Investigation of the Influence of Wound-Treatment-Relevant Buffer Systems on the Colloidal and Optical Properties of Gold Nanoparticles.

Biocompatible gold nanoparticles (AuNPs) are used in wound healing due to their radical scavenging activity. They shorten wound healing time by, for example, improving re-epithelialization and promoting the formation of new connective tissue. Another approach that promotes wound healing through cell proliferation while inhibiting bacterial growth is an acidic microenvironment, which can be achieved with acid-forming buffers. Accordingly, a combination of these two approaches appears promising and is the focus of the present study. Here, 18 nm and 56 nm gold NP (Au) were prepared with Turkevich reduction synthesis using design-of-experiments methodology, and the influence of pH and ionic strength on their behaviour was investigated. The citrate buffer had a pronounced effect on the stability of AuNPs due to the more complex intermolecular interactions, which was also confirmed by the changes in optical properties. In contrast, AuNPs dispersed in lactate and phosphate buffer were stable at therapeutically relevant ionic strength, regardless of their size. Simulation of the local pH distribution near the particle surface also showed a steep pH gradient for particles smaller than 100 nm. This suggests that the healing potential is further enhanced by a more acidic environment at the particle surface, making this strategy a promising approach.

Extreme Concentration and Nanoscale Interaction of Light.

Concentrating light strongly calls for appropriate polarization patterns of the focused light beam and for up to a full 4π solid angle geometry. Focusing on the extreme requires efficient coupling to nanostructures of one kind or another via cylindrical vector beams having such patterns, the details of which depend on the geometry and property of the respective nanostructure. Cylindrical vector beams can not only be used to study a nanostructure, but also vice versa. Closely related is the discussion of topics such as the ultimate diffraction limit, a resonant field enhancement near nanoscopic absorbers, as well as speculations about nonresonant field enhancement, which, if it exists, might be relevant to pair production in vacuum. These cases do require further rigorous simulations and more decisive experiments. While there is a wide diversity of scenarios, there are also conceptually very different models offering helpful intuitive pictures despite this diversity.

Absolute characterization of high numerical aperture microscope objectives utilizing a dipole scatterer.

Measuring the aberrations of optical systems is an essential step in the fabrication of high precision optical components. Such a characterization is usually based on comparing the device under investigation with a calibrated reference object. However, when working at the cutting-edge of technology, it is increasingly difficult to provide an even better or well-known reference device. In this manuscript we present a method for the characterization of high numerical aperture microscope objectives, functioning without the need of calibrated reference optics. The technique constitutes a nanoparticle, acting as a dipole-like scatterer, that is placed in the focal volume of the microscope objective. The light that is scattered by the particle can be measured individually and serves as the reference wave in our system. Utilizing the well-characterized scattered light as nearly perfect reference wave is the main idea behind this manuscript.

Microsphere kinematics from the polarization of tightly focused nonseparable light.

Recently, it was shown that vector beams can be utilized for fast kinematic sensing via measurements of their global polarization state [Optica2, 864 (2015)10.1364/OPTICA.2.000864]. The method relies on correlations between the spatial and polarization degrees of freedom of the illuminating field which result from its nonseparable mode structure. Here, we extend the method to the nonparaxial regime. We study experimentally and theoretically the far-field polarization state generated by the scattering of a dielectric microsphere in a tightly focused vector beam as a function of the particle position. Using polarization measurements only, we demonstrate position sensing of a Mie particle in three dimensions. Our work extends the concept of back focal plane interferometry and highlights the potential of polarization analysis in optical tweezers employing structured light.

Hybrid Orthorhombic Carbon Flakes Intercalated with Bimetallic Au-Ag Nanoclusters: Influence of Synthesis Parameters on Optical Properties.

Until recently, planar carbonaceous structures such as graphene did not show any birefringence under normal incidence. In contrast, a recently reported novel orthorhombic carbonaceous structure with metal nanoparticle inclusions does show intrinsic birefringence, outperforming other natural orthorhombic crystalline materials. These flake-like structures self-assemble during a laser-induced growth process. In this article, we explore the potential of this novel material and the design freedom during production. We study in particular the dependence of the optical and geometrical properties of these hybrid carbon-metal flakes on the fabrication parameters. The influence of the laser irradiation time, concentration of the supramolecular complex in the solution, and an external electric field applied during the growth process are investigated. In all cases, the self-assembled metamaterial exhibits a strong linear birefringence in the visible spectral range, while the wavelength-dependent attenuation was found to hinge on the concentration of the supramolecular complex in the solution. By varying the fabrication parameters one can steer the shape and size of the flakes. This study provides a route towards fabrication of novel hybrid carbon-metal flakes with tailored optical and geometrical properties.

