Understanding the interplay between illumination and the electron distribution in metallic nanostructures is a crucial step towards developing applications such as plasmonic photo-catalysis for green fuels, nano-scale photo-detection and more. Elucidating this interplay is challenging, as it requires taking into account all channels of energy flow in the electronic system. Here, we develop such a theory, which is based on a coupled Boltzmann-heat equations and requires only energy conservation and basic thermodynamics, where the electron distribution, and the electron and phonon (lattice) temperatures are determined {\em uniquely}. Applying this theory to realistic illuminated nanoparticle systems, we find that the electron and phonon temperatures are similar, thus justifying the (classical) single temperature models. We show that while the fraction of high-energy ``hot'' carriers compared to thermalized carriers grows substantially with illumination intensity, it remains extremely small (on the order of $10^{-8}$). Importantly, most of the absorbed illumination power goes into heating rather than generating hot carriers, thus rendering plasmonic hot carrier generation extremely inefficient. Our formulation allows for the first time a unique quantitative comparison of theory and measurements of steady-state electron distributions in metallic nanostructures.
The authors of preprint arXiv:1810.00565 and paper in Light: Science & Applications (2019), Y. Dubi and Y. Sivan, made several wrong and inconsistent comments on several of our papers. In addition, the paper in Faraday Discuss. 214, 215-233 (2018) by the same authors also contains several wrong statements in relationship with our work. Moreover, the authors address in their comments features that were in fact not present in our work. In what follows we present correction to a number of specific points in which they either misrepresented or erroneously interpreted our published work.
Broadband absorption enhancement in ultra-thin crystalline Si solar cells by incorporating metallic and dielectric nanostructures in the back reflector
Optical properties of metallic nanoparticles are most often considered in terms of plasmons, the coupled states of light and quasi-free electrons. Here we predict that confinement of electrons inside the nanostructure leads to another, very different, type of resonance, which determines the optical properties in the frequency range significantly below the plasmonic resonance. We demonstrate that closely placed confinement-induces resonances typically join into a single composite "super-resonance" which produces giant nonlinearity at low frequencies. Our simulations show how such nonlinearities…
Over the last three decades, plasmonics using metallic nanostructures has become central to nanophotonics research. Recently, its targets have been extended to nonlinear optical phenomena. In a nonlinear regime, quantum mechanical effects, as exemplified by electron spill-out on the surface of nanostructures, significantly influence the optical response. Quantum hydrodynamic theory (QHT) is a promising basis for the analysis of nonlinear optical responses involving such quantum mechanical effects. Herein, QHT was applied to calculate the third-order optical nonlinearity of a spherical metallic…
Optical heating of resonant nanostructures is one of the key issues in modern nanophotonics, being either harmful or desirable effect depending on the applications. Despite a linear regime of light-to-heat conversion is well-studied both for metal and semiconductor resonant systems generalized as critical coupling condition, the clear strategy to optimize optical heating upon high-intensity light irradiation is still missing. In this work, we propose a simple analytical model for such problem taking into account material properties changes caused by the heating. It allows us to derive a new ge…
Photoluminescence (PL) phenomenon from metallic nanostructures has been explained and understood by several point of views. One of them is based on the classic harmonic oscillator model, which describes PL of single mode. In this study, we continue to expand this classic model to a coupling case, which involves two oscillators that interact with each other together with the excitation electric field. The new generated modes due to the coupling are carefully analyzed, including their behaviors varying with the coupling coefficients in different cases. Furthermore, for practical purpose, PL spec…
Recently, a new device to measure the Orbital Angular Momentum (OAM) electronic spectrum after elastic/inelastic scattering in a transmission electron microscope has been introduced. We modified the theoretical framework needed to describe conventional low loss electron energy loss spectroscopy (EELS) experiments in transmission electron microscopes (TEM) to study surface plasmons in metallic nanostructures, to allow for an OAM post selection and devise new experiments for the analysis of these excitations in nanostructures. We found that unprecedented information on the symmetries and on the …
Plasmonic excitations such as surface-plasmon-polaritons (SPPs) and graphene-plasmons (GPs), carry large momenta and are thus able to confine electromagnetic fields to small dimensions. This property makes them ideal platforms for subwavelength optical control and manipulation at the nanoscale. The momenta of these plasmons are even further increased if a scheme of metal-insulator-metal and graphene-insulator-metal are used for SPPs and GPs, respectively. However, with such large momenta, their far-field excitation becomes challenging. In this work, we consider hybrids of graphene and metallic…
We investigate - both experimentally and theoretically - the inelastic interaction between fast electrons and the electromagnetic field scattered by metallic apertures and nanostructures on dielectric membranes using photon induced near-field electron microscopy. The experiments - performed in a high brightness ultrafast transmission electron microscope - on gold apertures on silicon nitride membranes reveal strong modulations of the electron-light coupling strength. We demonstrates that this effect results from the combined action of the electric field scattered by the aperture edges and the …
This paper has presented inversely determining the resonant configuration of the bilateral nanostructures for periodic metallic slits with extraordinary optical transmission performance. The topology optimization approach is utilized to implement the inverse design procedure. Several geometrical configurations of the bilateral nanostructures are derived for periodic metallic slits. The resonant performance of the derived nanostructures are demonstrated by the transmission spectra, where the transmission peak is presented at the specified wavelength in the inverse design procedure. This provide…
