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V. Sandoghdar

Publications and source records attributed to V. Sandoghdar.

At least 19 recordsLinked to original sources

Single organic molecules for photonic quantum technologies

Isolating single molecules in the solid state has allowed fundamental experiments in basic and applied sciences. When cooled down to liquid helium temperature, certain molecules show transition lines, that are tens of megahertz wide, limited only by the excited state lifetime. The extreme flexibility in the synthesis of organic materials provides, at low costs, a wide palette of emission wavelengths and supporting matrices for such single chromophores. In the last decades, the controlled coupling to photonic structures has led to an optimized interaction efficiency with light. Molecules can hence be operated as single photon sources and as non-linear elements with competitive performance in terms of coherence, scalability and compatibility with diverse integrated platforms. Moreover, they can be used as transducers for the optical read-out of fields and material properties, with the promise of single-quanta resolution in the sensing of charges and motion. We show that quantum emitters based on single molecules hold promise to play a key role in the development of quantum science and technologies.

quant-ph

Nano-structured alkali-metal vapor cells

Atom-light interactions in nano-scale systems hold great promise for novel technologies based on integrated emitters and optical modes. We present the design architecture, construction method, and characterization of an all-glass alkali-metal vapor cell with nanometer-scale internal structure. Our cell has a glue-free design which allows versatile optical access, in particular with high numerical aperture optics, and incorporates a compact integrated heating system in the form of an external deposited ITO layer. By performing spectroscopy in different illumination and detection schemes, we investigate atomic densities and velocity distributions in various nanoscopic landscapes. We apply a two-photon excitation scheme to atoms confined in one dimension within our cells, achieving resonance line-widths more than an order of magnitude smaller than the Doppler width. We also demonstrate sub-Doppler line-widths for atoms confined in two dimensions to micron-sized channels. Furthermore, we illustrate control over vapor density within our cells through nano-scale confinement alone, which could offer a scalable route towards room-temperature devices with single atoms within an interaction volume. Our design offers a robust platform for miniaturized devices that could easily be combined with integrated photonic circuits.

physics.atom-ph

Experimental realization of an optical antenna for collecting 99% of photons from a quantum emitter

We present the fabrication and characterization of an optical antenna that converts the dipolar radiation of a quantum emitter to a directional beam with 99% efficiency. Aside from its implications for efficient detection of nanoscopic emitters, this antenna facilitates a deterministic single-photon source with applications in quantum information processing, metrology and sub-shot-noise detection of absorption. We discuss the photophysical limitations of the currently used quantum emitters for the realization of such a device.

quant-ph

Spontaneous emission enhancement of a single molecule by a double-sphere nanoantenna across an interface

We report on two orders of magnitude reduction in the fluorescence lifetime when a single molecule placed in a thin film is surrounded by two gold nanospheres across the film interface. By attaching one of the gold particles to the end of a glass fiber tip, we could control the modification of the molecular fluorescence at will. We find a good agreement between our experimental data and the outcome of numerical calculations.

physics.optics

Single-photon spectroscopy of a single molecule

Exploring the interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest both from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single photons with specific wavelengths, bandwidths and brightness as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a general approach based on the creation of single photons from a single emitter and their use for performing spectroscopy on a second emitter situated at a distance. Although we used organic molecules as emitters, our strategy is readily extendable to other material systems such as quantum dots and color centers. Our work ushers in a new line of experiments that provide access to the coherent and nonlinear couplings of few emitters and few propagating photons.

quant-ph

Controlling the phase of a light beam with a single molecule

We employ heterodyne interferometry to investigate the effect of a single organic molecule on the phase of a propagating laser beam. We report on the first phase-contrast images of individual molecules and demonstrate a single-molecule electro-optical phase switch by applying a voltage to the microelectrodes embedded in the sample. Our results may find applications in single-molecule holography, fast optical coherent signal processing, and single-emitter quantum operations.

quant-ph

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

Single emitters have been considered as sources of single photons in various contexts such as cryptography, quantum computation, spectroscopy, and metrology. The success of these applications will crucially rely on the efficient directional emission of photons into well-defined modes. To accomplish a high efficiency, researchers have investigated microcavities at cryogenic temperatures, photonic nanowires, and near-field coupling to metallic nano-antennas. However, despite an impressive progress, the existing realizations substantially fall short of unity collection efficiency. Here we report on a theoretical and experimental study of a dielectric planar antenna, which uses a layered structure for tailoring the angular emission of a single oriented molecule. We demonstrate a collection efficiency of 96% using a microscope objective at room temperature and obtain record detection rates of about 50 MHz. Our scheme is wavelength-insensitive and can be readily extended to other solid-state emitters such as color centers and semiconductor quantum dots.

quant-ph

A scanning microcavity for in-situ control of single-molecule emission

We report on the fabrication and characterization of a scannable Fabry-Perot microcavity, consisting of a curved micromirror at the end of an optical fiber and a planar distributed Bragg reflector. Furthermore, we demonstrate the coupling of single organic molecules embedded in a thin film to well-defined resonator modes. We discuss the choice of cavity parameters that will allow sufficiently high Purcell factors for enhancing the zero-phonon transition between the vibrational ground levels of the electronic excited and ground states.

quant-ph

Near-infrared single-photons from aligned molecules in ultrathin crystalline films at room temperature

We investigate the optical properties of Dibenzoterrylene (DBT) molecules in a spin-coated crystalline film of anthracence. By performing single molecule studies, we show that the dipole moments of the DBT molecules are oriented parallel to the plane of the film. Despite a film thickness of only 20 nm, we observe an exceptional photostability at room temperature and photon count rates around one million per second from a single molecule. These properties together with an emission wavelength around 800 nm make this system attractive for applications in nanophotonics and quantum optics.

