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Jean-Sébastien Lauret

Publications and source records attributed to Jean-Sébastien Lauret.

At least 19 recordsLinked to original sources

Critical dephasing rates for the observation of collective behavior in a pair of coupled quantum emitters

Efficient atom-photon interfaces require the controlled assembly of quantum emitters, where collective effects such as superradiance and subradiance can emerge. Recent experiments with subwavelength arrays of quantum dots have reported superradiance at room temperature, revealing a delicate competition between collective enhancement of coherent emission and pure dephasing $γ^*$, which destroys it. Motivated by these results, we theoretically study $N=2$ coupled quantum emitters and identify threshold values of $γ^*$, for four experimentally accessible observables, beyond which collective effects vanish. The thresholds depend sensitively on the chosen observable, highlighting the subtlety of detecting collective behavior. Our work provides a quantitative framework to guide experiments and optimize conditions for observing collective quantum phenomena.

quant-ph↗

Collective Fluorescence of Graphene Quantum Dots on a surface

This study explores the organization of graphene quantum dots on the surface of monocrystalline halide perovskite. We show that graphene quantum dots tends to aggregate on the surface of perovskite unlike in solution or on other substrates, even at very low concentration of the initial solution that should yield single-molecule samples. Spectral analysis on small clusters shows a back-and-forth dynamical transition between an uncoupled, monomer-like state, and an excimer state. Following this "dance" between states, a drastic one-way increase in fluorescence intensity combined with a shortening of the excited state lifetime has been observed on some clusters. This behavior is related to the emission of a collective state that may be a consequence of the dynamical organization of graphene quantum dots under illumination on the surface of the perovksite.

cond-mat.mes-hall↗

Shortcuts to equilibrium with a levitated particle in the underdamped regime

We report on speeding up equilibrium recovery in the previously unexplored general case of the underdamped regime using an optically levitated particle. We accelerate the convergence towards equilibrium by an order of magnitude compared to the natural relaxation time. We then discuss the efficiency of the studied protocols, especially for a multidimensional system. These results pave the way for optimizing realistic nanomachines with application to sensing and developing efficient nano-heat engines.

cond-mat.stat-mech↗

Thermometry of an optically levitated nanodiamond

Using the spin properties of nitrogen-vacancy (NV) centers in levitated diamond, we characterize the absorption of single nanodiamonds. We first calibrate the thermometry response of the NV centers embedded in our nanodiamonds. Then, using this calibration, we estimate the absorption cross-section of single levitated nanodiamonds. We show that this absorption is extrinsic and dominated by volumic effects. Our work opens the way to diamond materials optimization for levitation quantum experiments. It also demonstrates optical levitation as a unique platform to characterize material thermal properties at the nanoparticle level.

quant-ph↗

Hot Brownian motion of optically levitated nanodiamonds

The Brownian motion of a particle hotter than its environment is an iconic out-of-equilibrium system. Its study provides valuable insights into nanoscale thermal effects. Notably, it supplies an excellent diagnosis of thermal effects in optically levitated particles, a promising platform for force sensing and quantum physics tests. Thus, understanding the relevant parameters in this effect is critical. In this context, we test the role of particles' shape and material, using optically levitated nanodiamonds hosting NV centers to measure the particles' internal temperature and center-of-mass dynamics. We present a model to assess the nanodiamond internal temperature from its dynamics, adaptable to other particles. We also demonstrate that other mechanisms affect the nanodiamond dynamics and its stability in the trap. Finally, our work, by showing levitating nanodiamonds as an excellent tool for studying nano-thermal effects, opens prospects for increasing the trapping stability of optically levitated particles.

quant-ph↗

Directing random lasing emission using cavity exciton-polaritons

Random lasing is an intriguing phenomenon occurring in disordered structures with optical gain. In such lasers, the scattering of light provides the necessary feedback for lasing action. Because of the light scattering, the random lasing systems emit in all the directions in contrast with the directional emission of the conventional lasers. While this property can be desired in some cases, the control of the emission directionality remains required for most of the applications. Besides, it is well known that the excitation of cavity exciton-polaritons is intrinsically directional. Each wavelength (energy) of the cavity polariton, which is a superposition of an excitonic state and a cavity mode, corresponds to a well-defined propagation direction. We demonstrate in this article that coupling the emission of a 2D random laser with a cavity polaritonic resonance permits to control the direction of emission of the random laser. This results in a directional random lasing whose emission angle with respect to the microcavity axis can be tuned in a large range of angles by varying the cavity detuning. The emission angles reached experimentally in this work are 15.8$^\circ$ and 22.4$^\circ$.

physics.optics↗

Super-localization of excitons in carbon nanotubes at cryogenic temperature

At cryogenic temperature and at the single emitter level, the optical properties of single-wall carbon nanotubes depart drastically from that of a one-dimensional (1D) object. In fact, the (usually unintentional) localization of excitons in local potential wells leads to nearly 0D behaviors such as photon antibunching, spectral diffusion, inhomogeneous broadening, etc. Here, we present an hyperspectral imaging of this exciton self-localization effect at the single nanotube level using a super-resolved optical microscopy approach. We report on the statistical distribution of the traps localization, depth and width. We use a quasi-resonant photoluminescence excitation approach to probe the confined quantum states. Numerical simulations of the quantum states and exciton diffusion show that the excitonic states are deeply modified by the interface disorder inducing a remarkable discretization of the excitonic absorption spectrum and a quenching of the free 1D exciton absorption.

