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Christophe Voisin

Publications and source records attributed to Christophe Voisin.

At least 19 recordsLinked to original sources

Optical properties of single CsPbBr3 perovskite quantum dots synthesized by a modified ligand-assisted reprecipitation method

Colloidal perovskite quantum dots (pQDs) are promising quantum light emitters, and investigations at the single pQD scale have so far relied mostly on hot-injection synthesis, which requires precise temperature control and an inert atmosphere. While alternative synthesis routes under milder conditions are often associated with structural and surface defects that may have limited impact in ensemble measurements, demonstrating high optical quality at the level of individual pQDs constitutes the most stringent benchmark for a new synthesis protocol. Here, we demonstrate that a modified ligand-assisted reprecipitation (LARP) approach yields CsPbBr3 pQDs showing state-of-the-art optical properties at the scale of single emitters. By combining an amine-mediated post-synthetic size-trimming strategy with didodecyldimethylammonium bromide (DDAB) ligands for enhanced surface passivation and colloidal stability, we obtain isolated pQDs with stable emission and minimal spectral diffusion at cryogenic temperatures. Micro-photoluminescence experiments resolve the characteristic fine structure of the bright exciton, its low-energy optical phonon replicas, and the trion and biexciton states. Time-resolved and photon correlation measurements show a ~90 ps lifetime and high purity single photon emission, respectively. These results demonstrate that modified LARP synthesis constitutes an accessible alternative to hot injection, preserving the intrinsic excitonic and quantum optical properties of individual pQDs while offering greater flexibility for post-synthetic ligand engineering, as exemplified here by the use of DDAB for surface passivation.

cond-mat.mes-hall

Localized emission in MoSe$_2$ monolayers on GaN nanopillars

Solid-state quantum emitters (QEs) in two-dimensional semiconductors offer compact, chip-compatible sources for quantum photonics. In transition-metal dichalcogenides (TMDs), nanopillars are widely used to induce localized emission, yet the underlying confinement mechanism and the relative roles of strain versus dielectric environment remain unclear. The general problem addressed here is whether strain alone explains quantum emitter formation and placement in MoSe$_2$, or whether dielectric contrast at suspended-supported interfaces is also required. Here, we combine hyperspectral superlocalization of photoluminescence with co-registered AFM topography and phase to map the positions of localized states (LS) in MoSe$_2$ suspended on GaN pillars and correlate them with bending strain and the local dielectric context. Contrary to the common assumption of purely strain-driven activation, LS frequently occur at suspended--supported interfaces around the pillar apex and span a broad strain range without a clear threshold, while being scarce along high-strain ripples. Our data indicate that deterministic emitter positioning in Mo-based TMDs benefits from co-engineering both strain gradients and nanoscale dielectric heterogeneity, rather than strain alone. More broadly, this combined optical-mechanical characterization approach provides a general framework for mapping structure-property relationships in 2D quantum materials at the single-emitter level.

cond-mat.mes-hall

Cavity quantum electrodynamics with single perovskite quantum dots

Quantum emitters of single indistinguishable photons play a key role in quantum technologies. Among condensed matter systems, colloidal perovskite quantum dots have emerged as promising candidates, exhibiting high-purity single photon emission at room temperature and two-photon interference visibilities up to 0.5 at cryogenic temperatures. Achieving deterministic coupling of individual perovskite quantum dots to photonic structures is now a critical step towards harnessing cavity quantum electrodynamics (cQED) effects, such as the Purcell effect, to enhance single photon emission rate and indistinguishability. Here, we demonstrate the deterministic and reversible coupling of individual CsPbBr$_{3}$ perovskite quantum dots to a tunable, high-quality factor, low mode volume fiber-based Fabry-Pérot microcavity at 10~\si{\kelvin}. By spatially and spectrally tuning the cavity mode in resonance with the quantum dot emission, we observe up to a twofold increase in single photon emission rates. We build on the original multiplet excitonic fine structure to assess the vacuum Rabi coupling strength ($g \simeq$ 40~\si{\micro eV}) from the shaping of the spectral profile of the emission upon increasing the electromagnetic confinement. This approach also made it possible to delineate the contributions of spectral diffusion and pure dephasing to the total linewidth of emission, paving the way to a fully optimized control of the emission properties of cavity coupled perovskite quantum dots.

