Large-Area 3D Chiral Plasmonic Structures

Frank, Bettina; Yin, Xinghui; Schäferling, Martin; Zhao, Jun; Hein, Sven M.; Braun, Paul V.; Gießen, Harald

doi:10.1021/nn402370x

Cited by 270 publications

(273 citation statements)

References 51 publications

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“…Three-dimensional chiral geometries exhibit strong responses to polarization and a geometry that cannot be superimposed upon itself as discussed, for example, in Refs [21,22]. The existence of two-dimensional chirality in plasmonic structures has sometimes been debated, because even thin nanostructures-such as the nanospirals in our experiment, which have an aspect ratio of order 16-are not rigorously planar.…”

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confidence: 91%

Efficient forward second-harmonic generation from planar archimedean nanospirals

et al. 2015

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Abstract:The enhanced electric field at plasmonic resonances in nanoscale antennas can lead to efficient harmonic generation, especially when the plasmonic geometry is asymmetric on either inter-particle or intra-particle levels. The planar Archimedean nanospiral offers a unique geometrical asymmetry for second-harmonic generation (SHG) because the SHG results neither from arranging centrosymmetric nanoparticles in asymmetric groupings, nor from non-centrosymmetric nanoparticles that retain a local axis of symmetry. Here, we report forward SHG from planar arrays of Archimedean nanospirals using 15 fs pulses from a Ti:sapphire oscillator tuned to 800 nm wavelength. The measured harmonic-generation efficiencies are 2.6·10 −9 , 8·10 −9 and 1.3·10 −8 for left-handed circular, linear, and right-handed circular polarizations, respectively. The uncoated nanospirals are stable under average power loading of as much as 300 µW per nanoparticle. The nanospirals also exhibit selective conversion between polarization states. These experiments show that the intrinsic asymmetry of the nanospirals results in a highly efficient, two-dimensional harmonic generator that can be incorporated into metasurface optics.Keywords: nonlinear plasmonics, asymmetric nanoparticles, polarization conversion, metasurfaces, near-field enhancement, Archimedean nanospirals The second-order susceptibility governs a host of important nonlinear optical phenomena, including frequency mixing, sum-frequency and harmonic generation, and optical rectification. In crystalline and molecular materials, second-order nonlinearities are nonvanishing only at surfaces or in materials with a noncentrosymmetric crystal structure; moreover, the efficient generation of a second-order nonlinear effect requires that the fundamental incident and the nonlinear outgoing waves be phase matched through a macroscopic volume of material, typically on the order of cubic millimeters [1].Plasmonic nanostructures and nanostructure arrays also exhibit second-order nonlinearities, and can generate forward second harmonics if their geometries are not centrosymmetric. Such structures are inherently planar, and therefore compatible with thin-film optical and optoelectronic technologies and with metasurface optics. With advances in nanofabrication, the symmetry of the structures can be exquisitely controlled at the level of a few nanometers [2]. Combining these effects with ultrafast, high-intensity laser pulses yields massive electricfield enhancements and correspondingly greater secondharmonic yield. The localized surface plasmon resonance enhances efficiency and can be designed by selecting the nanoparticle shape for a given wavelength; selective polarization response can also be designed into the nanoparticle. A number of asymmetric plasmonic geometries have been used for harmonic generation, including L-and V-shaped nanoparticles, nanocups, and asymmetric trimers [3][4][5][6][7]. Larger plasmonic structures-such as the ratchet wheel-have also been shown to affect the polarization o...

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Efficient forward second-harmonic generation from planar archimedean nanospirals

et al. 2015

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“…The most intuitive approach to obtain large chiroptical activity is by forming nanoparticles with an actual chiral shape such as a gammadion or a helix. This has been achieved by lithographic methods [18][19][20] . Recently, there have been several reports on the preparation of chiral inorganic nanostructures through non-lithographic methods: Liedl and colleagues 21 formed chiral plasmonic shapes using DNA Origami.…”

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confidence: 99%

Enantioselective control of lattice and shape chirality in inorganic nanostructures using chiral biomolecules

et al. 2014

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A large number of inorganic materials form crystals with chiral symmetry groups. Enantioselectively synthesizing nanostructures of such materials should lead to interesting optical activity effects. Here we report the synthesis of colloidal tellurium and selenium nanostructures using thiolated chiral biomolecules. The synthesis conditions are tuned to obtain tellurium nanostructures with chiral shapes and large optical activity. These nanostructures exhibit visible optical and chiroptical responses that shift with size and are successfully simulated by an electromagnetic model. The model shows that they behave as chiral optical resonators. The chiral tellurium nanostructures are transformed into chiral gold and silver telluride nanostructures with very large chiroptical activity, demonstrating a simple colloidal chemistry path to chiral plasmonic and semiconductor metamaterials. These materials are natural candidates for studies related to interactions of chiral (bio)molecules with chiral inorganic surfaces, with relevance to asymmetric catalysis, chiral crystallization and the evolution of homochirality in biomolecules.

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“…However, these structures need oblique incidence of light to discriminate polarizations with opposite handedness and also exhibit weak dichroic selection. To maximize the interaction with light, chiral metamaterials should extrude along the third dimension, that is, by a stacked arrangement of a unit cell (quasi-three-dimensional (3D) objects) [10][11][12][13][14][15] . In particular, fully 3D helix-based metamaterials can be considered as the best candidates for pronounced chiral response integrated in compact devices, as demonstrated by the fully 3D helical metamaterials acting as circular polarizers in the infrared range 2 , and realized by direct laser writing.…”

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Triple-helical nanowires by tomographic rotatory growth for chiral photonics

et al. 2015

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Three dimensional helical chiral metamaterials resulted in effective manipulation of circularly polarized light in the visible infrared for advanced nanophotonics. Their potentialities are severely limited by the lack of full rotational symmetry preventing broadband operation, high signal-to-noise ratio and inducing high optical activity sensitivity to structure orientation. Complex intertwined three dimensional structures such as multiple-helical nanowires could overcome these limitations, allowing the achievement of several chiro-optical effects combining chirality and isotropy. Here we report three dimensional triple-helical nanowires, engineered by the innovative tomographic rotatory growth, on the basis of focused ion beam-induced deposition. These three dimensional nanostructures show up to 37% of circular dichroism in a broad range (500-1,000 nm), with a high signal-to-noise ratio (up to 24 dB). Optical activity of up to 8°only due to the circular birefringence is also shown, tracing the way towards chiral photonic devices that can be integrated in optical nanocircuits to modulate the visible light polarization.

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Large-Area 3D Chiral Plasmonic Structures

Cited by 270 publications

References 51 publications

Efficient forward second-harmonic generation from planar archimedean nanospirals

Efficient forward second-harmonic generation from planar archimedean nanospirals

Enantioselective control of lattice and shape chirality in inorganic nanostructures using chiral biomolecules

Triple-helical nanowires by tomographic rotatory growth for chiral photonics

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