Femtosecond Drift Photocurrents Generated by an Inversely Designed Plasmonic Antenna.

Photocurrents play a crucial role in various applications, including light detection, photovoltaics, and THz radiation generation. Despite the abundance of methods and materials for converting light into electrical signals, the use of metals in this context has been relatively limited. Nanostructures supporting surface plasmons in metals offer precise light manipulation and induce light-driven electron motion. Through the inverse design optimization of a gold nanostructure, we demonstrate enhanced volumetric, unidirectional, intense, and ultrafast photocurrents via a magneto-optical process derived from the inverse Faraday effect. This is achieved through fine-tuning the amplitude, polarization, and gradients in the local light field. The virtually instantaneous process allows dynamic photocurrent modulation by varying optical pulse duration, potentially yielding nanosources of intense, ultrafast, planar magnetic fields and frequency-tunable THz emission. These findings open avenues for ultrafast magnetic material manipulation and hold promise for nanoscale THz spectroscopy.

Coherent two-beam steering of delocalized nonlinear photoluminescence in a plasmon cavity.

We aim at controlling the spatial distribution of nonlinear photoluminescence in a shaped micrometer-size crystalline gold flake. Interestingly, the underlying surface plasmon modal landscape sustained by this mesoscopic structure can be advantageously used to generate nonlinear photoluminescence (nPL) in remote locations away from the excitation spot. By controlling the modal pattern, we show that the delocalized nonlinear photoluminescence intensity can be redistributed spatially. This is first accomplished by changing the polarization orientation of the pulsed laser excitation in order to select a subset of available surface plasmon modes within a continuum. We then propose a second approach to redistribute the nPL within the structure by implementing a phase control of the plasmon interference pattern arising from a coherent two-beam excitation. Control and engineering of the nonlinear photoluminescence spatial extension is a prerequisite for deploying the next generation of plasmonic-enabled integrated devices relying on hot carriers.

Vectorial probing of electric and magnetic transitions in variable optical environments and vice-versa.

We use europium doped single crystalline NaYF4nanorods for probing the electric and magnetic contributions to the local density of optical states (LDOS). Reciprocically, we determine intrinsic properties of the emitters (oscillator strength, quantum yield) by comparing their measured and simulated optical responses in front of a mirror. We first experimentally determine the specifications of the nanoprobe (orientation and oscillator strength of the electric and magnetic dipoles moments) and show significant orientation sensitivity of the branching ratios associated with electric and magnetic transitions. In a second part, we measure the modification of the LDOS in front of a gold mirror in a Drexhage's experiment. We discuss the role of the electric and magnetic LDOS on the basis of numerical simulations, taking into account the orientation of the dipolar emitters. We demonstrate that they behave like degenerated dipoles sensitive to polarized partial LDOS.

Modal and wavelength conversions in plasmonic nanowires.

We show that plasmonic nanowire-nanoparticle systems can perform nonlinear wavelength and modal conversions and potentially serve as building blocks for signal multiplexing and novel trafficking modalities. When a surface plasmon excited by a pulsed laser beam propagates in a nanowire, it generates a localized broadband nonlinear continuum at the nanowire surface as well as at active locations defined by sites where nanoparticles are absorbed (enhancement sites). The local response may couple to new sets of propagating modes enabling a complex routing of optical signals through modal and spectral conversions. Different aspects influencing the optical signal conversions are presented, including the parameters defining the local formation of the continuum and the subsequent modal routing in the nanowire.

Directional second-harmonic generation controlled by sub-wavelength facets of an organic mesowire.

Directional harmonic generation is an important property characterizing the ability of nonlinear optical antennas to diffuse the signal in a well-defined region of space. Herein, we show how sub-wavelength facets of an organic molecular mesowire crystal can be utilized to systematically vary the directionality of second-harmonic generation (SHG) in the forward-scattering geometry. We demonstrate this capability on crystalline diamonoanthraquinone (DAAQ) mesowires with sub-wavelength facets. We observed that the radial angles of the SHG emission can be tuned over a range of 130 deg. This angular variation arises due to spatially distributed nonlinear dipoles in the focal volume of the excitation as well as the geometrical cross section and facet orientation of the mesowire. Numerical simulations of the near-field excitation profile corroborate the role of the mesowire geometry in localizing the electric field. In addition to directional SHG from the mesowire, we experimentally observe optical waveguiding of the nonlinear two-photon excited fluorescence (TPEF). Interestingly, we observed that for a given pump excitation, the TPEF signal is isotropic and delocalized, whereas the SHG emission is directional and localized at the location of excitation. All the observed effects have direct implications not only in active nonlinear optical antennas but also in nonlinear signal processing.

Selective excitation of surface plasmon modes propagating in Ag nanowires.

Surface plasmon modes propagating in metal nanowires are conveniently excited by focusing a laser beam on one extremity of the nanowire. We find that the precise positioning of the nanowire inside the focal region drastically influences the excitation efficiency of the different SPP modes sustained by the plasmonic waveguide. We demonstrate a spatially selective excitation of bound and leaky surface plasmon modes with excitation maps that strongly depend on the orientation of the incident linear polarization. We discuss this modal selection by considering the inhomogeneous distribution of the field components inside the focus. Our finding provides a way to discriminate the effective indices of the modes offering thus an increased coupling agility for future nanowire-based plasmonic architectures.