quant-ph

The optical absorption in indirect semiconductor to semimetal PtSe2 arises from direct transitions

$\rm{PtSe_2}$ is a van der Waals material transitioning from an indirect bandgap semiconductor to a semimetal with increasing thickness. Its absorption threshold has been conjectured to originate from interband indirect transitions. By quantitative comparison between broadband ($0.8 - 3.0\,\rm{eV}$) optical absorption of high-quality exfoliated crystals and DFT ab-initio simulations, we prove instead that the optical absorption arises only from direct transitions. This understanding allows us to shed light on the semiconductor to semimetal transition and to explore the effect of stacking and excitons on the optical absorption.

cond-mat.mtrl-sci

Impact of bright-dark exciton thermal population mixing on the brightness of CsPbBr$_3$ nanocrystals

Understanding the interplay between bright and dark exciton states is crucial for deciphering the luminescence properties of low-dimensional materials. The origin of the outstanding brightness of lead halide perovskites remains elusive. Here, we analyse temperature-dependent time-resolved photoluminescence to investigate the population mixing between bright and dark exciton sublevels in individual CsPbBr$_3$ nanocrystals in the intermediate confinement regime. We extract bright and dark exciton decay rates, and show quantitatively that the decay dynamics can only be reproduced with second-order phonon transitions. Furthermore, we find that any exciton sublevel ordering is compatible with the most likely population transfer mechanism. The remarkable brightness of lead halide perovskite nanocrystals rather stems from a reduced asymmetry between bright-to-dark and dark-to-bright conversion originating from the peculiar second-order phonon-assisted transitions that freeze bright-dark conversion at low temperature together with the very fast radiative recombination and favourable degeneracy of the bright exciton state.

cond-mat.mes-hall

Luminescence properties of closely packed organic color centers grafted on a carbon nanotube

We report on the photo-luminescence of pairs of organic color centers in single-wall carbon nanotubes grafted with 3,5 dichlorobenzene. Using various techniques such as intensity correlations, super-localization microscopy or luminescence excitation spectroscopy, we distinguish two pairs of color centers grafted on the same nanotube; the distance between the pairs is on the order of several hundreds of nanometers. In contrast, by studying the strong temporal correlations in the spectral diffusion in the framework of photo-induced Stark effect, we can estimate the distance within each pair to be of the order of a few nanometers. Finally, the electronic population dynamics is investigated using time-resolved luminescence and saturation measurements, showing a biexponential decay with a fast overall recombination (compatible with a fast population transfer between the color centers within a pair) and a weak delayed repopulation of the traps possibly due to the diffusion of excitons along the tube axis.

cond-mat.mes-hall

Raman spectroscopy of monolayer to bulk PtSe2 exfoliated crystals

Raman spectroscopy is widely used to assess the quality of 2D materials thin films. This report focuses on $\rm{PtSe_2}$, a noble transition metal dichalcogenide which has the remarkable property to transit from a semi-conductor to a semi-metal with increasing layer number. While polycrystalline $\rm{PtSe_2}$ can be grown with various crystalline qualities, getting insight into the monocrystalline intrinsic properties remains challenging. We report on the study of exfoliated 1 to 10 layers $\rm{PtSe_2}$ by Raman spectroscopy, featuring record linewidth. The clear Raman signatures allow layer-thickness identification and provides a reference metrics to assess crystal quality of grown films.

cond-mat.mtrl-sci

A telecom band single-photon source using a grafted carbon nanotube coupled to a fiber Fabry-Perot cavity in the Purcell regime