Towards fully integrated photonic displacement sensors.

The field of optical metrology with its high precision position, rotation and wavefront sensors represents the basis for lithography and high resolution microscopy. However, the on-chip integration-a task highly relevant for future nanotechnological devices-necessitates the reduction of the spatial footprint of sensing schemes by the deployment of novel concepts. A promising route towards this goal is predicated on the controllable directional emission of the fundamentally smallest emitters of light, i.e., dipoles, as an indicator. Here we realize an integrated displacement sensor based on the directional emission of Huygens dipoles excited in an individual dipolar antenna. The position of the antenna relative to the excitation field determines its directional coupling into a six-way crossing of photonic crystal waveguides. In our experimental study supported by theoretical calculations, we demonstrate the first prototype of an integrated displacement sensor with a standard deviation of the position accuracy below λ/300 at room temperature and ambient conditions.

Towards polarization-based excitation tailoring for extended Raman spectroscopy.

Undoubtedly, Raman spectroscopy is one of the most elaborate spectroscopy tools in materials science, chemistry, medicine and optics. However, when it comes to the analysis of nanostructured specimens or individual sub-wavelength-sized systems, the access to Raman spectra resulting from different excitation schemes is usually very limited. For instance, the excitation with an electric field component oriented perpendicularly to the substrate plane is a difficult task. Conventionally, this can only be achieved by mechanically tilting the sample or by sophisticated sample preparation. Here, we propose a novel experimental method based on the utilization of polarization tailored light for Raman spectroscopy of individual nanostructures. As a proof of principle, we create three-dimensional electromagnetic field distributions at the nanoscale using tightly focused cylindrical vector beams impinging normally onto the specimen, hence keeping the traditional beam-path of commercial Raman systems. In order to demonstrate the convenience of this excitation scheme, we use a sub-wavelength diameter gallium-nitride nanostructure as a test platform and show experimentally that its Raman spectra depend sensitively on its location relative to the focal vector field. The observed Raman spectra can be attributed to the interaction with transverse and pure longitudinal electric field components. This novel technique may pave the way towards a characterization of Raman active nanosystems, granting direct access to growth-related parameters such as strain or defects in the material by using the full information of all Raman modes.

Chiral Surface Lattice Resonances.

Collective excitation of periodic arrays of metallic nanoparticles by coupling localized surface plasmon resonances to grazing diffraction orders leads to surface lattice resonances with narrow line width. These resonances may find numerous applications in optical sensing and information processing. Here, a new degree of freedom of surface lattice resonances is experimentally investigated by demonstrating handedness-dependent excitation of surface lattice resonances in arrays of chiral plasmonic crescents. The self-assembly of particles used as mask and modified colloidal lithography is applied to produce arrays of planar and 3D gold crescents over large areas. The excitation of surface lattice resonances as a function of the interparticle distance and the degree of order within the arrays is investigated. The chirality of the individual 3D crescents leads to the formation of chiral lattice modes, that is, surface lattice resonances that exhibit optical activity.

Emission of circularly polarized light by a linear dipole.

Controlling the polarization state and the propagation direction of photons is a fundamental prerequisite for many nanophotonic devices and a precursor for future on-chip communication, where the emission properties of individual emitters are particularly relevant. Here, we report on the emission of partially circularly polarized photons by a linear dipole. The underlying effect is linked to the near-field part of the angular spectrum of the dipole, and it occurs in any type of linear dipole emitter, ranging from atoms and quantum dots to molecules and dipole-like antennas. We experimentally observe it by near-field to far-field transformation at a planar dielectric interface and numerically demonstrate the utility of this phenomenon by coupling the circularly polarized light to the individual paths of crossing waveguides.

Experimental demonstration of linear and spinning Janus dipoles for polarisation- and wavelength-selective near-field coupling.

