Adiabatic nanofocusing on ultrasmooth single-crystalline gold tapers creates a 10-nm-sized light source with few-cycle time resolution.

We demonstrate adiabatic nanofocusing of few-cycle light pulses using ultrasharp and ultrasmooth single-crystalline gold tapers. We show that the grating-induced launching of spectrally broad-band surface plasmon polariton wavepackets onto the shaft of such a taper generates isolated, point-like light spots with 10 fs duration and 10 nm diameter spatial extent at its very apex. This nanofocusing is so efficient that nanolocalized electric fields inducing strong optical nonlinearities at the tip end are reached with conventional high repetition rate laser oscillators. We use here the resulting second harmonic to fully characterize the time structure of the localized electric field in frequency-resolved interferometric autocorrelation measurements. Our results strongly suggest that these nanometer-sized ultrafast light spots will enable new experiments probing the dynamics of optical excitations of individual metallic, semiconducting, and magnetic nanostructures.

Probing the Ca(2+) switch of the neuronal Ca(2+) sensor GCAP2 by time-resolved fluorescence spectroscopy.

We report fluorescence lifetime and rotational anisotropy measurements of the fluorescent dye Alexa647 attached to the guanylate cyclase-activating protein 2 (GCAP2), an intracellular myristoylated calcium sensor protein operating in photoreceptor cells. By linking the dye to different protein regions critical for monitoring calcium-induced conformational changes, we could measure fluorescence lifetimes and rotational correlation times as a function of myristoylation, calcium, and position of the attached dye, while GCAP2 was still able to regulate guanylate cyclase in a Ca(2+)-sensitive manner. We observe distinct site-specific variations in the fluorescence dynamics when externally changing the protein conformation. A clear reduction in fluorescence lifetime suggests that in the calcium-free state a dye marker in amino acid position 131 senses a more hydrophobic protein environment than in position 111. Saturating GCAP2 with calcium increases the fluorescence lifetime and hence leads to larger exposure of position 111 to the solvent and at the same time to a movement of position 131 into a hydrophobic protein cleft. In addition, we find distinct, biexponential anisotropy decays reflecting the reorientational motion of the fluorophore dipole and the dye/protein complex, respectively. Our experimental data are well described by a "wobbling-in-a-cone" model and reveal that for dye markers in position 111 of the GCAP2 protein both addition of calcium and myristoylation results in a pronounced increase in orientational flexibility of the fluorophore. Our results provide evidence that the up-and-down movement of an α-helix that is situated between position 111 and 131 is a key feature of the dynamics of the protein-dye complex. Operation of this piston-like movement is triggered by the intracellular messenger calcium.

Superfocusing of electric or magnetic fields using conical metal tips: effect of mode symmetry on the plasmon excitation method.

We compare single- and double-sided excitation methods of adiabatic surface plasmon polariton (SPP) wave superfocusing for scattering-type metallic near-field scanning optical microscopy (s-NSOM). Using the results of full 3D finite difference time domain analyses, the differences in field enhancement factors are explained and reveal the mode selectivity of a conical NSOM tip for adiabatic SPP superfocusing. Exploiting the mode-symmetric nature of the tip further, we also show that it is possible to selectively confine either the electric or magnetic field at the NSOM tip apex, by simply adjusting the relative phase between the SPP waves in the double-sided excitation approach.

Adiabatic nanofocusing scattering-type optical nanoscopy of individual gold nanoparticles.

We explore imaging of local electromagnetic fields in the vicinity of metallic nanoparticles using a grating-coupled scattering-type near-field scanning optical microscope. In this microscope, propagating surface plasmon polariton wavepackets are launched onto smooth gold tapers where they are adiabatically focused toward the nanometer-sized taper apex. We report two-dimensional raster-scanned optical images showing pronounced near-field contrast and demonstrating sub-30 nm resolution imaging of localized surface plasmon polariton fields of spherical and elliptical nanoparticles. By comparison to three-dimensional finite-difference time domain simulations, we conclude that virtually background-free near-field imaging is achieved. The microscope combines deep subwavelength resolution, high local field intensities and a straightforward imaging contrast, making it interesting for a variety of applications in linear and nonlinear nanospectroscopy.