cond-mat.mes-hall↗

Room temperature cavity polaritons with 3D hybrid perovskite - Towards low-cost polaritonic devices

Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons are experimentallly demonstrated from both reflectivity and photoluminescence experiments, at room temperature, in a 3$λ$/2 planar microcavity containing a large surface spin-coated $CH_3NH_3PbBr_3$ thin film. A microcavity quality factor of 92 was found and a large Rabi splitting of 70 meV was measured. This result paves the way to low-cost polaritonic devices operating at room temperature, potentially electrically injectable as 3D hybrid perovskites present good transport properties.

physics.optics↗

Exploiting one-dimensional exciton-phonon coupling for tunable and efficient single-photon generation with a carbon nanotube

Condensed-matter emitters offer enriched cavity quantum electrodynamical effects due to the coupling to external degrees of freedom. In the case of carbon nanotubes a very peculiar coupling between localized excitons and the one-dimensional acoustic phonon modes can be achieved, which gives rise to pronounced phonon wings in the luminescence spectrum. By coupling an individual nanotube to a tunable optical micro-cavity, we show that this peculiar exciton-phonon coupling is a valuable resource to enlarge the tuning range of the single-photon source while keeping an excellent exciton-photon coupling efficiency and spectral purity. Using the unique flexibility of our scanning fiber cavity, we are able to measure the efficiency spectrum of the very same nanotube in the Purcell regime for several mode volumes. Whereas this efficiency spectrum looks very much like the free-space luminescence spectrum when the Purcell factor is small (large mode volume), we show that the deformation of this spectrum at lower mode volumes can be traced back to the strength of the exciton-photon coupling. It shows an enhanced efficiency on the red wing that arises from the asymmetry of the incoherent energy exchange processes between the exciton and the cavity. This allows us to obtain a tuning range up to several hundred times the spectral width of the source.

cond-mat.mes-hall↗

Structural Properties of Double-Walled Carbon Nanotubes driven by Mechanical Interlayer Coupling

Structural identification of double-walled carbon nanotubes (DWNT) is presented through a robust procedure based on the latest generation of transmission electron microscope, making possible a statistical analysis based on numerous nano-objects. This approach reveals that inner and outer tubes of DWNTs are not randomly oriented, suggesting the existence of a mechanical coupling between the two concentric walls. With the support of atomic scale modelisations, we attribute it to the presence of incommensurate domains whose structures depend on the diameters and helicities of both tubes, and where inner tubes try to achieve a local stacking orientation to reduce strain effects.

cond-mat.mtrl-sci↗

Excitonic Emission in Organic-Inorganic Lead Iodide Perovskite Single Crystals

Hybrid perovskite thin films have demonstrated impressive performance for solar energy conversion and optoelectronic applications. However, further progress will benefit from a better knowledge of the intrinsic photophysics of materials. Here, the low temperature emission properties of CH3NH3PbI3 single crystals are investigated and compared to those of thin polycrystalline films by means of steady-state and time-resolved photoluminescence spectroscopy. While the emission properties of thin films and crystals appear relatively similar at room temperature, low temperature photoluminescence spectroscopy reveals striking differences between the two materials. Single crystals photoluminescence exhibits a sharp excitonic emission at high energy, with Full Width at Half Maximum of only 5 meV, assigned to free excitonic recombination and a broad band at low energy. We analyzed the thermal evolution of the free excitonic intensity and linewidth. An excitonic binding energy of 28 meV is extracted from the quenching of the photoluminescence. We highlight a strong broadening of the emission due to LO phonon coupling. The free excitonic emission turned to be very short-lived with a sub-nanosecond dynamics, mainly induced by the fast trapping of the excitons. The free excitonic emission is completely absent of the thin films spectra, which are dominated by trap states band. The trap states energies, width and recombination dynamics present important similarities between films and crystals. These results suggest that the trap states are formed at the surface and grain interface of perovskites.

cond-mat.mtrl-sci↗

Widely tunable single-photon source from a carbon nanotube in the Purcell regime

Single-Wall Carbon Nanotubes (SWNTs) are among the very few candidates for single-photon sources operating in the telecom bands since they exhibit large photon antibunching up to room temperature. However, coupling a nanotube to a photonic structure is highly challenging because of the random location and emission wavelength in the growth process. Here, we demonstrate the realization of a widely tunable single-photon source by using a carbon nanotube inserted in an original repositionable fiber micro-cavity : we fully characterize the emitter in the free-space and subsequently form the cavity around the nanotube. This brings an invaluable insight into the emergence of quantum electrodynamical effects. We observe an efficient funneling of the emission into the cavity mode with a strong sub-Poissonian statistics together with an up to 6-fold Purcell enhancement factor. By exploiting the cavity feeding effect on the phonon wings, we locked the single-photon emission at the cavity frequency over a 4~THz-wide band while keeping the mode width below 80~GHz. This paves the way to multiplexing and multiple qubit coupling.

