No Arabic abstract
Coherent broadband excitation of plasmons brings ultrafast photonics to the nanoscale. However, to fully leverage this potential for ultrafast nanophotonic applications, the capacity to engineer and control the ultrafast response of a plasmonic system at will is crucial. Here, we develop a framework for systematic control and measurement of ultrafast dynamics of near-field hotspots. We show deterministic design of the coherent response of plasmonic antennas at femtosecond timescales. Exploiting the emerging properties of coupled antenna configurations, we use the calibrated antennas to engineer two sought-after applications of ultrafast plasmonics: a subwavelength resolution phase shaper, and an ultrafast hotspot switch. Moreover, we demonstrate that mixing localized resonances of lossy plasmonic particles is the mechanism behind nanoscale coherent control. This simple, reproducible and scalable approach promises to transform ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid state physics and quantum biology.
Modern nonlinear optical materials allow light of one wavelength be efficiently converted into light at another wavelength. However, designing nonlinear optical materials to operate with ultrashort pulses is difficult, because it is necessary to match both the phase velocities and group velocities of the light. Here we show that self-organized nonlinear gratings can be formed with femtosecond pulses propagating through nanophotonic waveguides, providing simultaneous group-velocity matching and quasi-phase-matching for second harmonic generation. We record the first direct microscopy images of photo-induced nonlinear gratings, and demonstrate how these waveguides enable simultaneous $chi^{(2)}$ and $chi^{(3)}$ nonlinear processes, which we utilize to stabilize a laser frequency comb. Finally, we derive the equations that govern self-organized grating formation for femtosecond pulses and explain the crucial role of group-velocity matching. In the future, such nanophotonic waveguides could enable scalable, reconfigurable nonlinear optical systems.
Recent advancements in computational inverse design have begun to reshape the landscape of structures and techniques available to nanophotonics. Here, we outline a cross section of key developments at the intersection of these two fields: moving from a recap of foundational results to motivation of emerging applications in nonlinear, topological, near-field and on-chip optics.
Deterministic fractal antennas are employed to realize multimodal plasmonic devices. Such structures show strongly enhanced localized electromagnetic fields typically in the infrared range with a hierarchical spatial distribution. Realization of engineered fractal antennas operating in the optical regime would enable nanoplasmonic platforms for applications, such as energy harvesting, light sensing, and bio/chemical detection. Here, we introduce a novel plasmonic multiband metamaterial based on the Sierpinski carpet (SC) space-filling fractal, having a tunable and polarization-independent optical response, which exhibits multiple resonances from the visible to mid-infrared range. We investigate gold SCs fabricated by electron-beam lithography on CaF$_{2}$ and Si/SiO$_{2}$ substrates. Furthermore, we demonstrate that such resonances originate from diffraction-mediated localized surface plasmons, which can be tailored in deterministic fashion by tuning the shape, size, and position of the fractal elements. Moreover, our findings illustrate that SCs with high order of complexity present a strong and hierarchically distributed electromagnetic near-field of the plasmonic modes. Therefore, engineered plasmonic SCs provide an efficient strategy for the realization of compact active devices with a strong and broadband spectral response in the visible/mid-infrared range. We take advantage of such a technology by carrying out surface enhanced Raman spectroscopy (SERS) on Brilliant Cresyl Blue molecules deposited onto plasmonic SCs. We achieve a broadband SERS enhancement factor up to $10^{4}$, thereby providing a proof-of-concept application for chemical diagnostics.
Femtosecond-scale polarization state conversion is experimentally found in optical response of a plasmonic nanograting by means of time-resolved polarimetry. Simultaneous measurements of the Stokes parameters as a function of time with an averaging time-gate of 130 fs reveal a remarkable alteration of polarization state inside a single fs-pulse reflected from a plasmonic crystal. Time-dependent depolarization is experimentally found and described within an analytical model which predicts the four-fold enhancement of the polarization conversion effect with the use of the narrower gate. The effect is attributed to excitation of time-delayed polarization-sensitive surface plasmons with a highly birefringent Fano-type spectral profile.
Recent progress in nanotechnology has enabled us to fabricate subwavelength architectures that function as antennas for improving the exchange of optical energy with nanoscale matter. We describe the main features of optical antennas for enhancing quantum emitters and review designs that increase the spontaneous emission rate by orders of magnitude from the ultraviolet up to the near-infrared spectral range. To further explore how optical antennas may lead to unprecedented regimes of light-matter interaction, we draw a relationship between metal nanoparticles, radio-wave antennas and optical resonators. Our analysis points out how optical antennas may function as nanoscale resonators and how these may offer unique opportunities with respect to state-of-the-art microcavities.