Nonlinear chiral imaging of subwavelength-sized twisted-cross gold nanodimers [Invited]

Huttunen, Mikko J.; Bautista, Godofredo; Decker, Manuel; Lindén, Stefan; Wegener, Martin; Kauranen, Martti

doi:10.1364/ome.1.000046

Cited by 70 publications

(66 citation statements)

References 61 publications

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“…Fabrication variations in individual structures can indeed play a nontrivial role in the SHG from plasmonic nanostructures. 13,45 In summary, the SHG from a Fano resonant system has been studied both theoretically and experimentally. The nonlinear SHG in the engineered silver heptamers is shown to be significantly stronger when utilizing the generation of a high near-field at the fundamental wavelength by reducing scattering losses, while assuring a strong scattering at the second harmonic.…”

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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Section: * S Supporting Informationmentioning

confidence: 99%

Augmenting Second Harmonic Generation Using Fano Resonances in Plasmonic Systems

2013

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“…Overcoming this major obstacle would lead to novel functional materials based on the control of both electric and magnetic material responses at optical frequencies, namely, to negative refractive index [10][11][12] , chirality [13][14][15][16][17][18] and subwavelength imaging 19 as well as to compact nanolasers and spasers 20,21 . Finally, active metamaterials might also enter new, unexplored areas such as quantum metamaterials [22][23][24] .…”

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Dual-channel spontaneous emission of quantum dots in magnetic metamaterials

et al. 2013

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Metamaterials, artificial electromagnetic media realized by subwavelength nano-structuring, have become a paradigm for engineering electromagnetic space, allowing for independent control of both electric and magnetic responses of the material. Whereas most metamaterials studied so far are limited to passive structures, the need for active metamaterials is rapidly growing. However, the fundamental question on how the energy of emitters is distributed between both (electric and magnetic) interaction channels of the metamaterial still remains open. Here we study simultaneous spontaneous emission of quantum dots into both of these channels and define the control parameters for tailoring the quantum-dot coupling to metamaterials. By superimposing two orthogonal modes of equal strength at the wavelength of quantum-dot photoluminescence, we demonstrate a sharp difference in their interaction with the magnetic and electric metamaterial modes. Our observations reveal the importance of mode engineering for spontaneous emission control in metamaterials, paving a way towards loss-compensated metamaterials and metamaterial nanolasers.

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“…The experimental study is performed with second harmonic generation (SHG) microscopy, a technique whose usefulness for visualizing fi eld enhancements in nanostructures has been demonstrated in several works already. [22][23][24][25][26][27] We use ultrafast pulsed lasers ( ∼ 100 fs, 82 MHz), which are capable of delivering very high electric fi eld intensities to the electron population in the nanostructures. When the intense electric fi eld of light becomes comparable with the electric near-fi elds, the oscillations of the electron density are driven in the nonlinear (anharmonic) regime.…”

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Distributing the Optical Near‐Field for Efficient Field‐Enhancements in Nanostructures

et al. 2012

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Circularly polarized light imparts a sense of rotation on the electron density in ring‐shaped gold nanostructures. As a consequence, the near‐field enhancement becomes homogeneous on the surface of the nanostructures, thereby increasing the opportunity for interaction with molecules. This type of nanostructured samples can find a broad range of applications in chemical processes where the interaction between molecules and local field enhancements play an important role.

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Nonlinear chiral imaging of subwavelength-sized twisted-cross gold nanodimers [Invited]

Cited by 70 publications

References 61 publications

Augmenting Second Harmonic Generation Using Fano Resonances in Plasmonic Systems

Augmenting Second Harmonic Generation Using Fano Resonances in Plasmonic Systems

Dual-channel spontaneous emission of quantum dots in magnetic metamaterials

Distributing the Optical Near‐Field for Efficient Field‐Enhancements in Nanostructures

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