Interference between Selected Dipoles and Octupoles in the Optical Second-Harmonic Generation from Spherical Gold Nanoparticles

Butet, Jérémy; Bachelier, Guillaume; Russier‐Antoine, Isabelle; Jonin, Christian; Bénichou, Emmanuel; Brevet, P. F.

doi:10.1103/physrevlett.105.077401

Cited by 143 publications

(145 citation statements)

References 23 publications

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“…These results are in agreement with experimental |SHG-CD| values equal in the range of 20 %, taking into account that the resultant SHG originates from a coherent mixture of the discussed microscopic sources. In the case of gold, the surface normal contribution is commonly assumed to be dominant over the two other tangential and bulk sources [18,31,41]. Among them, the bulk contribution may be more or less important, depending on whether the metal is formed as a thin film or as a nanoparticle.…”

Section: Shg Scattering Simulationsmentioning

confidence: 99%

Octupolar Plasmonic Meta-Molecules for Nonlinear Chiral Watermarking at Subwavelength Scale

et al. 2015

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Nonlinear chiroptical effects of precisely designed chiral plasmonic nanomaterials can be much stronger than such effects observed in the linear regime. We take advantage of this property to demonstrate the use of circularly polarized second-harmonic generation microscopy towards the efficient read-out of a microscopic pattern encoded by an array of triangular gold nanoprisms forming arrangements of adequate chiral symmetry. Strong chiroptical effects are observed in the backscattered second-harmonic generation intensity, enabling clear distinction of the laterally arranged enantiomers, down to nearly 1 µm resolution with an overall intensity contrast of about 40 % (second-harmonic generation circular dichroism of 20 %). Numerical simulations show a noticeable change in the spatial distribution of plasmonic hot spots within the individual nanostructures under excitation by circularly polarized light of different handedness. This leads to rather weak chiroptical effect in the linear backscattering (theoretical circular dichroism not exceeding 3 %), in contrast with the much more significant change of the second-harmonic generation in the far-field (secondharmonic generation circular dichroism from 16 up to 37%). These results open the possibility of designing deeply subwavelength chiral nanostructures for encoding microscopic "watermarks", which cannot be easily accessed by linear optical methods, moreover requiring a nonlinear microscopy set-up for reading out the encoded pattern. Graphic Over the past two decades, research devoted to the second-harmonic generation (SHG) from plasmonic nanostructures evolved from the investigation of hyper-Rayleigh scattering in colloidal suspensions of metal nanoparticles [1-3] towards the measurements of SHG from individual plasmonic nano-objects [4][5][6]. Far-field SHG radiation pattern has been demonstrated as a highly sensitive probe of the nanoscale optical field distribution [7], allowing for the investigation of multipolar plasmon modes [8][9][10], the analysis of surface plasmon polariton (SPP)-mediated interactions [11,12], refractive index sensing [13] and precise characterization of the nanostructure geometry [14][15][16]. In parallel, advanced theoretical tools for SHG modelling were developed, based on numerical methods such as finite elements to solve Maxwell equations and yield the scattered SHG radiation [17][18][19]. Among the geometrical properties that can be addressed by SHG microscopy, chirality stands-out as one of the most interesting probes of light-matter interactions, especially in the context of chiral plasmonic meta-materials which have been reported to exhibit giant optical activity in the linear regime [20,21]. Valev et al. have thus reported extensive work on chirality in SHG from specially patterned superchiral meta-surfaces [7,[22][23][24]. The location of plasmonic hot spots and their influence on the chiroptical response have been thoroughly addressed [22,23], leading to reports of nonlinear chiroptical effects reaching magnitudes as high as 5...

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Section: Shg Scattering Simulationsmentioning

confidence: 99%

Octupolar Plasmonic Meta-Molecules for Nonlinear Chiral Watermarking at Subwavelength Scale

et al. 2015

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“…These enhancements find a practical application in tip-enhanced SHG scanning near-field microscopy [24], in further enhancing the SHG in nonlinear optical materials, such as GaAs [25] and in the possibility to detect single nanoparticles [26][27]. From the fundamental point of view, the local field enhanced SHG allows the study of contributions to the signal from physical mechanisms that are typically very small, namely multipolar contributions to the SHG [28][29][30] or electric dipole contributions from the bulk [31]. Additionally, the plasmonic mechanisms themselves, such as coupling between the charge oscillations, can be studied in the SHG enhanced signal [32][33][34][35].…”

Section: Introductionmentioning

confidence: 99%

The role of chiral local field enhancements below the resolution limit of Second Harmonic Generation microscopy

Valev¹,

Clercq²,

Zheng³

et al. 2011

Opt. Express

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Abstract:While it has been demonstrated that, above its resolution limit, Second Harmonic Generation (SHG) microscopy can map chiral local field enhancements, below that limit, structural defects were found to play a major role. Here we show that, even below the resolution limit, the contributions from chiral local field enhancements to the SHG signal can dominate over those by structural defects. We report highly homogeneous SHG micrographs of star-shaped gold nanostructures, where the SHG circular dichroism effect is clearly visible from virtually every single nanostructure. Most likely, size and geometry determine the dominant contributions to the SHG signal in nanostructured systems. References and links1. J. B. Pendry, "A chiral route to negative refraction," Science 306(5700), 1353-1355 (2004 1983-1986 (1983). 7. T. Petralli-Mallow, T. M. Wong, J. D. Byers, H. I. Yee, and J. M. Hicks, "Circular dichroism spectroscopy at interfaces: a surface second harmonic generation study," J. Phys. Chem. 97(7), 1383-1388 (1993). 8. P. Fischer and F. Hache, "Nonlinear optical spectroscopy of chiral molecules," Chirality 17(8), 421-437 (2005).

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“…28,29 Furthermore, polarization resolved hyper-Rayleigh scattering has been shown to allow for a straightforward separation between even and odd mode contributions to the SH scattered wave. 40,41 …”

Section: Theoretical Methodsmentioning

confidence: 99%

Universal scaling of plasmon coupling in metal nanostructures: Checking the validity for higher plasmonic modes using second harmonic generation

et al. 2013

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The universal scaling of plasmon coupling in metallic nanostructures is now a well-established feature. However, if the interaction between dipolar plasmon modes has been intensively studied, this is not the case of the coupling between higher order ones. Using Mie theory extended to second harmonic generation, we investigate the coupling between quadrupolar plasmon modes in metallic nanoshells. Like in the case of dipolar plasmon modes, a universal scaling behavior is observed in agreement with the plasmon hybridization model.

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Interference between Selected Dipoles and Octupoles in the Optical Second-Harmonic Generation from Spherical Gold Nanoparticles

Cited by 143 publications

References 23 publications

Octupolar Plasmonic Meta-Molecules for Nonlinear Chiral Watermarking at Subwavelength Scale

Octupolar Plasmonic Meta-Molecules for Nonlinear Chiral Watermarking at Subwavelength Scale

The role of chiral local field enhancements below the resolution limit of Second Harmonic Generation microscopy

Universal scaling of plasmon coupling in metal nanostructures: Checking the validity for higher plasmonic modes using second harmonic generation

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