Dr. Jan Renger

Optical nanoantennas have revolutionised the way we manipulate single photons emitted by individual light sources in a nanostructured photonic environment. Complex plasmonic architectures allow for multiscale light control by shortening or stretching the light wavelength for a fixed operating frequency, meeting the size of the emitter and that of propagating modes. Here, we study self-assembled semi-continuous gold films and lithographic gold networks characterised by large local density of optical state (LDOS) fluctuations around the electrical percolation threshold, a regime where the surface is characterised by large metal clusters with fractal topology. We study the formation of plasmonic networks and their effect on light emission from embedded fluorescent probes in these systems. Through fluorescence dynamics experiments we discuss the role of global long-range interactions linked to the degree of percolation and to the network fractality, as well as the local near-field contributions coming from the local electro-magnetic fields and the topology. Our experiments indicate that local properties dominate the fluorescence modification.

Nanoantennae show potential for photosynthesis research for two reasons; first by spatially confining light for experiments which require high spatial resolution, and second by enhancing the photon emission of single light-harvesting complexes. For effective use of nanoantennae a detailed understanding of the interaction between the nanoantenna and the light-harvesting complex is required. Here we report how the excitation and emission of multiple purple bacterial LH2s (light-harvesting complex 2) are controlled by single gold nanorod antennae. LH2 complexes were chemically attached to such antennae, and the antenna length was systematically varied to tune the resonance with respect to the LH2 absorption and emission. There are three main findings. (i) The polarization of the LH2 emission is fully controlled by the resonant nanoantenna. (ii) The largest fluorescence enhancement, of 23 times, is reached for excitation with light at lambda = 850 nm, polarized along the long antenna-axis of the resonant antenna. The excitation enhancement is found to be 6 times, while the emission efficiency is increased 3.6 times. (iii) The fluorescence lifetime of LH2 depends strongly on the antenna length, with shortest lifetimes of ~40 ps for the resonant antenna. The lifetime shortening arises from an 11 times resonant enhancement of the radiative rate, together with a 2–3 times increase of the non-radiative rate, compared to the off-resonant antenna. The observed length dependence of radiative and non-radiative rate enhancement is in good agreement with simulations. Overall this work gives a complete picture of how the excitation and emission of multi-pigment light-harvesting complexes are influenced by a dipole nanoantenna.

Here is your text with all HTML and paragraph breaks removed, and without changing the original wording:<br><br>The nature of the highly efficient energy transfer in photosynthetic light-harvesting complexes is a subject of intense research. Unfortunately, the low fluorescence efficiency and limited photostability hampers the study of individual light-harvesting complexes at ambient conditions. Here we demonstrate an over 500-fold fluorescence enhancement of light-harvesting complex 2 (LH2) at the single-molecule level by coupling to a gold nanoantenna. The resonant antenna produces an excitation enhancement of circa 100 times and a fluorescence lifetime shortening to ~20 ps. The radiative rate enhancement results in a 5.5-fold-improved fluorescence quantum efficiency. Exploiting the unique brightness, we have recorded the first photon antibunching of a single light-harvesting complex under ambient conditions, showing that the 27 bacteriochlorophylls coordinated by LH2 act as a non-classical single-photon emitter. The presented bright antenna-enhanced LH2 emission is a highly promising system to study energy transfer and the role of quantum coherence at the level of single complexes.

Label-free biosensing based on metallic nanoparticles supporting localized surface plasmon resonances (LSPR) has recently received growing interest (Anker, J. N., et al. Nat. Mater.2008, 7, 442–453). Besides its competitive sensitivity (Yonzon, C. R., et al. J. Am. Chem. Soc.2004, 126, 12669–12676; Svendendahl, M., et al. Nano Lett.2009, 9, 4428–4433) when compared to the surface plasmon resonance (SPR) approach based on extended metal films, LSPR biosensing features a high-end miniaturization potential and a significant reduction of the interrogation device bulkiness, positioning itself as a promising candidate for point-of-care diagnostic and field applications. Here, we present the first, paralleled LSPR lab-on-a-chip realization that goes well beyond the state-of-the-art, by uniting the latest advances in plasmonics, nanofabrication, microfluidics, and surface chemistry. Our system offers parallel, real-time inspection of 32 sensing sites distributed across 8 independent microfluidic channels with very high reproducibility/repeatability. This enables us to test various sensing strategies for the detection of biomolecules. In particular we demonstrate the fast detection of relevant cancer biomarkers (human alpha-feto-protein and prostate specific antigen) down to concentrations of 500 pg/mL in a complex matrix consisting of 50% human serum.

Nanopositioning of single quantum emitters to control their coupling to integrated photonic structures is a crucial step in the fabrication of solid-state quantum optics devices. We use the optical near-field enhancement produced by nanofabricated gold antennas subject to near-infrared illumination to deterministically trap and position single nanodiamonds (NDs) hosting nitrogen-vacancy (NV) centers. The positioning of the NDs at the antenna regions of maximum field intensity is first characterized using both fluorescence and electron microscopy imaging. We further study the interaction between the nanoantenna and the delivered NV center by analyzing its change in fluorescence lifetime, which is driven by the increase in the local density of optical states at the trapping positions. Additionally, the plasmonic enhancement of the near-field intensity allows us to optically control the NV excited lifetime using relatively low NIR illumination intensities, some 20 times lower than in the absence of the antennas.

Recent advances in nanotechnologies have prompted the need for tools to accurately and non-invasively manipulate individual nano-objects. Among the possible strategies, optical forces have been predicted to provide researchers with nano-optical tweezers capable of trapping a specimen and moving it in three dimensions. In practice, however, the combination of weak optical forces and photothermal issues has thus far prevented their experimental realization. Here, we demonstrate the first three-dimensional optical manipulation of single 50 nm dielectric objects with near-field nanotweezers. The nano-optical trap is built by engineering a bowtie plasmonic aperture at the extremity of a tapered metal-coated optical fibre. Both the trapping operation and monitoring are performed through the optical fibre, making these nanotweezers totally autonomous and free of bulky optical elements. The achieved trapping performances allow for the trapped specimen to be moved over tens of micrometres over a period of several minutes with very low in-trap intensities. This non-invasive approach is foreseen to open new horizons in nanosciences by offering an unprecedented level of control of nanosized objects, including heat-sensitive biospecimens.

The ultrafast coherent control of light localization in resonant plasmonic nanostructures is intricately related to the phase response of the involved plasmon resonances. In this work, we exploit the second harmonic signal generated by single optical nanoantennas subject to broadband phase-controlled femtosecond pulses to study and tailor the coherent resonance response. Our results reveal that both the spectral phase and the amplitude components associated with the plasmon resonance of arbitrary individual nanoantennas can be accurately determined.