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Brahim Lounis

Publications and source records attributed to Brahim Lounis.

At least 19 recordsLinked to original sources

Addressing the correlation of Stokes-shifted photons emitted from two quantum emitters

In resonance fluorescence excitation experiments, light emitted from solid-state quantum emitters is typically filtered to eliminate the laser photons, ensuring that only red-shifted Stokes photons are detected. However, theoretical analyses of the fluorescence intensity correlation often model emitters as two-level systems, focusing on light emitted exclusively from the purely electronic transition (the zero-phonon line), or they rely on statistical approaches based on conditional probabilities that neglect the quantum coherence between the emitters and the coherence between the electric fields they generate. Here, we propose a model to characterize the correlation of either zero-phonon line photons or Stokes-shifted photons. This model successfully reproduces the experimental correlation of Stokes-shifted photons emitted from two interacting molecules and predicts that this correlation is affected by quantum coherence. Besides, we analyze the role of quantum coherence in the Stokes-shifted emission from two distant emitters, showing a sharp peak at zero time delay due to the Hanbury Brown--Twiss effect.

quant-ph

Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films

Colloidal perovskite quantum dots (PQDs) are an exciting platform for on-demand quantum, and classical optoelectronic and photonic devices. However, their potential success is limited by the extreme sensitivity and low stability arising from their weak intrinsic lattice bond energy and complex surface chemistry. Here we report a novel platform of buried perovskite quantum dots (b-PQDs) in a three-dimensional perovskite thin-film, fabricated using one-step, flash annealing, which overcomes surface related instabilities in colloidal perovskite dots. The b-PQDs demonstrate ultrabright and stable single-dot emission, with resolution-limited linewidths below 130 {\mu}eV, photon-antibunching (g^2(0)=0.1), no blinking, suppressed spectral diffusion, and high photon count rates of 10^4/s, consistent with unity quantum yield. The ultrasharp linewidth resolves exciton fine-structures (dark and triplet excitons) and their dynamics under a magnetic field. Additionally, b-PQDs can be electrically driven to emit single photons with 1 meV linewidth and photon-antibunching (g^2(0)=0.4). These results pave the way for on-chip, low-cost single-photon sources for next generation quantum optical communication and sensing.

physics.optics

Sub-nanosecond coherent optical manipulation of a single aromatic molecule at cryogenic temperature

Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on-off intensity ratio ($\sim 3\times 10^5$) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2$^\circ$K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5$^\circ$K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.

physics.optics

Nonlinear Optics of optomagnetics: Quantum and Classical Treatments

Optomagnetics emerges as a growing field of research cross-linking optics, magnetism and material science. Here, we provide a microscopic quantum mechanical and a macroscopic classical models to describe optomagnetic effects from nonlinear optics point of view. Our self-consistent quantum mechanical formulation considers all orders of perturbing field and results not only in finding generalized Pitaevskii's relationship, where photoinduced magnetization can be expanded in terms of light power, but also provide compact and analytical expressions for optical gyration vector coefficients. classical treatment is then developed based on the anharmonic Drude-Lorentz model showing that the photo-induced DC magnetization is proportional to odd harmonics of the light power. The difference in quantum and classical results are revealed and discussed. Having a pomp-probe setup in mind, we describe how a probe light signal can propagate down an optomagnetic medium, i.e. a medium that is magnetized by intense circularly-polarized pump light, via its permittivity tensor and find light propagation characteristics. Inverse Faraday and Cotton-Mouton Effects are discussed as a result of circular and linear birefringences and their Verdet constants have been analytically found.

physics.optics

Memories in the Photoluminescence Intermittency of Single Cesium Lead Bromide Nanocrystals

Single cesium lead bromide (CsPbBr3) nanocrystals show strong photoluminescence blinking, with on- and off- dwelling times following power-law distributions. We investigate the memory effect in the photoluminescence blinking of single CsPbBr3 nanocrystals and find positive correlations for successive on-times and successive off-times. This memory effect is not sensitive to the nature of the surface capping ligand and the embedding polymer. These observations suggest that photoluminescence intermittency and its memory are mainly controlled by intrinsic traps in the nanocrystals. These findings will help optimizing light-emitting devices based on inorganic perovskite nanocrystals.