The electromagnetic field scattered by nano-objects contains a broad range of wavevectors and can be efficiently coupled to waveguided modes. The dominant contribution to scattering from subwavelength dielectric and plasmonic nanoparticles is determined by electric and magnetic dipolar responses. Here, we experimentally demonstrate spectral and phase selective excitation of Janus dipoles, sources with electric and magnetic dipoles oscillating out of phase, in order to control near-field interference and directional coupling to waveguides. We show that by controlling the polarisation state of the dipolar excitations and the excitation wavelength to adjust their relative contributions, directionality and coupling strength can be fully tuned. Furthermore, we introduce a novel spinning Janus dipole featuring cylindrical symmetry in the near and far field, which results in either omnidirectional coupling or noncoupling. Controlling the propagation of guided light waves via fast and robust near-field interference between polarisation components of a source is required in many applications in nanophotonics and quantum optics.

Investigating the Optical Properties of a Laser Induced 3D Self-Assembled Carbon-Metal Hybrid Structure.

Carbon-based and carbon-metal hybrid materials hold great potential for applications in optics and electronics. Here, a novel material made of carbon and gold-silver nanoparticles is discussed, fabricated using a laser-induced self-assembly process. This self-assembled metamaterial manifests itself in the form of cuboids with lateral dimensions on the order of several micrometers and a height of tens to hundreds of nanometers. The carbon atoms are arranged following an orthorhombic unit cell, with alloy nanoparticles intercalated in the crystalline carbon matrix. The optical properties of this metamaterial are analyzed experimentally using a microscopic Müller matrix measurement approach and reveal a high linear birefringence across the visible spectral range. Theoretical modeling based on local-field theory applied to the carbon matrix links the birefringence to the orthorhombic unit cell, while finite-difference time-domain simulations of the metamaterial relates the observed optical response to the distribution of the alloy nanoparticles and the optical density of the carbon matrix.

Weak Measurement Enhanced Spin Hall Effect of Light for Particle Displacement Sensing.

A spherical nanoparticle can scatter tightly focused optical beams in a spin-segmented manner, meaning that the far field of the scattered light exhibits laterally separated left- and right-handed circularly polarized components. This effect, commonly referred to as giant spin Hall effect of light, strongly depends on the position of the scatterer in the focal volume. Here, a scheme that utilizes an optical weak measurement in a cylindrical polarization basis is put forward to drastically enhance the spin-segmentation and, therefore, the sensitivity to small displacements of a scatterer. In particular, we experimentally achieve a change of the spin-splitting signal of 5% per nanometer displacement.

Transverse Kerker Scattering for Angstrom Localization of Nanoparticles.

Angstrom precision localization of a single nanoantenna is a crucial step towards advanced nanometrology, medicine, and biophysics. Here, we show that single nanoantenna displacements down to few angstroms can be resolved with sub-angstrom precision using an all-optical method. We utilize the tranverse Kerker scattering scheme where a carefully structured light beam excites a combination of multipolar modes inside a dielectric nanoantenna, which then, upon interference, scatters directionally into the far field. We spectrally tune our scheme such that it is most sensitive to the change in directional scattering per nanoantenna displacement. Finally, we experimentally show that antenna displacement down to 3 Å is resolvable with a localization precision of 0.6 Å.

Chiroptical response of a single plasmonic nanohelix.

We investigate the chiroptical response of a single plasmonic nanohelix interacting with a weakly focused circularly polarized Gaussian beam. The optical scattering at the fundamental resonance is characterized experimentally and numerically. The angularly resolved scattering of the excited nanohelix is verified experimentally and it validates the numerical results. We employ a multipole decomposition analysis to study the fundamental and first higher-order resonance of the nanohelix, explaining their chiral properties in terms of the formation of chiral dipoles.

Weak Measurement of Elliptical Dipole Moments by C-Point Splitting.

We investigate points of circular polarization in the far field of elliptically polarized dipoles and establish a relation between the angular position and helicity of these C points and the dipole moment. In the case of highly eccentric dipoles, the C points of opposite handedness exhibit only a small angular separation and occur in the low intensity region of the emission pattern. In this regard, we introduce an optical weak measurement approach that utilizes the transverse electric (azimuthal) and transverse magnetic (radial) far-field polarization basis. Projecting the far field onto a spatially varying postselected polarization state reveals the angular separation and the helicity of the C points. We demonstrate the applicability of this approach and determine the elliptical dipole moment of a particle sitting on an interface by measuring the C points in its far field.

Free-space propagation of high-dimensional structured optical fields in an urban environment.

