Abstract
We investigate the nonlinear optical properties of gold nanoparticle pairs. Two excitation beams of frequencies ω1 and ω2 are used to induce nonlinear polarizations at the junction of a particle dimer. Nonlinearities of the second and third order can be controllably induced as a function of the dimer geometry, leading predominantly to second-harmonic generation (SHG), sum frequency generation (SFG) and four-wave mixing (4WM). Due to their center symmetry, dimers with identical particle diameters give rise to a very weak second-order response, without affecting the third-order response. Therefore, a sharp probe functionalized with a symmetric metal dimer acts as a nanoscale photon source emitting narrow-band photons of frequency 2ω1 − ω2. We demonstrate that this source can be employed as a near-field optical probe for high-resolution fluorescence imaging.
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