arXiv subjects

Vahid Sandoghdar

Publications and source records attributed to Vahid Sandoghdar.

At least 55 records · Page 3Linked to original sources

arXiv2014

High-cooperativity nanofiber laser

Cavity-free efficient coupling between emitters and guided modes is of great current interest for nonlinear quantum optics as well as efficient and scalable quantum information processing. In this work, we extend these activities to the coupling of organic dye molecules to a highly confined mode of a nanofiber, allowing mirrorless and low-threshold laser action in an effective mode volume of less than 100 femtoliters. We model this laser system based on semi-classical rate equations and present an analytic compact form of the laser output intensity. Despite the lack of a cavity structure, we achieve a coupling efficiency of the spontaneous emission to the waveguide mode of 0.07(0.01), in agreement with our calculations. In a further experiment, we also demonstrate the use of a plasmonic nanoparticle as a dispersive output coupler. Our laser architecture is promising for a number of applications in optofluidics and provides a fundamental model system for studying nonresonant feedback stimulated emission.

physics.optics↗

arXiv2013

Tracking single particles on supported lipid membranes: multi-mobility diffusion and nanoscopic confinement

Supported lipid bilayers have been studied intensively over the past two decades. In this work, we study the diffusion of single gold nanoparticles (GNPs) with diameter of 20 nm attached to GM1 ganglioside or DOPE lipids at different concentrations in supported DOPC bilayers. The indefinite photostability of GNPs combined with the high sensitivity of interferometric scattering microscopy (iSCAT) allows us to achieve 1.9 nm spatial precision at 1 ms temporal resolution, while maintaining long recording times. Our trajectories visualize strong transient confinements within domains as small as 20 nm, and the statistical analysis of the data reveals multiple mobilities and deviations from normal diffusion. We present a detailed analysis of our findings and provide interpretations regarding the effect of the supporting substrate and GM1 clustering. We also comment on the use of high-speed iSCAT for investigating diffusion of lipids, proteins or viruses in lipid membranes with unprecedented spatial and temporal resolution.

physics.bio-ph↗

arXiv2013

Detection, spectroscopy and state preparation of a single praseodymium ion in a crystal

Solid-state emitters with atom-like optical and magnetic transitions are highly desirable for efficient and scalable quantum state engineering and information processing. Quantum dots, color centers and impurities embedded in inorganic hosts have attracted a great deal of attention in this context, but influences from the matrix continue to pose challenges on the degree of attainable coherence in each system. We report on a new solid-state platform based on the optical detection of single praseodymium ions via 4f intrashell transitions, which are well shielded from their surroundings. By combining cryogenic high-resolution laser spectroscopy with fluorescence microscopy, we were able to spectrally select and spatially resolve individual ions. In addition to elaborating on the essential experimental steps for achieving this long-sought goal, we demonstrate state preparation and read out of the three ground-state hyperfine levels, which are known to have lifetimes of the order of hundred seconds.

quant-ph↗

arXiv2013

Direct optical sensing of single unlabeled small proteins and super-resolution microscopy of their binding sites

More than twenty years ago, scientists succeeded in pushing the limits of optical detection to single molecules using fluorescence. This breakthrough has revolutionized biophysical measurements, but restrictions in photophysics and labeling protocols have motivated many efforts to achieve fluorescence-free single-molecule sensitivity in biological studies. Although several interesting mechanisms using vibrational spectroscopy, photothermal detection, plasmonics or microcavities have been proposed for biosensing at the single-protein level, no method has succeeded in direct label-free detection of single proteins. Here, we present the first results using interferometric detection of scattering (iSCAT) from single proteins without the need for any label, optical nanostructure or microcavity. Furthermore, we demonstrate super-resolution imaging of protein binding with nanometer localization precision. The ease of iSCAT instrumentation promises a breakthrough for industrial usage as well as fundamental laboratory experiments.

physics.bio-ph↗

arXiv2012

Coherent interaction of a metallic structure with a single quantum emitter: from super absorption to cloaking

