Limitations of Particle-Based Spasers.

We present a semiclassical analytic model for spherical core-shell surface plasmon lasers. Within this model, we drop the widely used one-mode approximations in favor of fully electromagnetic Mie theory. This allows for incorporation of realistic gain relaxation rates that so far are massively underestimated. Especially, higher order modes can undermine and even reverse the beneficial effects of the strong Purcell effect in such systems. Our model gives a clear view on gain and resonator requirements, as well as on the output characteristics that will help experimenters to design more efficient particle-based spasers.

Investigation of Line Width Narrowing and Spectral Jumps of Single Stable Defect Centers in ZnO at Cryogenic Temperature.

Finding new solid state defect centers in novel host materials is crucial for realizing integrated hybrid quantum photonic devices. We present a preparation method for defect centers with photostable bright single photon emission in zinc oxide, a material with promising properties in terms of processability, availability, and applications. A detailed optical study reveals a complex dynamic of intensity fluctuations at room temperature. Measurements at cryogenic temperatures show very sharp (<60 GHz) zero phonon lines (ZPLs) at 580 nm to  620 nm (≈ 2.0 eV) with frozen out fast fluctuations. Remaining discrete jumps of the ZPL, which depend on the excitation power, are observed. The low temperature results will narrow down speculations on the origin of visible-near-infrared (NIR) wavelength defect emission in zinc oxide and provide a basis for improved theoretical models.

Bulk-suppressed and surface-sensitive Raman scattering by transferable plasmonic membranes with irregular slot-shaped nanopores.

Raman spectroscopy enables the non-destructive characterization of chemical composition, crystallinity, defects, or strain in countless materials. However, the Raman response of surfaces or thin films is often weak and obscured by dominant bulk signals. Here we overcome this limitation by placing a transferable porous gold membrane, (PAuM) on the surface of interest. Slot-shaped nanopores in the membrane act as plasmonic antennas and enhance the Raman response of the surface or thin film underneath. Simultaneously, the PAuM suppresses the penetration of the excitation laser into the bulk, efficiently blocking its Raman signal. Using graphene as a model surface, we show that this method increases the surface-to-bulk Raman signal ratio by three orders of magnitude. We find that 90% of the Raman enhancement occurs within the top 2.5 nm of the material, demonstrating truly surface-sensitive Raman scattering. To validate our approach, we quantify the strain in a 12.5 nm thin Silicon film and analyze the surface of a LaNiO3 thin film. We observe a Raman mode splitting for the LaNiO3 surface-layer, which is spectroscopic evidence that the surface structure differs from the bulk. These results validate that PAuM gives direct access to Raman signatures of thin films and surfaces.

Fiber-integrated diamond-based single photon source.

An alignment free, micrometer-scale single photon source consisting of a single quantum emitter on an optical fiber operating at room temperature is demonstrated. It easily integrates into fiber optic networks for quantum cryptography or quantum metrology applications.(1) Near-field coupling of a single nitrogen-vacancy center is achieved in a bottom-up approach by placing a preselected nanodiamond directly on the fiber facet. Its high photon collection efficiency is equivalent to a far-field collection via an objective with a numerical aperture of 0.82. Furthermore, simultaneous excitation and re-collection through the fiber is possible by introducing a fiber-connected single emitter sensor.

Single defect centers in diamond nanocrystals as quantum probes for plasmonic nanostructures.

We present two applications of a single nitrogen vacancy center in a nanodiamond as quantum probe for plasmonic nanostructures. Coupling to the nanostructures is achieved in a highly controlled manner by picking up a pre-characterized nanocrystal with an atomic force microscope and placing it at the desired position. Local launching of single excitations into a nanowire with a spatial control of few nanometers is demonstrated. Further, a two dimensional map of the electromagnetic environment of a plasmonic bowtie antenna was derived, resembling an ultimate limit of fluorescence lifetime nanoscopy.

Self-Assembly of Plasmonic Nanoantenna-Waveguide Structures for Subdiffractional Chiral Sensing.

Spin-momentum locking is a peculiar effect in the near-field of guided optical or plasmonic modes. It can be utilized to map the spinning or handedness of electromagnetic fields onto the propagation direction. This motivates a method to probe the circular dichroism of an illuminated chiral object. In this work, we demonstrate local, subdiffraction limited chiral coupling of light and propagating surface plasmon polaritons in a self-assembled system of a gold nanoantenna and a silver nanowire. A thin silica shell around the nanowire provides precise distance control and also serves as a host for fluorescent molecules, which indicate the direction of plasmon propagation. We characterize our nanoantenna-nanowire systems comprehensively through correlated electron microscopy, energy-dispersive X-ray spectroscopy, dark-field, and fluorescence imaging. Three-dimensional numerical simulations support the experimental findings. Besides our measurement of far-field polarization, we estimate sensing capabilities and derive not only a sensitivity of 1 mdeg for the ellipticity of the light field, but also find 103 deg cm2/dmol for the circular dichroism of an analyte locally introduced in the hot spot of the antenna-wire system. Thorough modeling of a prototypical design predicts on-chip sensing of chiral analytes. This introduces our system as an ultracompact sensor for chiral response far below the diffraction limit.

