Journal
NATURE NANOTECHNOLOGY
Volume 10, Issue 5, Pages 412-417Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NNANO.2015.69
Keywords
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Funding
- Fondazione Cariplo through the project SHAPES [2013-0736]
- EC through the Graphene Flagship project [CNECT-ICT-604391]
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Boosting nonlinear frequency conversion in extremely confined volumes remains a challenge in nano-optics research(1), but can enable applications in nanomedicine(2), photocatalysis(3) and background-free biosensing(4). To obtain brighter nonlinear nanoscale sources, approaches that enhance the electromagnetic field intensity and counter the lack of phase matching in nanoplasmonic systems are often employed(5-8). However, the high degree of symmetry in the crystalline structure of plasmonic materials (metals in particular) and in nanoantenna designs strongly quenches second harmonic generation(5). Here, we describe doubly-resonant single-crystalline gold nanostructures with no axial symmetry(9) displaying spatial mode overlap at both the excitation and second harmonic wavelengths. The combination of these features allows the attainment of a nonlinear coefficient for second harmonic generation of similar to 5 x 10(-10) W-1, enabling a second harmonic photon yield higher than 3 x 10(6) photons per second. Theoretical estimations point toward the use of our nonlinear plasmonic nanoantennas as efficient platforms for label-free molecular sensing.
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