Molecular Fluctuations as a Ruler of Force-Induced Protein Conformations.

Molecular fluctuations directly reflect the underlying energy landscape. Variance analysis examines protein dynamics in several biochemistry-driven approaches, yet measurement of probe-independent fluctuations in proteins exposed to mechanical forces remains only accessible through steered molecular dynamics simulations. Using single molecule magnetic tweezers, here we conduct variance analysis to show that individual unfolding and refolding transitions occurring in dynamic equilibrium in a single protein under force are hallmarked by a change in the protein's end-to-end fluctuations, revealing a change in protein stiffness. By unfolding and refolding three structurally distinct proteins under a wide range of constant forces, we demonstrate that the associated change in protein compliance to reach force-induced thermodynamically stable states scales with the protein's contour length increment, in agreement with the sequence-independent freely jointed chain model of polymer physics. Our findings will help elucidate the conformational dynamics of proteins exposed to mechanical force at high resolution which are of central importance in mechanosensing and mechanotransduction.

Modal Coupling of Single Photon Emitters Within Nanofiber Waveguides.

Nanoscale generation of individual photons in confined geometries is an exciting research field aiming at exploiting localized electromagnetic fields for light manipulation. One of the outstanding challenges of photonic systems combining emitters with nanostructured media is the selective channelling of photons emitted by embedded sources into specific optical modes and their transport at distant locations in integrated systems. Here, we show that soft-matter nanofibers, electrospun with embedded emitters, combine subwavelength field localization and large broadband near-field coupling with low propagation losses. By momentum spectroscopy, we quantify the modal coupling efficiency identifying the regime of single-mode coupling. These nanofibers do not rely on resonant interactions, making them ideal for room-temperature operation, and offer a scalable platform for future quantum information technology.

Percolating plasmonic networks for light emission control.

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.

Multipolar interference for directed light emission.

By directing light, optical antennas can enhance light-matter interaction and improve the efficiency of nanophotonic devices. Here we exploit the interference among the electric dipole, quadrupole, and magnetic dipole moments of a split-ring resonator to experimentally realize a compact directional optical antenna. This single-element antenna design robustly directs emission even when covered with nanometric emitters at random positions, outperforming previously demonstrated nanoantennas with a bandwidth of 200 nm and a directivity of 10.1 dB from a subwavelength structure. The advantages of this approach bring directional optical antennas closer to practical applications.

Plasmonic antennas as design elements for coherent ultrafast nanophotonics.

Broadband excitation of plasmons allows control of light-matter interaction with nanometric precision at femtosecond timescales. Research in the field has spiked in the past decade in an effort to turn ultrafast plasmonics into a diagnostic, microscopy, computational, and engineering tool for this novel nanometric-femtosecond regime. Despite great developments, this goal has yet to materialize. Previous work failed to provide the ability to engineer and control the ultrafast response of a plasmonic system at will, needed to fully realize the potential of ultrafast nanophotonics in physical, biological, and chemical applications. Here, we perform systematic measurements of the coherent response of plasmonic nanoantennas at femtosecond timescales and use them as building blocks in ultrafast plasmonic structures. We determine the coherent response of individual nanoantennas to femtosecond excitation. By mixing localized resonances of characterized antennas, we design coupled plasmonic structures to achieve well-defined ultrafast and phase-stable field dynamics in a predetermined nanoscale hotspot. We present two examples of the application of such structures: control of the spectral amplitude and phase of a pulse in the near field, and ultrafast switching of mutually coherent hotspots. This simple, reproducible and scalable approach transforms ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid-state physics, and quantum biology.

Aluminum for nonlinear plasmonics: resonance-driven polarized luminescence of Al, Ag, and Au nanoantennas.

Resonant optical antennas are ideal for nanoscale nonlinear optical interactions due to their inherent strong local field enhancement. Indeed second- and third-order nonlinear response of gold nanoparticles has been reported. Here we compare the on- and off-resonance properties of aluminum, silver, and gold nanoantennas, by measuring two-photon photoluminescence. Remarkably, aluminum shows 2 orders of magnitude higher luminescence efficiency than silver or gold. Moreover, in striking contrast to gold, the aluminum emission largely preserves the linear incident polarization. Finally, we show the systematic resonance control of two-photon excitation and luminescence polarization by tuning the antenna width and length independently. Our findings point to aluminum as a promising metal for nonlinear plasmonics.