Dissipation of electromagnetic energy through absorption is a fundamental process that underpins phenomena ranging from photovoltaics to photography, analytical spectroscopy, photosynthesis, and human vision. Absorption is also a dynamic process that depends on the duration of the optical illumination. Here we report on the resonant plasmonic absorption of a nanostructured metamaterial and the non-resonant absorption of an unstructured gold film at different optical pulse durations. By examining the absorption in travelling and standing waves, we observe a plasmonic relaxation time of 11 fs as the characteristic transition time. The metamaterial acts as a beam-splitter with low absorption for shorter pulses, while as a good absorber for longer pulses. The transient nature of the absorption puts a frequency limit of ~90 THz on the bandwidth of coherently-controlled, all-optical switching devices, which is still a thousand times faster than other leading switching technologies.
Dewetting of thin metal films is one of the most widespread method for functional plasmonic nanostructures fabrication. However, simple thermal-induced dewetting does not allow to control degree of nanostructures order without additional lithographic process steps. Here we propose a novel method for lithography-free and large-scale fabrication of plasmonic nanostructures via controllable femtosecond laser-induced dewetting. The method is based on femtosecond laser surface pattering of a thin film followed by a nanoscale hydrodynamical instability, which is found to be very controllable under s…
Nanoscale pulsed light is highly desirable in nano-integrated optics. In this letter, we obtained femtosecond pulses with THz repetition frequency via the strong coupling between quantum emitters (QEs) and plasmonic resonators. Our structure consists of a V-groove (VG) plasmonic resonator and a nanowire embedded with two-level QEs. The influences of the incident light intensity and QE number density on the transmission response for this hybrid system are investigated through semi-classical theory and simulation. It is found that the transmission response can be modulated to the pulse form. The…
We explore the nonlinear response of plasmonic materials driven by ultrashort pulses of electromagnetic radiation with temporal duration of few femtoseconds and high peak intensity. By developing the Fokker-Planck-Landau theory of electron collisions, we solve analytically the collisional integral and derive a novel set of hydrodynamical equations accounting for plasma dynamics at ultrashort time scales. While in the limit of small light intensities we recover the well established Drude model of plasmas, in the high intensity limit we observe nonlinear quenching of collision-induced damping le…
Raman spectroscopic characterization of crater walls formed upon single-shot high energy femtosecond laser irradiation of dimethacrylate polymer doped with plasmonic gold nanorods
Nanosphere-on-mirror plasmonic antennas, each having a monolayer graphene or MoS2 sheet in the gap, were pumped with a femtosecond laser. Abrupt turnings in the scattering linewidth and peak intensity trends as the laser power changed were experimentally observed. Theoretical modelling of dynamic plasmon evolvement attributes the turning to transitioning between two plasmon states, with a universal switching threshold of four-wave mixing efficiency around 0.14%. This bistability is rendered by a strong feedback from the nonlinear gap current to the gap plasmons, and involvement of both four an…
We demonstrate polarization controlled absorption in plasmonic bimetallic metamaterials. We fabricate and experimentally characterize Au/Ni ring resonator arrays, where by varying the wavelength and polarization of the incident wave, local electromagnetic fields and dissipation can be suppressed or enhanced in the Au and Ni areas of the rings.