Spatially structured optical fields have been used to enhance the functionality of a wide variety of systems that use light for sensing or information transfer. As higher-dimensional modes become a solution of choice in optical systems, it is important to develop channel models that suitably predict the effect of atmospheric turbulence on these modes. We investigate the propagation of a set of orthogonal spatial modes across a free-space channel between two buildings separated by 1.6 km. Given the circular geometry of a common optical lens, the orthogonal mode set we choose to implement is that described by the Laguerre-Gaussian (LG) field equations. Our study focuses on the preservation of phase purity, which is vital for spatial multiplexing and any system requiring full quantum-state tomography. We present experimental data for the modal degradation in a real urban environment and draw a comparison to recognized theoretical predictions of the link. Our findings indicate that adaptations to channel models are required to simulate the effects of atmospheric turbulence placed on high-dimensional structured modes that propagate over a long distance. Our study indicates that with mitigation of vortex splitting, potentially through precorrection techniques, one could overcome the challenges in a real point-to-point free-space channel in an urban environment.

Exotic looped trajectories of photons in three-slit interference.

The validity of the superposition principle and of Born's rule are well-accepted tenants of quantum mechanics. Surprisingly, it has been predicted that the intensity pattern formed in a three-slit experiment is seemingly in contradiction with the most conventional form of the superposition principle when exotic looped trajectories are taken into account. However, the probability of observing such paths is typically very small, thus rendering them extremely difficult to measure. Here we confirm the validity of Born's rule and present the first experimental observation of exotic trajectories as additional paths for the light by directly measuring their contribution to the formation of optical interference fringes. We accomplish this by enhancing the electromagnetic near-fields in the vicinity of the slits through the excitation of surface plasmons. This process increases the probability of occurrence of these exotic trajectories, demonstrating that they are related to the near-field component of the photon's wavefunction.

Chiral optical response of planar and symmetric nanotrimers enabled by heteromaterial selection.

Chirality is an intriguing property of certain molecules, materials or artificial nanostructures, which allows them to interact with the spin angular momentum of the impinging light field. Due to their chiral geometry, they can distinguish between left- and right-hand circular polarization states or convert them into each other. Here we introduce an approach towards optical chirality, which is observed in individual two-dimensional and geometrically mirror-symmetric nanostructures. In this scheme, the chiral optical response is induced by the chosen heterogeneous material composition of a particle assembly and the corresponding resonance behaviour of the constituents it is built from, which breaks the symmetry of the system. As a proof of principle, we investigate such a structure composed of individual silicon and gold nanoparticles both experimentally, as well as numerically. Our proposed concept constitutes an approach for designing two-dimensional chiral media tailored at the nanoscale, allowing for high tunability of their optical response.

Experimental generation of amplitude squeezed vector beams.

We present an experimental method for the generation of amplitude squeezed high-order vector beams. The light is modified twice by a spatial light modulator such that the vector beam is created by means of a collinear interferometric technique. A major advantage of this approach is that it avoids systematic losses, which are detrimental as they cause decoherence in continuous-variable quantum systems. The utilisation of a spatial light modulator (SLM) gives the flexibility to switch between arbitrary mode orders. The conversion efficiency with our setup is only limited by the efficiency of the SLM. We show the experimental generation of Laguerre-Gauss (LG) modes with radial indices 0 or 1 and azimuthal indices up to 3 with complex polarization structures and a quantum noise reduction up to -0.9dB±0.1dB. The corresponding polarization structures are studied in detail by measuring the spatial distribution of the Stokes parameters.

Optical Polarization Möbius Strips and Points of Purely Transverse Spin Density.

Tightly focused light beams can exhibit complex and versatile structured electric field distributions. The local field may spin around any axis including a transverse axis perpendicular to the beams' propagation direction. At certain focal positions, the corresponding local polarization ellipse can even degenerate into a perfect circle, representing a point of circular polarization or C point. We consider the most fundamental case of a linearly polarized Gaussian beam, where-upon tight focusing-those C points created by transversely spinning fields can form the center of 3D optical polarization topologies when choosing the plane of observation appropriately. Because of the high symmetry of the focal field, these polarization topologies exhibit nontrivial structures similar to Möbius strips. We use a direct physical measure to find C points with an arbitrarily oriented spinning axis of the electric field and experimentally investigate the fully three-dimensional polarization topologies surrounding these C points by exploiting an amplitude and phase reconstruction technique.