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.
Highlights
It has been almost two centuries since Jean-Baptiste Biot discovered the interaction of chiral materials and polarized light
We report highly homogeneous Second Harmonic Generation (SHG) micrographs of star-shaped gold nanostructures, where the SHG circular dichroism effect is clearly visible from virtually every single nanostructure
Size and geometry determine the dominant contributions to the SHG signal in nanostructured systems
Summary
It has been almost two centuries since Jean-Baptiste Biot discovered the interaction of chiral materials and polarized light. The capability of mapping chiral local field enhancements is lost below the resolution limit of SHG microscopy; where, recently, it has been reported that, in ~300 nm large gold nanodimers at λ = 1060 nm, structural defects play an important role [43]. Structural defects, such as bumps, pits and other small-scale structural deviations [44], are well known sources of SHG enhancement [45,46] and it has been proposed that they contribute through effective higher order multipoles [47,48]. We should start by saying that our nanostructures differ both in size and in shape from those that were studied in [32] and [44]
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