Vahid Sandoghdar

Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna.

We investigate the coupling of a single molecule to a single spherical gold nanoparticle acting as a nanoantenna. Using scanning probe technology, we position the particle in front of the molecule with nanometer accuracy and measure a strong enhancement of more than 20 times in the fluorescence intensity simultaneous to a 20-fold shortening of the excited state lifetime. Comparisons with three-dimensional calculations guide us to decipher the contributions of the excitation enhancement, spontaneous emission modification, and quenching. Furthermore, we provide direct evidence for the role of the particle plasmon resonance in the molecular excitation and emission processes.

A single gold particle as a probe for apertureless scanning near-field optical microscopy

We report on the fabrication, characterization and application of a probe consisting of a single gold nanoparticle for apertureless scanning near‐field optical microscopy. Particles with diameters of 100 nm have been successfully and reproducibly mounted at the end of sharp glass fibre tips. We present the first optical images taken with such a probe. We have also recorded plasmon resonances of gold particles and discuss schemes for exploiting the wavelength dependence of their scattering cross‐section for a novel form of apertureless scanning near‐field optical microscopy.

Optical microscopy using a single-molecule light source

Rapid progress in science on nanoscopic scales has promoted increasing interest in techniques of ultrahigh-resolution optical microscopy. The diffraction limit can be surpassed by illuminating an object in the near field through a sub-wavelength aperture at the end of a sharp metallic probe. Proposed modifications of this technique involve replacing the physical aperture by a nanoscopic active light source. Advances in the spatial and spectral detection of individual fluorescent molecules, using near-field and far-field methods, suggest the possibility of using a single molecule as the illumination source. Here we present optical images taken with a single molecule as a point-like source of illumination, by combining fluorescence excitation spectroscopy with shear-force microscopy. Our single-molecule probe has potential for achieving molecular resolution in optical microscopy; it should also facilitate controlled studies of nanometre-scale phenomena (such as resonant energy transfer) with improved lateral and axial spatial resolution.

A planar dielectric antenna for directional single-photon emission and near-unity collection efficiency

Single-photon sources have been discussed as the building blocks of quantum cryptography, optical quantum computation, spectroscopy, and metrology. However, when using sources based on single emitters, the success of these proposals depends on the ability to achieve near-unity collection efficiency into well-defined modes. Some of the current state-of-the-art efforts aimed at achieving these criteria have been demonstrated, but despite an impressive progress the results still fall short. In particular, a collection efficiency of 38% were reported using microresonators [1], while a nanowire device reached an efficiency of 72% at cryogenic temperatures [2]. Here we report on a broad-band room-temperature scheme, which uses a layered dielectric antenna for realizing ultra-bright single photon sources with near-unity collection efficiency.

Splitting of high-Q Mie modes induced by light backscattering in silica microspheres

We have observed that very high-Q Mie resonances in silica microspheres are split into doublets. This splitting is attributed to internal backscattering that couples the two degenerate whispering-gallery modes propagating in opposite directions along the sphere equator. We have studied this doublet structure by high-resolution spectroscopy. Time-decay measurements have also been performed and show a beat note corresponding to the coupling rate between the clockwise and counterclockwise modes. A simple model of coupled oscillators describes our data well, and the backscattering efficiency that we measure is consistent with what is observed in optical fibers.

Design of plasmonic nanoantennae for enhancing spontaneous emission

We apply two- and three-dimensional numerical calculations to study optical nanoantennae made of two coupled gold nanostructures, enclosing a single emitter in their gap. We show that, using structures manufacturable with todays nanotechnology, it is possible to increase the radiative decay rate by three orders of magnitude while keeping a quantum efficiency larger than 80% in the near-infrared regime. We examine the competition between the radiative and nonradiative processes in the presence of the antennae as a function of wavelength and antenna geometry. Our results hold great promise for improving the quantum efficiency of poor emitters such as silicon nanocrystals or carbon nanotubes.

High-speed nanoscopic tracking of the position and orientation of a single virus.

Optical studies have revealed that, after binding, virions move laterally on the plasma membrane, but the complexity of the cellular environment and the drawbacks of fluorescence microscopy have prevented access to the molecular dynamics of early virus-host couplings, which are important for cell infection. Here we present a colocalization methodology that combines scattering interferometry and single-molecule fluorescence microscopy to visualize both position and orientation of single quantum dot–labeled Simian virus 40 (SV40) particles. By achieving nanometer spatial and 8 ms temporal resolution, we observed sliding and tumbling motions during rapid lateral diffusion on supported lipid bilayers, and repeated back and forth rocking between nanoscopic regions separated by 9 nm. Our findings suggest recurrent swap of receptors and viral pentamers as well as receptor aggregation in nanodomains. We discuss the prospects of our technique for studying virus-membrane interactions and for resolving nanoscopic dynamics of individual biological nano-objects.

Controlled coupling of counterpropagating whispering-gallery modes by a single Rayleigh scatterer: a classical problem in a quantum optical light.

We present experiments where a single subwavelength scatterer is used to examine and control the backscattering induced coupling between counterpropagating high-Q modes of a microsphere resonator. Our measurements reveal the standing wave character of the resulting symmetric and antisymmetric eigenmodes, their unbalanced intensity distributions, and the coherent nature of their coupling. We discuss our findings and the underlying classical physics in the framework common to quantum optics and provide a particularly intuitive explanation of the central processes.

A single-molecule optical transistor

The transistor is one of the most influential inventions of modern times and is ubiquitous in present-day technologies. In the continuing development of increasingly powerful computers as well as alternative technologies based on the prospects of quantum information processing, switching and amplification functionalities are being sought in ultrasmall objects, such as nanotubes, molecules or atoms. Among the possible choices of signal carriers, photons are particularly attractive because of their robustness against decoherence, but their control at the nanometre scale poses a significant challenge as conventional nonlinear materials become ineffective. To remedy this shortcoming, resonances in optical emitters can be exploited, and atomic ensembles have been successfully used to mediate weak light beams. However, single-emitter manipulation of photonic signals has remained elusive and has only been studied in high-finesse microcavities or waveguides. Here we demonstrate that a single dye molecule can operate as an optical transistor and coherently attenuate or amplify a tightly focused laser beam, depending on the power of a second ‘gating’ beam that controls the degree of population inversion. Such a quantum optical transistor has also the potential for manipulating non-classical light fields down to the single-photon level. We discuss some of the hurdles along the road towards practical implementations, and their possible solutions.

Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

Single dye molecules at cryogenic temperatures exhibit many spectroscopic phenomena known from the study of free atoms and are thus promising candidates for experiments in fundamental quantum optics. However, the existing techniques for their detection have either sacrificed information on the coherence of the excited state or have been inefficient. Here, we show that these problems can be addressed by focusing the excitation light near to the extinction cross-section of a molecule. Our detection scheme enables us to explore resonance fluorescence over nine orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first direct observation of the Mollow fluorescence triplet from a single solid-state emitter. Under weak excitation, we report the detection of a single molecule with an incident power as faint as 600 aW, paving the way for studying nonlinear effects with only a few photons.