cond-mat.mes-hall↗

Universal non-resonant absorption in carbon nanotubes

Photoluminescence excitation measurements in semi-conducting carbon nanotubes show a systematic non-resonant contribution between the well known excitonic resonances. Using a global analysis method, we were able to delineate the contribution of each chiral species including its tiny non-resonant component. By comparison with the recently reported excitonic absorption cross-section on the $S_{22}$ resonance, we found a universal non-resonant absorbance which turns out to be of the order of one half of that of an equivalent graphene sheet. This value as well as the absorption line-shape in the non-resonant window is in excellent agreement with microscopic calculations based on the density matrix formalism. This non-resonant absorption of semi-conducting nanotubes is essentially frequency independent over 0.5~eV wide windows and reaches approximately the same value betweeen the $S_{11}$ and $S_{22}$ resonances or between the $S_{22}$ and $S_{33}$ resonances. In addition, the non-resonant absorption cross- section turns out to be the same for all the chiral species we measured in this study. From a practical point of view, this study puts firm basis on the sample content analysis based on photoluminescence studies by targeting specific excitation wavelengths that lead to almost uniform excitation of all the chiral species of a sample within a given diameter range.

cond-mat.mes-hall↗

Quantum confinement of zero-dimensional hybrid organic-inorganic polaritons at room temperature

We report on the quantum confinement of zero-dimensional polaritons in perovskite-based microcavity at room temperature. Photoluminescence of discrete polaritonic states are observed for polariton localized in symmetric sphere-like defects which are spontaneously nucleated on the top dielectric Bragg mirror. The linewidth of these confined states are found much sharper (almost one order of magnitude) than that of photonic modes in the perovskite planar microcavity. Our results show the possibility to study organic-inorganic cavity polariton in confined microstructure and suggest a fabrication method to realize integrated polaritonic devices operating at room temperature.

cond-mat.mes-hall↗

Unifying the low-temperature photoluminescence spectra of carbon nanotubes: the role of acoustic phonon confinement

At low temperature the photoluminescence of single-wall carbon nanotubes show a large variety of spectral profiles ranging from ultra narrow lines in suspended nanotubes to broad and asymmetrical line-shapes that puzzle the current interpretation in terms of exciton-phonon coupling. Here, we present a complete set of photoluminescence profiles in matrix embedded nanotubes including unprecedented narrow emission lines. We demonstrate that the diversity of the low-temperature luminescence profiles in nanotubes originates in tiny modifications of their low-energy acoustic phonon modes. When low energy modes are locally suppressed, a sharp photoluminescence line as narrow as 0.7 meV is restored. Furthermore, multi-peak luminescence profiles with specific temperature dependence show the presence of confined phonon modes.

cond-mat.mes-hall↗

Chirality dependence of the absorption cross-section of carbon nanotubes

The variation of the optical absorption of carbon nanotubes with their geometry has been a long standing question at the heart of both metrological and applicative issues, in particular because optical spectroscopy is one of the primary tools for the assessment of the chiral species abundance of samples. Here, we tackle the chirality dependence of the optical absorption with an original method involving ultra-efficient energy transfer in porphyrin/nanotube compounds that allows uniform photo-excitation of all chiral species. We measure the absolute absorption cross-section of a wide range of semiconducting nanotubes at their S22 transition and show that it varies by up to a factor of 2.2 with the chiral angle, with type I nanotubes showing a larger absorption. In contrast, the luminescence quantum yield remains almost constant.

cond-mat.mes-hall↗

Coupled study by TEM/EELS and STM/STS of electronic properties of C- and CNx-nanotubes

Carbon nanotubes are the focus of considerable research efforts due to their fascinating physical properties. They provide an excellent model system for the study of one dimensional materials and molecular electronics. The chirality of nanotubes can lead to very different electronic behaviours, either metallic or semiconducting. Their electronic spectrum consists of a series of Van Hove singularities defining a bandgap for semiconducting tubes and molecular orbitals at the corresponding energies. A promising way to tune the nanotubes electronic properties for future applications is to use doping by heteroatoms. Here we report on experimental investigation of the role of many-body interactions in nanotube bandgaps, the visualization in direct space of the molecular orbitals of nanotubes and the properties of nitrogen doped nanotubes using scanning tunneling microscopy and transmission electron microscopy as well as electron energy loss spectroscopy.

cond-mat.mtrl-sci↗

Measuring many-body effects in carbon nanotubes with a scanning tunneling microscope

Electron-electron interactions and excitons in carbon nanotubes are locally measured by combining Scanning tunneling spectroscopy and optical absorption in bundles of nanotubes. The largest gap deduced from measurements at the top of the bundle is found to be related to the intrinsic quasi-particle gap. From the difference with optical transitions, we deduced exciton binding energies of 0.4 eV for the gap and 0.7 eV for the second Van Hove singularity. This provides the first experimental evidence of substrate-induced gap renormalization on SWNTs.

cond-mat.mtrl-sci↗