Enhanced second-harmonic generation from double resonant plasmonic antennae

Thyagarajan, K.; Rivier, S.; Lovera, Andrea; Martin, Olivier J. F.

doi:10.1364/oe.20.012860

Cited by 242 publications

(224 citation statements)

References 27 publications

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“…The DRA, a nanoantenna composed of three arms (two small arms and one long arm) and made of aluminum, 72 is a good example of such multiresonant nanostructures for nonlinear plasmonics, Figure 1c. 42 Following the previous approach developed for the Al DA, the intensity enhancement in the gaps when the DRA is driven by a planewave, and the enhancement of the dipole radiation has been evaluated using the SIE method, Figure 5 and Table 2. As expected, an enhancement of the intensity in both gaps is observed for wavelengths close to λ = 400 and 800 nm.…”

Section: ■ Numerical Methodsmentioning

confidence: 99%

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

Butet

Martin

2015

J. Phys. Chem. C

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The plasmon enhancement of molecular hyperRaman scattering, the nonlinear counterpart of Raman scattering, which involves the absorption of two fundamental photons, is investigated with emphasis on low energy molecular vibrations. The two-photon excitation of the molecule is treated using its hyperpolarizability β, and the emission of the hyperRaman photons is computed using a dipole emitter located at the molecule position. The electromagnetic response of the plasmonic systems is evaluated using a surface integral equation method, which makes possible considering both planewave and dipole excitations in a single formalism. Taking into account different geometries (including multiresonant antennas and silver heptamers supporting Fano resonances), the experimental parameters influencing the enhancement of the molecular hyperRaman scattering are discussed in detail. In particular, it is shown that a good excitation at the fundamental stage is not sufficient for reaching a good enhancement factor and that an optimization of the electromagnetic response of the plasmonic substrate is also important at the emission wavelength. The competition between the molecular hyper-Raman scattering signal and the background signal, that is, the second harmonic generation, is discussed. The latter can be reduced in specific structures by taking advantages of the key role played by the symmetry of the structure for hyper-Raman scattering and second harmonic generation. This way, we propose a nanostructure where the second harmonic generation can be reduced in the detection direction, enabling the hyper-Raman scattering signal from single donor−acceptor "push−pull" chromophores to be experimentally recorded with a low noise level using surface-enhanced hyper-Raman scattering. It is particularly remarkable that the hyper-Raman signal from one molecule can be stronger than the second harmonic generation from a complete plasmonic nanostructure, despite the considerable volume difference between both nano-objects. This fundamental observation stems from the different selection rules for both nonlinear optical processes.

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Section: ■ Numerical Methodsmentioning

confidence: 99%

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

Butet

Martin

2015

J. Phys. Chem. C

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“…The DRA based on double resonances both at the fundamental and second harmonic produces a 1.5 stronger SHG intensity than the DA (see Figure 4). 16 This finite improvement is due to the additional resonance at the second harmonic wavelength. The silver heptamer has more gaps where the field is enhanced and therefore even off-Fano resonance, exhibits a 2.7 times stronger SHG as compared to the DA.…”

Section: * S Supporting Informationmentioning

confidence: 99%

Augmenting Second Harmonic Generation Using Fano Resonances in Plasmonic Systems

2013

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Significant augmentation of second harmonic generation using Fano resonances in plasmonic heptamers made of silver is theoretically and experimentally demonstrated. The geometry is engineered to simultaneously produce a Fano resonance at the fundamental wavelength, resulting in a strong localization of the fundamental field close to the system, and a higher order scattering peak at the second harmonic wavelength. These results illustrate the versatility of Fano resonant structures to engineer specific optical responses both in the linear and nonlinear regimes thus paving the way for future investigations on the role of dark modes in nonlinear and quantum optics. 1 One such property is the generation of hot spots, whose presence in nanostructures, such as optical antennae, is promising for applications in nonlinear optics, since they require a strong electric near-field.2 Recent studies have reported the observation of different nonlinear optical phenomena in such nanosystems, like, for example, second harmonic generation (SHG), 3 multiphoton luminescence, 4,5 third harmonic generation, 6,7 higher harmonic generation, 8 and four-wave mixing. 9 SHG is significantly dependent on the symmetry of both the material being used and the structure being studied and therefore is a sensitive tool for characterizing plasmonic structures.10−13 SHG from centrosymmetric materials is due to the breaking of inversion symmetry at their surfaces and is therefore used as a surface probe.14 In recent years, strong SHG has been observed in metallic nanostructures such as sharp metallic tips, 15 multiple resonant nanostructures, 16,17 split-ring resonators, 18 metamaterials 19,20 and nanocups, 21 underlining the fast growing interest in the area of nonlinear plasmonics. 22,23 Efficient SHG requires the presence of strong SHG sources, that is, nonlinear polarization currents oscillating at the second harmonic frequency, at the nanostructure surface as well as an efficient scattering of the SHG signal into the far-field. Several strategies have been developed to enhance SHG from metallic nanostructures including using multiple resonances at both the fundamental and the second harmonic wavelengths, 16 breaking the centrosymmetry using noncentrosymmetric nanostructures 20 and even enhancing the electric fields using nanogaps. 24 However, the efficiency of SHG is restricted by two fundamental classes of losses that electromagnetic waves suffer in such metallic structures, namely radiative "losses" like optical scattering and nonradiative losses like the generation of heat. 25 Therefore, to increase the detected SHG in the far-field the structures must decrease the radiative losses at the fundamental wavelength while increasing them at the second harmonic wavelength and at the same time increase the near-field at the fundamental wavelength. Because the SHG yield increases as the square of the fundamental field intensity, 26 a higher near-field at the fundamental is required to increase the near-field at the second harmonic. The wid...

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“…As can be seen in Fig. 2, the Fano lineshape 09012-p. 2 can be tuned to exhibit a strong dip in the case of strong coupling or a weak dip in the case of weak coupling. It is possible to show that the ideal regime where the intensity enhancement is the strongest while maintaining low radiative and non-radiative losses occurs when the structures are fabricated such that the , that is, the radiative and non-radiative losses are equal [4].…”

Section: Simulationsmentioning

confidence: 99%

“…Second harmonic generation (SHG) is one such important nonlinear optical effect which has the added advantage of being sensitive to symmetry. In earlier works, we proposed and tested the possibility to enhance SHG from nanostructures using Fano resonances [1], or double-resonant plasmonic antennae [2]. In this work, we propose to study the influence of the plasmon damping time -both radiative and non-radiativeat the fundamental frequency on the intensity enhancement at the second harmonic.…”

Section: Introductionmentioning

confidence: 99%

Influencing the ultrafast plasmon damping time using Fano resonances for nonlinear plasmonics

Thyagarajan

Martin

2013

EPJ Web of Conferences

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Enhanced second-harmonic generation from double resonant plasmonic antennae

Cited by 242 publications

References 27 publications

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

Augmenting Second Harmonic Generation Using Fano Resonances in Plasmonic Systems

Influencing the ultrafast plasmon damping time using Fano resonances for nonlinear plasmonics

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