation techniques on the same near-field microscope, in order to measure the encoded birefringence direction., Comment: 13 pages, 5 figures