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Register a new userSecond-harmonic generation from coupled plasmon modes in a single dimer of gold nanospheres
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We show that a dimer made of two gold nanospheres exhibits a remarkable efficiency for second-harmonic generation under femtosecond optical excitation. The detectable nonlinear emission for the given particle size and excitation wavelength arises when the two nanoparticles are as close as possible to contact, as in situ controlled and measured using the tip of an atomic force microscope. The excitation wavelength dependence of the second-harmonic signal supports a coupled plasmon resonance origin with radiation from the dimer gap. This nanometer-size light source might be used for high-resolution near-field optical microscopy.
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The selective optical detection of individual metallic nanoparticles (NPs) with high spatial and temporal resolution is a challenging endeavour, yet is key to the understanding of their optical response and their exploitation in applications from miniaturised optoelectronics and sensors to medical diagnostics and therapeutics. However, only few reports on ultrafast pump-probe spectroscopy on single small metallic NPs are available to date. Here, we demonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy in heterodyne detection to resolve for the first time the ultrafast changes of real and imaginary part of the dielectric function of single small (<40nm) spherical gold NPs. The results are quantitatively described via the transient electron temperature and density in gold considering both intraband and interband transitions at the surface plasmon resonance. This novel microscopy technique enables background-free detection of the complex susceptibility change even in highly scattering environments and can be readily applied to any metal nanostructure.
Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Apart from suggesting an approach for directional enhancement of nonlinear response in plasmonic systems, we anticipate that our findings can be used as a rapid and non-destructive method for characterization of crystal quality and orientation that may be of significant importance in future applications.
A hallmark of wave-matter duality is the emergence of quantum-interference phenomena when an electronic transition follows different trajectories. Such interference results in asymmetric absorption lines such as Fano resonances, and gives rise to secondary effects like electromagnetically induced transparency (EIT) when multiple optical transitions are pumped. Few solid-state systems show quantum interference and EIT, with quantum-well intersubband transitions in the IR offering the most promising avenue to date to devices exploiting optical gain without inversion. Quantum interference is usually hampered by inhomogeneous broadening of electronic transitions, making it challenging to achieve in solids at visible wavelengths and elevated temperatures. However, disorder effects can be mitigated by raising the oscillator strength of atom-like electronic transitions - excitons - which arise in monolayers of transition-metal dichalcogenides (TMDCs). Quantum interference, probed by second-harmonic generation (SHG), emerges in monolayer WSe2, without a cavity, splitting the SHG spectrum. The splitting exhibits spectral anticrossing behaviour, and is related to the number of Rabi flops the strongly driven system undergoes. The SHG power-law exponent deviates strongly from the canonical value of 2, showing a Fano-like wavelength dependence which is retained at room temperature. The work opens opportunities in solid-state quantum-nonlinear optics for optical mixing, gain without inversion and quantum-information processing.
The generation process of second harmonic (SH) radiation from holes periodically arranged on a metal surface is investigated. Three main modulating factors affecting the optical response are identified: the near-field distribution at the wavelength of the fundamental harmonic, how SH light couples to the diffraction orders of the lattice, and its propagation properties inside the holes. It is shown that light generated at the second harmonic can excite electromagnetic modes otherwise inaccessible in the linear regime under normal incidence illumination. It is demonstrated that the emission of SH radiation is only allowed along off-normal paths precisely due to that symmetry. Two different regimes are studied in the context of extraordinary optical transmission, where enhanced linear transmission either occurs through localized electromagnetic modes or is aided by surface plasmon polaritons (SPPs). While localized resonances in metallic hole arrays have been previously investigated, the role played by SPPs in SH generation has not been addressed so far. In general, good agreement is found between our calculations (based on the finite difference time domain method) and the experimental results on localized resonances, even though no free fitting parameters were used in describing the materials. It is found that SH emission is strongly modulated by enhanced fields at the fundamental wavelength (either localized or surface plasmon modes) on the glass metal interface. This is so in the transmission side but also in reflection, where emission can only be explained by an efficient tunneling of SH photons through the holes from the output to the input side. Finally, the existence of a dark SPP at the fundamental field is identified through a noninvasive method for the first time, by analyzing the efficiency and far-field pattern distribution in transmission at the second harmonic.
The second-order nonlinear optical susceptibility $Pi^{(2)}$ for second harmonic generation is calculated for gapped graphene. The linear and second-order nonlinear plasmon excitations are investigated in context of second harmonic generation (SHG). We report a red shift and an order of magnitude enhancement of the SHG resonance with growing gap, or alternatively, reduced electro-chemical potential.
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