Stefan Schietinger

Plasmon-Enhanced Upconversion in Single NaYF4:Yb3+/Er3+ Codoped Nanocrystals

In this Letter we report the plasmon-enhanced upconversion in single NaYF(4) nanocrystals codoped with Yb(3+)/Er(3+). Single nanocrystals and gold nanospheres are investigated and assembled in a combined confocal and atomic force microscope setup. The nanocrystals show strong upconversion emission in the green and red under excitation with a continuous wave laser in the near-infrared at 973 nm. By the use of the atomic force microscope, we couple single nanocrystals with gold spheres (30 and 60 nm in diameter) to obtain enhanced upconversion emission. An overall enhancement factor of 3.8 is reached. A comparison of time-resolved measurements on the bare nanocrystal and the coupled nanocrystal-gold sphere systems unveil that faster excitation as well as faster emission occurs in the nanocrystals.

Plasmon-Enhanced Single Photon Emission from a Nanoassembled Metal−Diamond Hybrid Structure at Room Temperature

In this Letter we present the controlled coupling of a single nitrogen vacancy center to a plasmonic structure. With the help of an atomic force microscope, a single nanodiamond containing a single nitrogen vacancy center and two gold nanospheres are assembled step-by-step. We show that both the excitation rate and the radiative decay rate of the color center are enhanced by about 1 order of magnitude, while the single photon character of the emission is maintained. Hot spots between diamond and gold nanoparticles provide an efficient near-field coupling, despite the mismatch in size and shape. Our approach provides hybrid systems as important building blocks for novel nanophotonic light sources in advanced plasmonic devices stable even at room temperature.

Observation of Size Dependence in Multicolor Upconversion in Single Yb3+, Er3+ Codoped NaYF4 Nanocrystals

In this Letter we report on the investigation of the upconversion emission of single NaYF(4) nanocrystals codoped with Yb(3+) and Er(3+). Single nanocrystals on a coverslip are excited with continuous wave laser light at 973 nm in a confocal setup and the upconversion fluorescence is analyzed with a spectrometer. With the help of an atomic force microscope the size of the nanocrystals is simultaneously determined. A strong size-dependence of the spectral properties of the upconversion signal of individual nanocrystals is observed. We attribute this to a differing number of available phonons in the individual crystals for multiphonon relaxation processes, depending on their size. We believe that this result provides a new strategy in the synthesis of upconversion nanoparticles with different spectral properties by changing only their size as it is well-known from the case of semiconductor quantum dots.

Nanoassembled Plasmonic-Photonic Hybrid Cavity for Tailored Light-Matter Coupling

We propose and demonstrate a hybrid cavity system in which metal nanoparticles are evanescently coupled to a dielectric photonic crystal cavity using a nanoassembly method. While the metal constituents lead to strongly localized fields, optical feedback is provided by the surrounding photonic crystal structure. The combined effect of plasmonic field enhancement and high quality factor (Q approximately 900) opens new routes for the control of light-matter interaction at the nanoscale.

One-by-One Coupling of Single Defect Centers in Nanodiamonds to High-Q Modes of an Optical Microresonator

In this letter, we present the on-demand coupling of single NV(-) defect centers in nanodiamonds to a polystyrene microspherical resonator. From an ensemble on a coverslip, we select single nanodiamonds containing a single defect proven by a pronounced antibunching dip. With the help of a scanning near-field probe, we can attach these nanodiamonds to a microsphere resonator one-by-one. A clearly modulated fluorescence spectrum demonstrates coupling of the single defect centers to high-Q whispering-gallery modes. Our experiments establish a toolbox to assemble complex systems consisting of single quantum emitters and (coupled) microresonators.

Coupling single NV-centres to high-Q whispering gallery modes of a preselected frequency-matched microresonator

In this paper, we report the controlled coupling of fluorescence from a single NV-centre in a single nanodiamond to the high-Q modes of a preselected microsphere. Microspheres from an ensemble with a finite size distribution can be characterized precisely via white light Mie-scattering. The mode spectrum of individual spheres can be determined with high precision. A sphere with an appropriate spectrum can be selected, and a nanodiamond containing a single NV-centre can be coupled to it. The spectral position of the calculated lowest order whispering gallery modes are found to be in very good agreement with the experimentally observed resonances of the coupled fluorescence from the single NV-centre.

In Situ Observation of Plasmon Tuning in a Single Gold Nanoparticle during Controlled Melting

In this Letter we study the relations among shape, symmetry, and plasmon resonance shift in a single gold nanoparticle during laser melting. A beam of an argon ion laser is focused on a selected particle, while its optical and shape properties can be observed with the help of a combined dark-field/photoluminescence microscope and an atomic force microscope, respectively. Starting from a spherical shape, radiation pressure forms the melting gold particle into an upright standing rod on a glass substrate, showing a characteristic dipole scattering pattern. A red-shift of the photoluminescence signal and the scattering spectrum is observed. The melting process can be controlled allowing the formation of different particle heights and plasmon resonance shifts. In situ tuning of the plasmon resonance of individual particles is possible with this reversible melting process.

Measuring the quantum nature of light with a single source and a single detector

We realized the most fundamental quantum optical experiment to prove the non-classical character of light: Only a single quantum emitter and a single superconducting nanowire detector were used. A particular appeal of our experiment is its elegance and simplicity. Yet its results unambiguously enforce a quantum theory for light. Previous experiments relied on more complex setups, such as the Hanbury-Brown-Twiss configuration, where a beam splitter directs light to two photodetectors, giving the false impression that the beam splitter is required. Our work results in a major simplification of the widely used photon-correlation techniques with applications ranging from quantum information processing to single-molecule detection.

Silica-coated Au/Ag nanorods with tunable surface plasmon bands for nanoplasmonics with single particles

We present the synthesis and analysis of silica-coated Au/Ag bimetallic nanorods with controlled surface plasmon bands. Depending on the thickness of Ag shell deposited on the Au nanorod surface, there is a blue-shift on the longitudinal surface plasmon band of Au nanorods, which can be expressed by an approximate formula derived from the absorption profile of light in Ag films using finite difference time domain simulations. The subsequent coating of silica shell not only enhances the stability of the Au/Ag bimetallic nanorods but also provides a mesoporous host for optically active species. Minute red-shifts of the longitudinal resonance mode, induced by stepwise increased silica shell volumes, are shown. Application as carrier for fluorescent rhodamine B molecules is demonstrated by photoluminescence analysis. On the single-particle level, dark field microscopy of Au/Ag-silica nanorods was finally employed. This introduces a route towards revealing the relation between structure, shape, and optical (plasmonic) properties of complex composite metal particles as well as fabrication strategies for nanoassemblies of tailored structures in the field of nanoplasmonics.

Assembly of fundamental photonic elements from single nanodiamonds

We demonstrate the ability to modify the emission properties and enhance the interaction strength of single emitters coupled to nanophotonic structures based on metals and dielectrics. Assembly of individual diamond nanocrystals, metal nanoparticles and photonic crystal cavities to meta-structures is introduced. Experiments concerning controlled coupling of single defect centers in nanodiamonds to silver nanowires with the goal to investigate quantum plasmonic effects are reported. Furthermore, we demonstrate the formation of a hybrid cavity system in which metal nanostructures are evanescently coupled to a dielectric photonic crystal cavity. This structure allows combined exploitation of both resonant dielectric as well as plasmonic enhancement.