We provide a general theoretical platform based on quantized radiation in absorptive and inhomogeneous media for investigating the coherent interaction of light with metallic structures in the immediate vicinity of quantum emitters. In the case of a very small metallic cluster, we demonstrate extreme regimes where a single emitter can either counteract or enhance particle absorption by three orders of magnitude. For larger structures, we show that an emitter can eliminate both scattering and absorption and cloak a plasmonic antenna. We provide physical interpretations of our results and discuss their applications in active metamaterials and quantum plasmonics.

physics.optics↗

arXiv2012

Metallo-dielectric hybrid antennas for ultrastrong enhancement of spontaneous emission

We devise new optical antennas that reduce the excited-state radiative lifetimes of emitters to the order of 100 femtoseconds while maintaining quantum efficiencies of about 80% at a broadband operation. Here, we combine metallic nanoparticles with planar dielectric structures and exploit design strategies from plasmonic nanoantennas and concepts from Cavity Quantum Electrodynamics to maximize the local density of states and minimize the nonradiative losses incurred by the metallic constituents. The proposed metallo-dielectric hybrid antennas promise important impact on various fundamental and applied research fields, including photophysics, ultrafast plasmonics, bright single photon sources and Raman spectroscopy.

physics.optics↗

arXiv2011

99% efficiency in collecting photons from a single emitter

In Nature Photonics 5, 166 (2011), we reported on a planar dielectric antenna that achieved 96% efficiency in collecting the photons emitted by a single molecule. In that work the transition dipole moment of the molecule was set perpendicular to the antenna plane. Here, we present an extension of that scheme that reaches collection efficiencies beyond 99% for emitters with arbitrarily oriented dipole moments. Our work opens important doors in a wide range of contexts including quantum optics, quantum metrology, nano-analytics, and biophysics. In particular, we provide antenna parameters to realize ultrabright single-photon sources in high-index materials such as semiconductor quantum dots and color centers in diamond, as well as sensitive detection of single molecules in nanofluidic devices.

quant-ph↗

arXiv2010

Coherent Nonlinear Single Molecule Microscopy

We investigate a nonlinear localization microscopy method based on Rabi oscillations of single emitters. We demonstrate the fundamental working principle of this new technique using a cryogenic far-field experiment in which subwavelength features smaller than $λ$/10 are obtained. Using Monte Carlo simulations, we show the superior localization accuracy of this method under realistic conditions and a potential for higher acquisition speed or a lower number of required photons as compared to conventional linear schemes. The method can be adapted to other emitters than molecules and allows for the localization of several emitters at different distances to a single measurement pixel.

quant-ph↗

arXiv2010

Direct detection of single molecules by optical absorption

The advent of single molecule optics has had a profound impact in fields ranging from biophysics to material science, photophysics, and quantum optics. However, all existing room-temperature single molecule methods have been based on fluorescence detection of highly efficient emitters. Here we demonstrate that standard, modulation-free measurements known from conventional absorption spectrometers can indeed detect single molecules. We report on quantitative measurements of the absorption cross section of single molecules under ambient condition even in their dark state, for example during photoblinking or strong quenching. Our work extends single-molecule microscopy and spectroscopy to a huge class of materials that absorb light but do not fluoresce efficiently.

cond-mat.mes-hall↗

arXiv2010

Fluorescence enhancement with the optical (bi-) conical antenna

We investigate the properties of finite gold nanocones as optical antennas for enhancing molecular fluorescence. We compute the modification of the excitation rate, spontaneous emission rate, and quantum efficiency as a function of the nanocone base and length, showing that the maximum field and fluorescence enhancements do not occur for the same nanocone parameters. We compare the results with those for nanorods and nanospheroids and find that nanocones perform better.