We investigate the scattering and absorption properties of anisotropic metal-dielectric core-shell nanoparticles. It is revealed that the radially anisotropic dielectric layer can accelerate the evanescent decay of the localized resonant surface modes, leading to Q-factor and absorption rate enhancement. Moreover, the absorption cross section can be maximized to reach the single resonance absorption limit. We further show that such artificial anisotropic cladding materials can be realized by isotropic layered structures, which may inspire many applications based on scattering and absorption of…
Plasmonics can be used to improve absorption in optoelectronic devices and has been intensively studied for solar cells and photodetectors. Graphene has recently emerged as a powerful plasmonic material. It shows significantly less losses compared to traditional plasmonic materials such as gold and silver and its plasmons can be tuned by changing the Fermi energy with chemical or electrical doping. Here we propose the usage of graphene plasmonics for light trapping in optoelectronic devices and show that the excitation of localized plasmons in doped, nanostructured graphene can enhance optical…
Absorption induced transparency is an optical phenomenon that occurs in metallic arrays of nanoholes when materials featuring narrow lines in their absorption spectra are deposited on top of it. First reported in the visible range, using dye lasers as cover materials, it has been described as transmission peaks unexpectedly close to the absorption energies of the dye laser. In this work, amplification of light is demonstrated in the active regime of absorption induced transparency. Amplification of stimulated emission can be achieved when the dye laser behaves as a gain material. Intense illum…
A quantum mechanical approach and local response theory are applied to study plasmons propagating in nanometer-thin gold slabs sandwiched between different dielectrics. The metal slab supports two different kinds of modes, classified as long-range and short-range plasmons. Quantum spill-out is found to significantly increase the imaginary part of their mode indices, and, surprisingly, even for slabs wide enough to approach bulk the increase is 20%. This is explained in terms of enhanced plasmonic absorption, which mainly takes place at narrow peaks located near the slab surface.
We propose a new concept for generation of ultrashort pulses based on transient plasmonic resonance in nanoparticle composites. Photoionization and free-carriers plasma change the susceptibility of nanoparticles on a few-femtosecond scale. This results in a narrow time window during the pump pulse duration when the system is in plasmonic resonance, accompanied by a short burst of the local field. During this process, frequency-tunable few-fs pulses are generated. We elucidate the details of the above mechanism, and investigate the influences of different contributing processes.
Exploiting the dynamics of Plasmonic Parametric Resonance (PPR), we introduce the theory of Plasmonic Parametric Absorbers (PPA). The key insight informing the PPA idea is that in the PPR process a pump field experiences an extinction rate that strongly depends on the intensity of the pump itself, creating two distinct regimes: one of weak absorption under low intensity illumination, and one of strong absorption when the threshold of parametric resonance is met or exceeded. Due to this reverse saturable absorption behavior, PPAs are promising candidates for optical limiting applications.
By combining analytical and numerical approaches, we theoretically investigate the effect of fabrication imperfections, e.g. roughness at metal interfaces, on nanometer metal-insulator-metal waveguides supporting slow gap-plasmon modes. Realistic devices with vapor deposition- and chemically-grown metal films are considered. We obtain quantitative predictions for the attenuations induced by absorption and by backscattering, and analytically derive how both attenuations scale with respect to the group velocity. Depending on the material parameters and fabrication quality, roughness-induced back…
Femtosecond spectroscopy is an important tool for tracking rapid photoinduced processes in a variety of materials. To spatially map the processes in a sample would substantially expand the capabilities of the method. This is, however, difficult to achieve due to the necessity to use low-noise detection and to maintain feasible data acquisition time. Here we demonstrate realization of an imaging pump-probe setup, featuring sub-100 fs temporal resolution, by a straightforward modification of a standard pump-probe technique, using a randomly structured probe beam. The structured beam, made by a d…