Axial localization and tracking of self-interference nanoparticles by lateral point spread functions.

Sub-diffraction limited localization of fluorescent emitters is a key goal of microscopy imaging. Here, we report that single upconversion nanoparticles, containing multiple emission centres with random orientations, can generate a series of unique, bright and position-sensitive patterns in the spatial domain when placed on top of a mirror. Supported by our numerical simulation, we attribute this effect to the sum of each single emitter's interference with its own mirror image. As a result, this configuration generates a series of sophisticated far-field point spread functions (PSFs), e.g. in Gaussian, doughnut and archery target shapes, strongly dependent on the phase difference between the emitter and its image. In this way, the axial locations of nanoparticles are transferred into far-field patterns. We demonstrate a real-time distance sensing technology with a localization accuracy of 2.8 nm, according to the atomic force microscope (AFM) characterization values, smaller than 1/350 of the excitation wavelength.

Silver nanowires with optimized silica coating as versatile plasmonic resonators.

Metal nanoparticles are the most frequently used nanostructures in plasmonics. However, besides nanoparticles, metal nanowires feature several advantages for applications. Their elongation offers a larger interaction volume, their resonances can reach higher quality factors, and their mode structure provides better coupling into integrated hybrid dielectric-plasmonic circuits. It is crucial though, to control the distance of the wire to a supporting substrate, to another metal layer or to active materials with sub-nanometer precision. A dielectric coating can be utilized for distance control, but it must not degrade the plasmonic properties. In this paper, we introduce a controlled synthesis and coating approach for silver nanowires to fulfill these demands. We synthesize and characterize silver nanowires of around 70 nm in diameter. These nanowires are coated with nm-sized silica shells using a modified Stöber method to achieve a homogeneous and smooth surface quality. We use transmission electron microscopy, dark-field microscopy and electron-energy loss spectroscopy to study morphology and plasmonic resonances of individual nanowires and quantify the influence of the silica coating. Thorough numerical simulations support the experimental findings showing that the coating does not deteriorate the plasmonic properties and thus introduce silver nanowires as usable building blocks for integrated hybrid plasmonic systems.

A realistic fabrication and design concept for quantum gates based on single emitters integrated in plasmonic-dielectric waveguide structures.

Tremendous enhancement of light-matter interaction in plasmonic-dielectric hybrid devices allows for non-linearities at the level of single emitters and few photons, such as single photon transistors. However, constructing integrated components for such devices is technologically extremely challenging. We tackle this task by lithographically fabricating an on-chip plasmonic waveguide-structure connected to far-field in- and out-coupling ports via low-loss dielectric waveguides. We precisely describe our lithographic approach and characterize the fabricated integrated chip. We find excellent agreement with rigorous numerical simulations. Based on these findings we perform a numerical optimization and calculate concrete numbers for a plasmonic single-photon transistor.

Micro-concave waveguide antenna for high photon extraction from nitrogen vacancy centers in nanodiamond.

The negatively charged nitrogen-vacancy colour center (NV(-) center) in nanodiamond is an excellent single photon source due to its stable photon generation in ambient conditions, optically addressable nuclear spin state, high quantum yield and its availability in nanometer sized crystals. In order to make practical devices using nanodiamond, highly efficient and directional emission of single photons in well-defined modes, either collimated into free space or waveguides are essential. This is a Herculean task as the photoluminescence of the NV centers is associated with two orthogonal dipoles arranged in a plane perpendicular to the NV defect symmetry axis. Here, we report on a micro-concave waveguide antenna design, which can effectively direct single photons from any emitter into either free space or into waveguides in a narrow cone angle with more than 80% collection efficiency irrespective of the dipole orientation. The device also enhances the spontaneous emission rate which further increases the number of photons available for collection. The waveguide antenna has potential applications in quantum cryptography, quantum computation, spectroscopy and metrology.

A scanning probe-based pick-and-place procedure for assembly of integrated quantum optical hybrid devices.

Integrated quantum optical hybrid devices consist of fundamental constituents such as single emitters and tailored photonic nanostructures. A reliable fabrication method requires the controlled deposition of active nanoparticles on arbitrary nanostructures with highest precision. Here, we describe an easily adaptable technique that employs picking and placing of nanoparticles with an atomic force microscope combined with a confocal setup. In this way, both the topography and the optical response can be monitored simultaneously before and after the assembly. The technique can be applied to arbitrary particles. Here, we focus on nanodiamonds containing single nitrogen vacancy centers, which are particularly interesting for quantum optical experiments on the single photon and single emitter level.