Dispersive ground plane core-shell type optical monopole antennas fabricated with electron beam induced deposition.

We present the bottom-up fabrication of dispersive silica core, gold cladding ground plane optical nanoantennas. The structures are made by a combination of electron-beam induced deposition of silica and sputtering of gold. The antenna lengths range from 300 to 2100 nm with size aspect ratios as large as 20. The angular emission patterns of the nanoantennas are measured with angle-resolved cathodoluminescence spectroscopy and compared with finite-element methods. Good overall correspondence between the the measured and calculated trends is observed. The dispersive nature of these plasmonic monopole antennas makes their radiation profile highly tunable.

Reversible polarization control of single photon emission.

We present reversible and a-priori control of the polarization of a photon emitted by a single molecule by introducing a nanoscale metal object in its near field. It is experimentally shown that, with the metal close to the emitter, the polarization ratio of the emission can be varied by a factor of 2. The tunability of polarization decays, when the metal is displaced by typically 30 nm. Calculations based on the multiple multipole method agree well with our experiments and predict even further enhancement with a suitable nanoantenna design.

Enhanced nonlinear optical effects with a tapered plasmonic waveguide.

Infrared surface plasmon polaritons (SPPs) are concentrated in a laterally tapered planar Ag waveguide. The near field of SPPs excited with 1490 nm light at a Ag-sapphire interface is probed using the photoluminescence of upconverted Er ions at 550 and 660 nm. SPP interference patterns are observed that exhibit clear evidence of SPP concentration toward the taper end. The concentration leads to an enhancement of the upconversion luminescence intensity from Er energy levels that are populated by multiphoton processes.

Lambda/4 resonance of an optical monopole antenna probed by single molecule fluorescence.

We present a resonant optical nanoantenna positioned at the end of a metal-coated glass fiber near-field probe. Antenna resonances, excitation conditions, and field localization are directly probed in the near field by single fluorescent molecules and compared to finite integration technique simulations. It is shown that the antenna is equivalent to its radio frequency analogue, the monopole antenna. For the right antenna length and local excitation conditions, antenna resonances occur that lead to an enhanced localized field near the antenna apex. Direct mapping of this field with single fluorescent molecules reveals a spatial localization of 25 nm, demonstrating the importance of such antennas for nanometer resolution optical microscopy.

Exciton polaritons confined in a ZnO nanowire cavity.

Semiconductor nanowires of high purity and crystallinity hold promise as building blocks for miniaturized optoelectrical devices. Using scanning-excitation single-wire emission spectroscopy, with either a laser or an electron beam as a spatially resolved excitation source, we observe standing-wave exciton polaritons in ZnO nanowires at room temperature. The Rabi splitting between the polariton branches is more than 100 meV. The dispersion curve of the modes in the nanowire is substantially modified due to light-matter interaction. This finding forms a key aspect in understanding subwavelength guiding in these nanowires.

Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems.

We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.

Probing the negative permittivity perfect lens at optical frequencies using near-field optics and single molecule detection.

Recently, the existence of a perfect lens has been predicted, made of an artificial material that has a negative electric permittivity and a negative magnetic permeability. For optical frequencies a poormans version is predicted to exist in the sub-wavelength limit. Then, only the permittivity has to be negative, a demand that metals fulfill at optical frequencies. We propose a new measurement scheme to verify the performance of such a negative permittivity near-perfect lens at optical frequencies. The scheme is based on near-field scanning optical microscopy and single molecule detection. Prerequisite near-field single molecule data, necessary to assess the performance of the lens, is presented. A numerical evaluation, which includes absorption, of the expected performance of a slab of a realistic negative permittivity material confirms the merits of the scheme.

Local probing of Bloch mode dispersion in a photonic crystal waveguide.

The local dispersion relation of a photonic crystal waveguide is directly determined by phase-sensitive near-field microscopy. We readily demonstrate the propagation of Bloch waves by probing the band diagram also beyond the first Brillouin zone. Both TE and TM polarized modes were distinguished in the experimental band diagram. Only the TE polarized defect mode has a distinctive Bloch wave character. The anomalous dispersion of this defect guided mode is demonstrated by local measurements of the group velocity. The measured dispersion relation and measured group velocities are both in good agreement with theoretical calculations.

Segment dynamics in thin polystyrene films probed by single-molecule optics.

Single fluorescent molecules (represented by spheres with a volume equal to the actual van der Waals volume of the molecule) has been embedded in a polystyrene matrix (left). Such molecules act as probes for the study of polymer nanoscale (segmental scale) dynamics in thin films deposited on a glass cover slide (right).

Beta-cyclodextrin host-guest complexes probed under thermodynamic equilibrium: thermodynamics and AFM force spectroscopy.

The rupture forces of individual host-guest complexes between beta-cyclodextrin (beta-CD) heptathioether monolayers on Au(111) and several surface-confined guests were measured in aqueous medium by single molecule force spectroscopy using an atomic force microscope. Anilyl, toluidyl, tert-butylphenyl, and adamantylthiols (0.2-1%) were immobilized in mixed monolayers with 2-mercaptoethanol on gold-coated AFM tips. For all guests and for all surface coverages, the force-displacement curves measured between the functionalized tips and monolayers of beta-CD exhibited single, as well as multiple, pull-off events. The histograms of the pull-off forces showed several maxima at equidistant forces, with force quanta characteristic for each guest of 39 +/- 15, 45 +/- 15, 89 +/- 15, and 102 +/- 15 pN, respectively. These force quanta were independent of the loading rate, indicating that, because of the fast complexation/decomplexation kinetics, the rupture forces were probed under thermodynamic equilibrium. The force values followed the same trend as the free binding energy Delta G degrees measured for model guest compounds in solution or on beta-CD monolayers, as determined by microcalorimetry and surface plasmon resonance measurements, respectively. A descriptive model was developed to correlate quantitatively the pull-off force values with the Delta G degrees of the complexes, based on the evaluation of the energy potential landscape of tip-surface interaction.