The interaction of light with metallic nanostructures produces a collective excitation of electrons at the metal surface, also known as surface plasmons. These collective excitations lead to resonances that enable the confinement of light in deep-subwavelength regions, thereby leading to large near-field enhancements. The simulation of plasmon resonances presents notable challenges. From the modeling perspective, the realistic behavior of conduction-band electrons in metallic nanostructures is not captured by Maxwell's equations, thus requiring additional modeling. From the simulation perspect…
In this work, we report numerical simulations and experiments of the optical response of a gold nanostrip embedded in a silicon strip waveguide gap at telecom wavelengths. We show that the spectral features observed in transmission and reflection when the metallic nanostructure is inserted in the gap are extremely different to those observed in free-space excitation. First, we find that interference between the guided field and the electric dipolar resonance of the metallic nanostructure results in high-contrast (> 10) spectral features showing an asymmetric Fano spectral profile. Secondly, we…
Quantum hydrodynamic theory (QHT) can describe some of the characteristic features of quantum electron dynamics that appear in metallic nanostructures, such as spatial nonlocality, electron spill-out, and quantum tunneling. Furthermore, numerical simulations based on QHT are more efficient than fully quantum mechanical approaches, as exemplified by time-dependent density functional theory using a jellium model. However, QHT involves kinetic energy functionals, the practical implementation of which typically induces significant numerical instabilities, particularly in nonlinear optical phenomen…
We investigate an efficient two-photon up-conversion process in more than one molecule coupled to an optical antenna. In the previous work [Y. Osaka et al., PRL 112, 133601 (2014)], we considered the two-photon up-conversion process in a single molecule within one-dimensional input-output theory, and revealed that controlling the antenna-molecule coupling enables the efficient up-conversion with radiative loss in the antenna suppressed. In this work, aiming to propose a way to enhance the total probability of antenna-photon scattering, we extend the model to the case of multiple molecules. In …
The ability of metallic nanostructures to confine light at the sub-wavelength scale enables new perspectives and opportunities in the field of nanotechnology. Making use of this unique advantage, nano-optical trapping techniques have been developed to tackle new challenges in a wide range of areas from biology to quantum optics. In this work, starting from basic theories, we present a review of research progress in near-field optical manipulation techniques based on metallic nanostructures, with an emphasis on some of the most promising advances in molecular technology, such as the precise con…
Fourier modal method and coordinate transformation method under nonclassical electromagnetic boundary condition for the electromagnetism of mesoscale metallic nanostructures
Controlled integration of metallic nanoparticles (NPs) onto photonic nanostructures enables realization of complex devices for extreme light confinement and enhanced light-matter interaction. This can be achieved combining Nanoparticle-on-Mirror (NPoM) nanocavities with the light manipulation capabilities of micron-scale metallic antennas and/or photonic integrated waveguides. However, metallic nanoparticles are usually deposited via drop-casting, which prevents their accurate positioning. Here we present a methodology for precise transfer and positioning of individual NPs onto different photo…
A thermostat senses the temperature of a physical system and switches heating or cooling devices on or off, regulating the flow of heat to maintain the system's temperature near a desired setpoint. Taking advantage of recent advances in radiative heat transfer technologies, here we propose a passive radiative "thermostat" based on phase-change photonic nanostructures for thermal regulation at room temperature. By self-adjusting their visible to mid-IR absorptivity and emissivity responses depending on the ambient temperature, the proposed devices use the sky to passively cool or heat during da…
Characteristic Mode Analysis of Composite Nanostructures using a Coupled System of Volume Integral and Hydrodynamic Equations
King Abdullah University of Science and Technology (KAUST)（阿卜杜拉国王科技大学）；University of Electronic Science and Technology of China (UESTC)（电子科技大学）；Light Academy College of Engineering（光学院工程学院）
We demonstrate theoretically that ultrafast heating of metal nanoparticles by the laser pulse should lead to the generation of coherent terahertz (THz) radiation during the heat redistribution process. It is shown that after the femtosecond laser pulse action the time-dependent gradient of the electronic temperature induces low-frequency particle polarization with the characteristic timescale of about fractions of picosecond. In the case of the directed metallic pattern, the THz pulse waveform can be controlled by changing geometry of the individual particle. The generation mechanism proposed …
Hot charge carrier extraction from metallic nanostructures is a very promising approach for applications in photo-catalysis, photovoltaics and photodetection. One limitation is that many metallic nanostructures support a single plasmon resonance thus restricting the light-to-charge-carrier activity to a spectral band. Here we demonstrate that a monolayer of plasmonic nanoparticles can be assembled on a multi-stack layered configuration to achieve broad-band, near-unit light absorption, which is spatially localised on the nanoparticle layer. We show that this enhanced light absorbance leads to …
Effect of 1-D photonic crystals on optical transmission of VO2 is studied by depositing thin films of VO2 nanoparticles on SiO2/TiO2 distributed Bragg reflectors (DBR) in the near infrared (IR) spectrum as per earlier theoretical predictions of J. Phys. D: Appl. Phys. 51 375102 (2018). Monoclinic VO2 nanoparticles with tuned crystallinity were synthesized by a facile solution processing method. Moderately crystalline (MC) and highly crystalline (HC) VO2 nanostructures were obtained by varying its synthesis temperature and post growth annealing conditions. Both MC VO2 and HC VO2 films exhibit e…