We present experimental evidence of plasmonic-enhanced optical tweezers, of polystyrene beads in deionized water in the vicinity of metal-coated nanostructures. The optical tweezers operate with a continuous wave (CW) near-infrared laser. We employ a Cu/Au bilayer that significantly improves dissipation of heat generated by the trapping laser beam and avoid de-trapping from heat convection currents. We investigate the improvement of the optical trapping force, the effective trapping quality factor, and observe an exponential distance dependence of the trapping force from the nanostructures, ex…
A plasmonic nanoantenna probed by a plane-polarized optical field in a medium with no gain materials can show zero absorption or even amplification, while exhibiting maximal polarizability. This occurs through coupling to an adjacent nanoantenna in a specially designed metamolecule, which is pumped by an orthogonal optical field with phase shift. The introduced scheme is a classical counterpart of an effect known in quantum optics as enhancement of the index of refraction (EIR). In contrary to electromagnetically induced transparency (EIT), where the medium is rendered highly dispersive at the…
We propose a scheme to realize nonlinear coherent perfect absorption (CPA) at the nanoscale using epsilon-near-zero (ENZ) plasmonic waveguides. The general conditions to achieve CPA in a linear ENZ plasmonic waveguide are analyzed and presented. The proposed ENZ waveguides support an effective ENZ response at their cut-off frequency, where the CPA effect occurs under the illumination of two counter-propagating plane waves with equal amplitudes and appropriate phase distributions. In addition, the strong and uniform field enhancement inside the nanochannels of the waveguides at the ENZ resonanc…
The theory of energy transfer dynamics of a pair of donor and acceptor molecules located in the plasmonic hot spots is developed by means of the master equation approach and the electromagnetic Green's tensor technique. A nonlocal effect has been considered by using a hydrodynamic model. The coherent interaction between the two molecules in plasmonic nanostructures is investigated under some strong coupling conditions. It is shown that the energy transfer efficiency of a pair of molecules can be improved largely and the transfer time decreases to dozens of femtoseconds when the contribution of…
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 the nonlinear radiations can be 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 transported by the propagating surface plasmon at excitation frequency, enabling thereby polariton-mediate…
We experimentally demonstrate the coherent control, i.e., phase-dependent enhancement and suppression, of the optical absorption in an array of metallic nanoantennas covered by a thin lu- minescent layer. The coherent control is achieved by using two collinear, counter-propagating and phase-controlled incident waves with wavelength matching the absorption spectrum of dye molecules coupled to the array. Symmetry arguments shed light on the relation between the relative phase of the incident waves and the excitation efficiency of the optical resonances of the system. This coherent control is ass…
The electromagnetic response of subwavelength wires coated with a graphene monolayer illuminated by a linearly polarized plane waves is investigated. The results show that the scattering and extintion cross-sections of the coated wire can be dramatically enhanced when the incident radiation resonantly excites localized surface plasmons. The enhancements occur for p--polarized incident waves and for excitation frequencies that correspond to complex poles in the coefficients of the multipole expansion for the scattered field. By dynamically tuning the chemical potential of graphene, the spectral…
In this paper, we proposed a theoretical model in the far-infrared and terahertz (THz) bands, which is a dumbbell-shaped graphene metamaterial arrays with a combination of graphene nanorod and two semisphere-suspended heads. We report a detailed theoretical investigation on how to enhance localized electric field and the absorption in the dumbbell-shaped graphene metamaterial arrays. The simulation results show that by changing the geometrical parameters of the structure and the Fermi level of graphene, we can change the absorption characteristics. Furthermore, we have discovered that the reso…
Power dissipation in electromagnetic absorbers is a quadratic function of the incident fields. To characterize an absorber, one needs to deal with the coupling that may occur between different excitations. Energy Absorption Interferometry (EAI) is a technique that highlights the independent degrees of freedom through which a structure can absorb energy: the natural absorption modes of the structure. The coupling between these modes vanishes. In this paper, we use the EAI formalism to analyse different kinds of plasmonic periodic absorbers while rigorously accounting for the coupling: resonant …
Exceptional broadband absorption of nanoporous gold explained by plasmonic resonances at dangling ligaments