Spectral pointillism of enhanced Raman scattering for accessing structural and conformational information on single protein.

In this contribution, we provide new insights on the temporal fluctuations of surface enhanced Raman spectra (SERS) of large single molecules such as proteins. Because they can only fit partly into small active volume, SERS analysis is referred to spectral pointillism where only protein subdomains are shined and the whole protein landscape is built from the dynamics of successive individual spectra. By applying our approach on bovine serum albumin, we show that single protein subdomains are mostly comprised of three distinct amino acids. Surface amino acids such as lysine are preferentially detected in the open form of the protein. The investigation of the tryptophan Fermi doublet in the single protein regime is highly instructive on the protein conformation. We finally demonstrate that spectral pointillism enables to correlate individual amino acids with structural information.

Spontaneous Hot-Electron Light Emission from Electron-Fed Optical Antennas.

Nanoscale electronics and photonics are among the most promising research areas providing functional nanocomponents for data transfer and signal processing. By adopting metal-based optical antennas as a disruptive technological vehicle, we demonstrate that these two device-generating technologies can be interfaced to create an electronically driven self-emitting unit. This nanoscale plasmonic transmitter operates by injecting electrons in a contacted tunneling antenna feedgap. Under certain operating conditions, we show that the antenna enters a highly nonlinear regime in which the energy of the emitted photons exceeds the quantum limit imposed by the applied bias. We propose a model based upon the spontaneous emission of hot electrons that correctly reproduces the experimental findings. The electron-fed optical antennas described here are critical devices for interfacing electrons and photons, enabling thus the development of optical transceivers for on-chip wireless broadcasting of information at the nanoscale.

Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas.

Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that these nonlinear radiations are emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are locally induced by a propagating surface plasmon at the excitation frequency, enabling thereby a polariton-mediated spatial tailoring and design of coherent and incoherent nonlinear responses.

Nonlinear photon-assisted tunneling transport in optical gap antennas.

We introduce strongly coupled optical gap antennas to interface optical radiation with current-carrying electrons at the nanoscale. The transducer relies on the nonlinear optical and electrical properties of an optical gap antenna operating in the tunneling regime. We discuss the underlying physical mechanisms controlling the conversion involving d-band electrons and demonstrate that a simple two-wire optical antenna can provide advanced optoelectronic functionalities beyond tailoring the electromagnetic response of a single emitter. Interfacing an electronic command layer with a nanoscale optical device may thus be facilitated by the optical rectennas discussed here.

Reversible strong coupling in silver nanoparticle arrays using photochromic molecules.

In this Letter, we demonstrate a reversible strong coupling regime between a dipolar surface plasmon resonance and a molecular excited state. This reversible state is experimentally observed on silver nanoparticle arrays embedded in a polymer film containing photochromic molecules. Extinction measurements reveal a clear Rabi splitting of 294 meV, corresponding to ~13% of the molecular transition energy. We derived an analytical model to confirm our observations, and we emphasize the importance of spectrally matching the polymer absorption with the plasmonic resonance to observe coupled states. Finally, the reversibility of this coupling is illustrated by cycling the photochromic molecules between their two isomeric forms.

Light Emission and Conductance Fluctuations in Electrically Driven and Plasmonically Enhanced Molecular Junctions.

Electrically connected and plasmonically enhanced molecular junctions combine the optical functionalities of high field confinement and enhancement (cavity function), and of high radiative efficiency (antenna function) with the electrical functionalities of molecular transport. Such combined optical and electrical probes have proven useful for the fundamental understanding of metal-molecule contacts and contribute to the development of nanoscale optoelectronic devices including ultrafast electronics and nanosensors. Here, we employ a self-assembled metal-molecule-metal junction with a nanoparticle bridge to investigate correlated fluctuations in conductance and tunneling-induced light emission at room temperature. Despite the presence of hundreds of molecules in the junction, the electrical conductance and light emission are both highly sensitive to atomic-scale fluctuations-a phenomenology reminiscent of picocavities observed in Raman scattering and of luminescence blinking from photoexcited plasmonic junctions. Discrete steps in conductance associated with fluctuating emission intensities through the multiple plasmonic modes of the junction are consistent with a finite number of randomly localized, point-like sources dominating the optoelectronic response. Contrasting with these microscopic fluctuations, the overall plasmonic and electronic functionalities of our devices feature long-term survival at room temperature and under an electrical bias of a few volts, allowing for measurements over several months.

Memristive Control of Plasmon-Mediated Nonlinear Photoluminescence in Au Nanowires.