physics.app-ph

Generation of photoluminescent ultrashort carbon nanotubes through nanoscale exciton localization at sp3 -defect sites

The intrinsic near-infrared photoluminescence observed in long single walled carbon nanotubes is systematically quenched in ultrashort single-walled carbon nanotubes (usCNTs, below 100 nm length) due to their short dimension as compared to the exciton diffusion length. It would however be key for number of applications to have such tiny nanostructure displaying photoluminescence emission to complement their unique physical, chemical and biological properties. Here we demonstrate that intense photoluminescence can be created in usCNTs (~40 nm length) upon incorporation of emissive sp3-defect sites in order to trap excitons. Using super-resolution imaging at <25 nm resolution, we directly reveal the localization of excitons at the defect sites on individual usCNTs. They are found preferentially localized at nanotube ends which can be separated by less than 40 nm and behave as independent emitters. The demonstration and control of bright near-infrared photoluminescence in usCNTs through exciton trapping opens the possibility to engineering tiny carbon nanotubes for applications in various domains of research including quantum optics and bioimaging.

physics.app-ph

The 2015 super-resolution microscopy roadmap

Far-field optical microscopy using focused light is an important tool in a number of scientific disciplines including chemical, (bio)physical and biomedical research, particularly with respect to the study of living cells and organisms. Unfortunately, the applicability of the optical microscope is limited, since the diffraction of light imposes limitations on the spatial resolution of the image. Consequently the details of, for example, cellular protein distributions, can be visualized only to a certain extent. Fortunately, recent years have witnessed the development of 'super-resolution' far-field optical microscopy (nanoscopy) techniques such as stimulated emission depletion (STED), ground state depletion (GSD), reversible saturated optical (fluorescence) transitions (RESOLFT), photoactivation localization microscopy (PALM), stochastic optical reconstruction microscopy (STORM), structured illumination microscopy (SIM) or saturated structured illumination microscopy (SSIM), all in one way or another addressing the problem of the limited spatial resolution of far-field optical microscopy. While SIM achieves a two-fold improvement in spatial resolution compared to conventional optical microscopy, STED, RESOLFT, PALM/STORM, or SSIM have all gone beyond, pushing the limits of optical image resolution to the nanometer scale. Consequently, all super-resolution techniques open new avenues of biomedical research. Because the field is so young, the potential capabilities of different super-resolution microscopy approaches have yet to be fully explored, and uncertainties remain when considering the best choice of methodology. Thus, even for experts, the road to the future is sometimes shrouded in mist. The super-resolution optical microscopy roadmap of Journal of Physics D: Applied Physics addresses this need for clarity. It provides guidance to the outstanding questions through a collection of short review articles from experts in the field, giving a thorough discussion on the concepts underlying super-resolution optical microscopy, the potential of different approaches, the importance of label optimization (such as reversible photoswitchable proteins) and applications in which these methods will have a significant impact.

physics.bio-ph

Small Gold Nanorods with Tunable Absorption for Photothermal Microscopy in Cells

Over the last decade, single-molecule optical microscopy has become the gold-standard approach to decipher complex molecular processes in cellular environments. [1-3] Single-molecule fluorescence microscopy has several advantages such as ease of application, high sensitivity, low invasiveness and versatility due the large number of available fluorescent probes. It bears however some drawbacks related to the poor photostability of organic dye molecules [4] and auto-fluorescent proteins [5-7] and and to the relatively large size of semiconductor nanoparticles in the context of live cell applications. [4,8,9] The overall size of the functional biomarkers is a general issue for any imaging approach because of steric hindrance effects in confined cell regions. Small red-shifted nano-emitters that are highly photostable are not currently available, while they would combine the best physical and optical penetration properties in biological tissues. Although single-molecule absorption microscopy was early used to detect single-molecules [10] at cryogenic temperatures, it is only with the advent of photothermal microscopy [11,12] that practical applications of absorption microscopy were developed in single-molecule research. Photothermal imaging (PhI)