Hamburg University of Technology（汉堡工业大学）；Institute of Optical and Electronic Materials, Hamburg University of Technology（汉堡工业大学光学与电子材料研究所）；Helmholtz-Zentrum Geesthacht（赫尔姆霍茨盖斯特哈赫特中心）；Institute of Functional Materials for Sustainability, Helmholtz-Zentrum Geesthacht（赫尔姆霍茨盖斯特哈赫特中心可持续功能材料研究所）
Fundamental upper bounds are given for the plasmonic multipole absorption and scattering of a rotationally invariant dielectric sphere embedded in a lossy surrounding medium. A specialized Mie theory is developed for this purpose and when combined with the corresponding generalized optical theorem, an optimization problem is obtained which is explicitly solved by straightforward analysis. In particular, the absorption cross section is a concave quadratic form in the related Mie (scattering) parameters and the convex scattering cross section can be maximized by using a Lagrange multiplier const…
Research on multimode optical fibers is arousing a growing interest, for their capability to transport high-power laser beams, coupled with novel nonlinear optics-based applications. However, when beam intensities exceed a certain critical value, optical fiber breakdown associated with irreversible modifications of their refractive index occurs, triggered by multiphoton absorption. These processes have been largely exploited for fiber material microstructuration. Here we show that, for intensities slightly below the breakdown threshold, nonlinear absorption strongly affects the dynamics of a p…
Ultra-short pulses with high repetition frequency have great application prospects in the field of nano-optics. Here, in the case of continuous wave incidence, the femtosecond pulses with THz repetition frequency are achieved in the transmission system consisting of a rectangular cavity, a V-groove (VG) cavity and a nanowire embedded with quantum emitters (QEs). The generation mechanism of the ultra-short pulses with high repetition frequency is elucidated by semi-classical Dicke model. Attribute to the presence of the two-level QEs, the field amplitude in plasmonic resonator is oscillating wi…
Recently, plasmonic nanofluids (i.e., a suspension of plasmonic nanoparticles in a base fluid) have been widely employed in direct-absorption solar collectors because the localized surface plasmon supported by plasmonic nanoparticles can greatly improve the direct solar thermal conversion performance. Considering that the surface plasmon resonance frequency of metallic nanoparticles, such as gold, silver, and aluminum, is usually located in the ultraviolet to visible range, the absorption coefficient of a plasmonic nanofluid must be spectrally tuned for full utilization of the solar radiation …
Recently, asymmetric plasmonic nanojunctions [Karnetzky et. al., Nature Comm. 2471, 9 (2018)] have shown promise as on-chip electronic devices to convert femtosecond optical pulses to current bursts, with a bandwidth of multi-terahertz scale, although yet at low temperatures and pressures. Such nanoscale devices are of great interest for novel ultrafast electronics and opto-electronic applications. Here, we operate the device in air and at room temperature, revealing the mechanisms of photoemission from plasmonic nanojunctions, and the fundamental limitations on the speed of optical-to-electro…
We demonstrate a way to coherently control light at the nanoscale and achieve coherent perfect absorption (CPA) by using epsilon-near-zero (ENZ) plasmonic waveguides. The presented waveguides support an effective ENZ response at their cut-off frequency, combined with strong and homogeneous field enhancement along their nanochannels. The CPA conditions are perfectly satisfied at the ENZ frequency, surprisingly by a subwavelength plasmonic structure, resulting in strong CPA under the illumination of two counter-propagating plane waves with appropriate amplitudes and phases. In addition , we inve…
Despite more than a decade of active research, the fundamental problem of material loss remains a major obstacle in fulfilling the promise of the recently emerged fields of metamaterials and plasmonics to bring in revolutionary practical applications. In the present work, we demonstrate that the problem of strong material absorption that is inherent to plasmonic systems and metamaterials based on plasmonic components, can be addressed by utilizing the time dimension. By matching the pulse profile to the actual response of a lossy metamaterial, this approach allows to offset the effect of the m…
Surface plasmon resonance (SPR) has been widely utilized to improve the absorption performance in the photosensors. Graphene has emerged as a promising plasmonic material, which supports tunable SPR and shows significant flexibility over metals. In this letter, a hybrid photosensor based on the integration of periodic cross-shaped graphene arrays with an ultrathin light-absorbing semiconductor is proposed. A tenfold absorption enhancement over a large range of the incidence angle for both light polarizations as well as a considerably high photogeneration rate ($\sim10^{37}$) is demonstrated at…