physics.chem-ph↗

arXiv2009

Resolution and enhancement in nanoantenna-based fluorescence microscopy

Single gold nanoparticles can act as nanoantennas for enhancing the fluorescence of emitters in their near-fields. Here we present experimental and theoretical studies of scanning antenna-based fluorescence microscopy as a function of the diameter of the gold nanoparticle. We examine the interplay between fluorescence enhancement and spatial resolution and discuss the requirements for deciphering single molecules in a dense sample. Resolutions better than 20 nm and fluorescence enhancement up to 30 times are demonstrated experimentally. By accounting for the tip shaft and the sample interface in finite-difference time-domain calculations, we explain why the measured fluorescence enhancements are higher in the presence of an interface than the values predicted for a homogeneous environment.

physics.optics↗

arXiv2009

Highly efficient interfacing of guided plasmons and photons in nanowires

Successful exploitations of strongly confined surface plasmon-polaritons critically rely on their efficient and rapid conversion to lossless channels. We demonstrate a simple, robust, and broad-band butt-coupling technique for connecting a metallic nanowire and a dielectric nanofiber. Conversion efficiencies above 95% in the visible and close to 100% in the near infrared can be achieved with realistic parameters. Moreover, by combining butt-coupling with nanofocusing, we propose a broad-band high-throughput near-field optical microscope.

quant-ph↗

arXiv2009

Control and imaging of single-molecule spectral dynamics using a nano-electrode

We study the influence of a scanning nano-electrode on fluorescence excitation spectra of single terrylene molecules embedded in thin p-terphenyl films at cryogenic temperatures. We show that applied voltages less than 10 V can result in reversible Stark shifts of up to 100 times and linewidth increase greater than 10 times the natural linewidth. We discuss the potential of our experimental scheme for direct imaging of individual two-level systems (TLS) in the nanometer vicinity of single molecules.

physics.chem-ph↗

arXiv2009

Metal nanoparticles in strongly confined beams: transmission, reflection and absorption

We investigate the interaction of tightly focused light with the surface-plasmon-polariton resonances of metal nanospheres. In particular, we compute the scattering and absorption ratios as well as transmission and reflection coefficients. Inspired by our previous work in Ref. [1], we discuss how well a metal nanoparticle approximates a point-like dipolar radiator. We find that a 100 nm silver nanosphere is very close to such an ideal oscillator. Our results have immediate implications for single nanoparticle spectroscopy and microscopy as well as plasmonics.

physics.optics↗

arXiv2008

Coherent State Preparation and Observation of Rabi Oscillations in a Single Molecule

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first step toward coherent manipulation of the electronic states of single molecules with few photons.

quant-ph↗

arXiv2008

Gold, copper, silver and aluminum nanoantennas to enhance spontaneous emission

We compute the decay rates of emitters coupled to spheroidal nanoantennas made of gold, copper, silver, and aluminum. The spectral position of the localized surface plasmon-polariton resonance, the enhancement factors and the quantum efficiency are investigated as a function of the aspect ratio, background index and the metal composing the nanoantenna. While copper yields results similar to gold, silver and aluminum exhibit different performances. Our results show that with a careful choice of the parameters these nanoantennas can enhance emitters ranging from the UV to the near-IR spectrum.

physics.chem-ph↗

arXiv2008

Exploring the limits of single emitter detection in fluorescence and extinction

We present an experimental comparison and a theoretical analysis of the signal-to-noise ratios in fluorescence and extinction spectroscopy of a single emitter. We show that extinction measurements can be advantageous if the emitter is weakly excited. Furthermore, we discuss the potential of this method for the detection and spectroscopy of weakly emitting systems such as rare earth ions.

quant-ph↗

arXiv2007

Plasmon spectra of nanospheres under a tightly focused beam

We study the modification of the far-field cross sections and the near-field enhancement for gold and silver nanospheres illuminated by a tightly focused beam. Using a multipole-expansion approach we obtain an analytical solution to the scattering problem and provide insight on the effects of focusing on the optical response. Large differences with respect to Mie theory are found especially when the nanoparticle supports quadrupole or higher-order resonances.

physics.optics↗