physics.bio-ph

A solid state source of photon triplets based on quantum dot molecules

Producing advanced quantum states of light is a priority in quantum information technologies. While remarkable progress has been made on single photons and photon pairs, multipartite correlated photon states are usually produced in purely optical systems by post-selection or cascading, with extremely low efficiency and exponentially poor scaling. Multipartite states enable improved tests of the foundations of quantum mechanics as well as implementations of complex quantum optical networks and protocols. It would be favorable to directly generate these states using solid state systems, for better scaling, simpler handling, and the promise of reversible transfer of quantum information between stationary and flying qubits. Here we use the ground states of two optically active coupled quantum dots to directly produce photon triplets. The wavefunctions of photogenerated excitons localized in these ground states are correlated via molecular hybridization and Coulomb interactions. The formation of a triexciton leads to a triple cascade recombination and sequential emission of three photons with strong correlations. The quantum dot molecule is embedded in an epitaxially grown nanowire engineered for single-mode waveguiding and improved extraction efficiency at the emission wavelength. We record 65.62 photon triplets per minute, surpassing rates of all earlier reported sources, in spite of the moderate efficiency of our detectors. Our structure and data represent a breakthrough towards implementing multipartite photon entanglement and multi-qubit readout schemes in solid state devices, suitable for integrated quantum information processing.

quant-ph

Identification and super-resolution imaging of ligand-activated receptor dimers in live cells

Molecular interactions are key to many chemical and biological processes like protein function. In many signaling processes they occur in sub-cellular areas displaying nanoscale organizations and involving molecular assemblies. The nanometric dimensions and the dynamic nature of the interactions make their investigations complex in live cells. While super-resolution fluorescence microscopies offer live-cell molecular imaging with sub-wavelength resolutions, they lack specificity for distinguishing interacting molecule populations. Here we combine super-resolution microscopy and single-molecule Förster Resonance Energy Transfer (FRET) to identify dimers of receptors induced by ligand binding and provide super-resolved images of their membrane distribution in live cells. By developing a two-color universal-Point-Accumulation-In-the-Nanoscale-Topography (uPAINT) method, dimers of epidermal growth factor receptors (EGFR) activated by EGF are studied at ultra-high densities, revealing preferential cell-edge sub-localization. This methodology which is specifically devoted to the study of molecules in interaction, may find other applications in biological systems where understanding of molecular organization is crucial.

physics.bio-ph

Metrological Investigation of the (6,5) Carbon Nanotube Absorption Cross Section

Using single-nanotube absorption microscopy, we measured the absorption cross section of (6,5) carbon nanotubes at their second-order optical transition. We obtained a value of 3.2 10-17 cm2/C atom with a precision of 15% and an accuracy below 20%. This constitutes the first metrological investigation of the absorption cross section of chirality-identified nanotubes. Correlative absorption-luminescence microscopies performed on long nanotubes reveal a direct manifestation of exciton diffusion in the nanotube.

cond-mat.mes-hall

Massive Parallelization of STED Nanoscopy Using Optical Lattices

Recent developments in stimulated emission depletion (STED) microscopy achieved nanometer scale resolution and showed great potential in live cell imaging. Yet, STED nanoscopy techniques are based on single point-scanning. This constitutes a drawback for wide field imaging, since the gain in spatial resolution requires dense pixelation and hence long recording times. Here we achieve massive parallelization of STED nanoscopy using wide-field excitation together with well-designed optical lattices for depletion and a fast camera for detection. Acquisition of large field of view super-resolved images requires scanning over a single unit cell of the optical lattice which can be as small as 290 nm*290nm. Interference STED (In-STED) images of 2.9 μm* 2.9 μm with resolution down to 70 nm are obtained at 12.5 frames per second. The development of this technique opens many prospects for fast wide-field nanoscopy.

physics.bio-ph

Mechanism of Electrolyte-Induced Brightening in Single-Wall Carbon Nanotubes

While addition of electrolyte to sodium dodecyl sulfate suspensions of single-wall carbon nanotubes has been demonstrated to result in significant brightening of the nanotube photoluminescence (PL), the brightening mechanism has remained unresolved. Here, we probe this mechanism using time-resolved PL decay measurements. We find that PL decay times increase by a factor of 2 on addition of CsCl as the electrolyte. Such an increase directly parallels an observed near-doubling of PL intensity, indicating the brightening results primarily from changes in nonradiative decay rates associated with exciton diffusion to quenching sites. Our findings indicate that a reduced number of these sites results from electrolyte-induced reorientation of the surfactant surface structure that partially removes pockets of water from the tube surface where excitons can dissociate, and thus underscores the contribution of interfacial water in exciton recombination processes.