quant-ph

Spontaneous emission of a nanoscopic emitter in a strongly scattering disordered medium

Fluorescence lifetimes of nitrogen-vacancy color centers in individual diamond nanocrystals were measured at the interface between a glass substrate and a strongly scattering medium. Comparison of the results with values recorded from the same nanocrystals at the glass-air interface revealed fluctuations of fluorescence lifetimes in the scattering medium. After discussing a range of possible systematic effects, we attribute the observed lengthening of the lifetimes to the reduction of the local density of states. Our approach is very promising for exploring the strong three-dimensional localization of light directly on the microscopic scale.

quant-ph

Single-Photon Imaging and Efficient Coupling to Single Plasmons

We demonstrate strong coupling of single photons emitted by individual molecules at cryogenic and ambient conditions to individual nanoparticles. We provide images obtained both in transmission and reflection, where an efficiency greater than 55% was achieved in converting incident narrow-band photons to plasmon-polaritons (plasmons) of a silver nanoparticle. Our work paves the way to spectroscopy and microscopy of nano-objects with sub-shot noise beams of light and to triggered generation of single plasmons and electrons in a well-controlled manner.

quant-ph

Quantum Interference of Tunably Indistinguishable Photons from Remote Organic Molecules

We demonstrate two-photon interference using two remote single molecules as bright solid-state sources of indistinguishable photons. By varying the transition frequency and spectral width of one molecule, we tune and explore the effect of photon distinguishability. We discuss future improvements on the brightness of single-photon beams, their integration by large numbers on chips, and the extension of our experimental scheme to coupling and entanglement of distant molecules.

quant-ph

Molecules as Sources for Indistinguishable Single Photons

We report on the triggered generation of indistinguishable photons by solid-state single-photon sources in two separate cryogenic laser scanning microscopes. Organic fluorescent molecules were used as emitters and investigated by means of high resolution laser spectroscopy. Continuous-wave photon correlation measurements on individual molecules proved the isolation of single quantum systems. By using frequency selective pulsed excitation of the molecule and efficient spectral filtering of its emission, we produced triggered Fourier-limited single photons. In a further step, local electric fields were applied to match the emission wavelengths of two different molecules via Stark effect. Identical single photons are indispensible for the realization of various quantum information processing schemes proposed. The solid-state approach presented here prepares the way towards the integration of multiple bright sources of single photons on a single chip.

quant-ph

Coupling of plasmonic nanoparticles to their environments in the context of van der Waals-Casimir interactions

We present experiments in which the interaction of a single gold nanoparticle with glass substrates or with another gold particle can be tuned by in-situ control of their separations using scanning probe technology. We record the plasmon resonances of the coupled systems as a function of the polarization of the incident field and the particle position. The distinct spectral changes of the scattered light from the particle pair are in good agreement with the outcome of finite difference time-domain (FDTD) calculations. We believe our experimental technique holds promise for the investigation of the van der Waals-Casimir type interactions between nanoscopic neutral bodies.

quant-ph

Perfect Reflection of Light by an Oscillating Dipole

We show theoretically that a directional dipole wave can be perfectly reflected by a single point-like oscillating dipole. Furthermore, we find that in the case of a strongly focused plane wave up to 85 % of the incident light can be reflected by the dipole. Our results hold for the full spectrum of the electromagnetic interactions and have immediate implications for achieving strong coupling between a single propagating photon and a single quantum emitter.

quant-ph

Extinction imaging of a single quantum emitter in its bright and dark states

Room temperature detection of single quantum emitters has had a broad impact in fields ranging from biophysics to material science, photophysics, or even quantum optics. These experiments have exclusively relied on the efficient detection of fluorescence. An attractive alternative would be to employ direct absorption, or more correctly expressed "extinction" measurements. Indeed, small nanoparticles have been successfully detected using this scheme in reflection and transmission. Coherent extinction detection of single emitters has also been reported at cryogenic temperatures, but their room temperature implementation has remained a great laboratory challenge owing to the expected weak signal-to-noise ratio. Here we report the first extinction study of a single quantum emitter at ambient condition. We obtain a direct measure for the extinction cross section of a single semiconductor nanocrystal both during and in the absence of fluorescence, for example in the photobleached state or during blinking off-times. Our measurements pave the way for the detection and absorption spectroscopy of single molecules or clusters of atoms even in the quenched state.

cond-mat.other

Modifcation of single molecule fluorescence close to a nanostructure: radiation pattern, spontaneous emission and quenching

The coupling of nanostructures with emitters opens ways for the realization of man-made subwavelength light emitting elements. In this article, we investigate the modification of fluorescence when an emitter is placed close to a nanostructure. In order to control the wealth of parameters that contribute to this process, we have combined scanning probe technology with single molecule microscopy and spectroscopy. We discuss the enhancement and reduction of molecular excitation and emission rates in the presence of a dielectric or metallic nanoparticle and emphasize the role of plasmon resonances in the latter. Furthermore, we examine the spectral and angular emission characteristics of the molecule-particle system. Our experimental findings are in excellent semi-quantitative agreement with the outcome of theoretical calculations. We express our results in the framework of optical nanoantennae and propose arrangements that could lead to the modification of spontaneous emission by more than 1000 times.

cond-mat.other

Realization of two Fourier-limited solid-state single-photon sources

We demonstrate two solid-state sources of indistinguishable single photons. High resolution laser spectroscopy and optical microscopy were combined at T = 1.4 K to identify individual molecules in two independent microscopes. The Stark effect was exploited to shift the transition frequency of a given molecule and thus obtain single photon sources with perfect spectral overlap. Our experimental arrangement sets the ground for the realization of various quantum interference and information processing experiments.

quant-ph