We demonstrate an unexpectedly strong surface-plasmonic absorption at the interface of silver and high-index dielectrics based on electron and photon spectroscopy. The measured bandwidth and intensity of absorption deviate significantly from the classical theory. Our density-functional calculation well predicts the occurrence of this phenomenon. It reveals that due to the low metal-to-dielectric work function at such interfaces, conduction electrons can display a drastic quantum spillover, causing the interfacial electron-hole pair production to dominate the decay of surface plasmons. This fin…
One of the technical barriers impeding the wide applications of integrated photonic circuits is the lack of ultracompact, high speed, broadband electro-optical (EO) modulators, which up-convert electronic signals into high bit-rate photonic data. In addition to direct modulation of lasers, EO modulators can be classified into (i) phase modulation based on EO effect or free-carrier injection, or (ii) absorption modulation based on Franz-Keldysh effect or quantum-confined Stark effect. Due to the poor EO properties of regular materials, a conventional EO modulator has a very large footprint. Bas…
Nonlinear absorption of femtosecond laser pulses provides a unique opportunity to confine energy deposition in any medium to a region that is below the focal diameter of a pulse. Illumination of a polymer film through a transparent high bandgap material such as glass, followed by nonlinear absorption of 800 nm light in polymers, allows us to further restrict absorption to a very thin layer along the propagation direction. We demonstrate this confinement by simulating femtosecond-laser-induced polymer modification by linear, two-photon and three-photon absorption, and discuss the control over e…
The rapidly developing field of plasmonics can be roughly categorized into two branches: surface plasmon polaritons (SPPs) propagating in plasmonic waveguides and localized surface plasmons (LSPs) supported by scattering plasmonic particles. Investigations along these two directions usually employ quite different approaches and techniques, resulting in more or less a dogma that the two branches progress almost independently of each other, with few interactions. Here in this work we interpret LSPs from a Bohr model based geometric perspective relying on SPPs, thus establishing a connection betw…
Synthetic perovskites with photovoltaic properties open a new era in solar photovoltaics. Due to high optical absorption perovskite-based thin-film solar cells are usually considered as fully absorbing solar radiation on condition of ideal blooming. However, is it really so? The analysis of the literature data has shown that the absorbance of all photovoltaic pervoskites has the spectral hole at infrared frequencies where the solar radiation spectrum has a small local peak. This absorption dip results in the decrease of the optical efficiency of thin-film pervoskite solar cells by nearly 3% an…
Scattering from metal nanoparticles near their localized plasmon resonance; especially, the resonances of noble metals which are mostly in the visible or infrared part of the electromagnetic spectrum; is a way of improving light absorption in thin-film solar cells. The surface plasmon resonance can be affected by different factors such as the type, size, shape, and dielectric properties of the surrounding medium. Here we investigate, using the Finite Difference Time Domain (FDTD) method, how different shapes of aluminum nanoparticles affect absorption enhancement in silicon thin-film solar cel…
Herein, we investigate the optical properties of quantum plasmonic metasurfaces composed of metallic nano-objects with subnanometer gaps according to the time-dependent density functional theory, a fully quantum mechanical approach. When the quantum and classical descriptions are compared, the transmission, reflection, and absorption rates of the metasurface exhibit substantial differences at shorter gap distances. The differences are caused by electron transport through the gaps of the nano-objects. The electron transport has profound influences for gap distances less-than or approximately 0.…
Plasmonic nanoresonators of core-shell composition and nanorod shape were optimized to tune their absorption cross-section maximum to the central wavelength of a short pulse. Their distribution along a pulse-length scaled target was optimized to maximize the absorptance with the criterion of minimal absorption difference in between neighbouring layers. Successive approximation of layer distributions made it possible to ensure almost uniform deposited energy distribution up until the maximal overlap of two counter-propagating pulses. Based on the larger absorptance and smaller uncertainty in ab…