Nonlinear photoluminescence (N-PL) is a broadband photon emission arising from a nonequilibrium heated electron distribution generated at the surface of metallic nanostructures by ultrafast pulsed laser illumination. N-PL is sensitive to surface morphology, local electromagnetic field strength, and electronic band structure, making it relevant to probe optically excited nanoscale plasmonic systems. It also has been key to accessing the complex multiscale time dynamics ruling electron thermalization. Here, we show that plasmon-mediated N-PL emitted by a gold nanowire can be modified by an electrical architecture featuring a nanogap. Upon voltage activation, we observe that N-PL becomes dependent on the electrical transport dynamics and can thus be locally modulated. This finding brings an electrical leverage to externally control the photoluminescence generated from metal nanostructures and constitutes an asset for the development of emerging nanoscale interface devices managing photons and electrons.

Focus issue on surface plasmon photonics introduction.

The 6th International Conference on Surface Plasmon Photonics (SPP6) was held in Ottawa, Canada from May 26th to 31st, 2013. This independent series of biennial conferences is widely regarded as the premier series in the field, and the 6th edition maintained the tradition of excellence. This Focus Issue collects several papers related to research presented at SPP6, and although the number of papers it comprises is small compared to the total number of papers presented at the conference, the issue is representative and provides a good snapshot of the field at this point in time.

Launching propagating surface plasmon polaritons by a single carbon nanotube dipolar emitter.

We report on the excitation of propagating surface plasmon polaritons in thin metal films by a single emitter. Upon excitation in the visible regime, individual semiconducting single-walled carbon nanotubes are shown to act as directional near-infrared point dipole sources launching propagating surface plasmons mainly along the direction of the nanotube axis. Plasmon excitation and propagation is monitored in Fourier and real space by leakage radiation microscopy and is modeled by rigorous theoretical calculations. Coupling to plasmons almost completely reshapes the emission of nanotubes both spatially and with respect to polarization as compared to photoluminescence on a dielectric substrate.

Silencing and enhancement of second-harmonic generation in optical gap antennas.

Amplifying local electromagnetic fields by engineering optical interactions between individual constituents of an optical antenna is considered fundamental for efficient nonlinear wavelength conversion in nanometer-scale devices. In contrast to this general statement we show that high field enhancement does not necessarily lead to an optimized nonlinear activity. In particular, we demonstrate that second-harmonic responses generated at strongly interacting optical gap antennas can be significantly suppressed. Numerical simulations are confirming silencing of second-harmonic in these coupled systems despite the existence of local field amplification. We then propose a simple approach to restore and amplify the second-harmonic signal by changing the manner in which electrically-connected optical antennas are interacting in the charge-transfer plasmon regime. Our observations provide critical design rules for realizing optimal structures that are essential for a broad variety of nonlinear surface-enhanced characterizations and for realizing the next generation of electrically-driven optical antennas.

Performance of electro-optical plasmonic ring resonators at telecom wavelengths.

In this work we report on the characteristics of an electro-optical dielectric-loaded surface plasmon polariton waveguide ring resonator. By doping the dielectric host matrix with an electro-optical material and designing an appropriate set of planar electrodes, we measured a 16% relative change of transmission upon application of a controlled electric field. We have analyzed the temporal response of the device and conclude that electrostriction of the host matrix is playing a dominating role in the transmission response.

In-plane remote photoluminescence excitation of carbon nanotube by propagating surface plasmon.

In this work, we demonstrate propagating surface plasmon polariton (SPP) coupled photoluminescence (PL) excitation of single-walled carbon nanotube (SWNT). SPPs were launched at a few micrometers from individually marked SWNT, and plasmon-coupled PL was recorded to determine the efficiency of this remote in-plane addressing scheme. The efficiency depends upon the following factors: (i) longitudinal and transverse distances between the SPP launching site and the location of the SWNT and (ii) orientation of the SWNT with respect to the plasmon propagation wave vector (k(SPP)). Our experiment explores the possible integration of carbon nanotubes as a plasmon sensor in plasmonic and nanophotonic devices.

Optical rectification and thermal currents in optical tunneling gap antennas.

Electrically-contacted optical gap antennas are nanoscale interface devices enabling the transduction between photons and electrons. This new generation of device, usually constituted of metal elements (e.g. gold), captures visible to near infrared electromagnetic radiation and rectifies the incident energy in a direct-current (DC) electrical signal. However, light absorption by the metal may lead to additional thermal effects which need to be taken into account to understand the complete photo-response of the devices. The purpose of this communication is to discriminate the contribution of laser-induced thermo-electric effects in the photo-assisted electronic transport. We show case our analysis with the help of electromigrated devices.

Atomic scale memristive photon source.

Memristive devices are an emerging new type of devices operating at the scale of a few or even single atoms. They are currently used as storage elements and are investigated for performing in-memory and neuromorphic computing. Amongst these devices, Ag/amorphous-SiOx/Pt memristors are among the most studied systems, with the electrically induced filament growth and dynamics being thoroughly investigated both theoretically and experimentally. In this paper, we report the observation of a novel feature in these devices: The appearance of new photoluminescent centers in SiOx upon memristive switching, and photon emission correlated with the conductance changes. This observation might pave the way towards an intrinsically memristive atomic scale light source with applications in neural networks, optical interconnects, and quantum communication.