cond-mat.mtrl-sci

A highly specific gold nanoprobe for live-cell single-molecule imaging

Single molecule tracking in live cells is the ultimate tool to study subcellular protein dynamics, but it is often limited by the probe size and photostability. Due to these issues, long-term tracking of proteins in confined and crowded environments, such as intracellular spaces, remains challenging. We have developed a novel optical probe consisting of 5-nm gold nanoparticles functionalized with a small fragment of camelid antibodies that recognize widely used GFPs with a very high affinity, which we call GFP-nanobodies. These small gold nanoparticles can be detected and tracked using photothermal imaging for arbitrarily long periods of time. Surface and intracellular GFP-proteins were effectively labeled even in very crowded environments such as adhesion sites and cytoskeletal structures both in vitro and in live cell cultures. These nanobody-coated gold nanoparticles are probes with unparalleled capabilities; small size, perfect photostability, high specificity, and versatility afforded by combination with the vast existing library of GFP-tagged proteins.

physics.bio-ph

Biexciton, single carrier, and trion generation dynamics in single-walled carbon nanotubes

We present a study of free carrier photo-generation and multi-carrier bound states, such as biexcitons and trions (ionized excitons), in semiconducting single-walled carbon nanotubes. Pump-and-probe measurements performed with fs pulses reveal the effects of strong Coulomb interactions between carriers on their dynamics. Biexciton formation by optical transition from exciton population results in an induced absorption line (binding energy 130 meV). Exciton-exciton annihilation process is shown to evolve at high densities towards an Auger process that can expel carriers from nanotubes. The remaining carriers give rise to an induced absorption due to trion formation (binding energy 190 meV). These features show the dynamics of exciton and free carriers populations.

cond-mat.mes-hall

Single molecule detection of nanomechanical motion

We investigate theoretically how single-molecule spectroscopy techniques can be used to perform fast and high resolution displacement detection and manipulation of nanomechanical oscillators, such as singly clamped carbon nanotubes. We analyze the possibility of real time displacement detection by the luminescence signal and of displacement fluctuations by the degree of second order coherence. Estimates of the electro-mechanical coupling constant indicate that intriguing regimes of strong back-action between the two-level system of a molecule and the oscillator can be realized.

cond-mat.mes-hall

Nanoscale Thermotropic Phase Transitions Enhance Photothermal Microscopy Signals

The photothermal heterodyne imaging technique enabled studies of individual weakly absorbing nano-objects in various environments. It uses a photo-induced change in the refractive index of the environment. Taking advantage of the dramatic index of refraction change occurring around a thermotropic liquid crystalline phase transition, we demonstrate a 40-fold signal-to-noise ratio enhancement for gold nanoparticles imaged in 4-Cyano-4'-pentylbiphenyl (5CB) liquid crystals over those in a water environment. We studied the photothermal signal as a function of probe laser polarization, heating power, and sample temperature quantifying the optimal enhancement. This study established photothermal microscopy as a valuable technique for inducing and/or detecting local phase transitions at the nanometer scales.

physics.optics

Luminescence Properties of Individual Empty and Water-filled Single-Walled Carbon Nanotubes

The influence of water-filling on the photoluminescence (PL) properties of SWCNTs is studied by ensemble and single-molecule PL spectroscopy. Red-shifted PL and PL excitation spectra are observed upon water filling for 16 chiralities and can be used to unambiguously distinguish empty SWCNTs from filled ones. The effect of water-filling on the optical transitions is well reproduced by a continuum dielectric constant model previously developed to describe the influence of the nanotube outer environment. Empty nanotubes display narrower luminescence lines and lower inhomogeneous broadening, signatures of reduced extrinsic perturbations. The radial breathing mode (RBM) phonon side band is clearly observed in the PL spectrum of small diameter empty tubes and a strong exciton-phonon coupling is measured for this vibration. Biexponential PL decays are observed for empty and water filled tubes, and only the short living component is influenced by the water-filling. This may be attributed to a shortening of the radiative lifetime of the bright state by the inner dielectric environment.

cond-mat.mes-hall