We report on the coupling of a reconfigurable high Q fiber micro-cavity to an organic color center grafted to a carbon nanotube for telecom wavelength emission of single photons in the Purcell regime. Using three complementary approaches we assess various figures of merit of this tunable single photon source and of the cavity quantum electrodynamical effects : the brightening of the emitter is obtained by comparison of the count rates of the very same emitter in free-space and cavity coupled regimes. We demonstrate a fiber coupled single-photon output rate up to 20 MHz at 1275~nm. Using time-resolved and saturation measurements, we determine independently the radiative quantum yield and the Purcell factor of the system with values up to 30 for the smallest mode volumes. Finally, we take advantage of the tuning capability of the cavity to measure the spectral profile of the brightness of the source which gives access to the vacuum Rabi splitting $g$ with values up to $25 \; μ$eV.

quant-ph

Spectral fingerprint of quantum confinement in single CsPbBr$_3$ nanocrystals

Lead halide perovskite nanocrystals are promising materials for classical and quantum light emission. To understand these outstanding properties, a thorough analysis of the band-edge exciton emission is needed which is not reachable in ensemble and room temperature studies because of broadening effects. Here, we report on a cryogenic-temperature study of the photoluminescence of single CsPbBr$_3$ NCs in the intermediate quantum confinement regime. We reveal the size-dependence of the spectral features observed: the bright-triplet exciton energy splittings, the trion and biexciton binding energies as well as the optical phonon replica spectrum. In addition, we show that bright triplet energy splittings are consistent with a pure exchange model and that the variety of polarisation properties and spectra recorded can be rationalised simply by considering the orientation of the emitting dipoles and the populations of the emitting states.

cond-mat.mes-hall

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

Effect of phonon bath dimensionality on the spectral efficiency of single-photon emitters in the Purcell regime

We develop a theoretical frame to investigate the single-photon emission spectral efficiency of a solid-state nano-emitter embedded in a high quality factor micro-cavity. This study encompasses the case of localized excitons embedded in a one, two or three-dimensional matrix. The populations evolutions are calculated based on a spin-boson model, using the non-interacting blip approximation (NIBA). We find that the single-photon spectral efficiency of the cavity-coupled emitter can be expressed by a simple formula, taking as inputs the free-space emission and absorption spectra of the emitter as well as the loss rates of the system. In other words, the information on the interaction between the exciton and the phonon bath, encoded in the free-space behavior of the emitter, is sufficient to obtain the dynamics of the system in the cavity. We compute numerically the spectral efficiency for several types of localized emitters and show distinct behaviors depending on the phonon bath dimensionality. In particular, a pronounced asymmetric energy exchange between the emitter and the cavity on the side-bands can yield a considerable extension of the tuning range of the sources through phonon-assisted cavity feeding.

cond-mat.mes-hall

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

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

Measuring the photon coalescence time-window in the continuous-wave regime for resonantly driven semiconductor quantum dots

We revisit Mandel's notion that the degree of coherence equals the degree of indistinguishability by performing Hong-Ou-Mandel- (HOM-)type interferometry with single photons elastically scattered by a cw resonantly driven excitonic transition of an InAs/GaAs epitaxial quantum dot. We present a comprehensive study of the temporal profile of the photon coalescence phenomenon which shows that photon indistinguishability can be tuned by the excitation laser source, in the same way as their coherence time. A new figure of merit, the coalescence time window, is introduced to quantify the delay below which two photons are indistinguishable. This criterion sheds new light on the interpretation of HOM experiments under cw excitation, particularly when photon coherence times are longer than the temporal resolution of the detectors. The photon indistinguishability is extended over unprecedented time scales beyond the detectors' response time, thus opening new perspectives to conducting quantum optics with single photons and conventional detectors.

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

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

Photo-draining and slow capture of carriers in quantum dots probed by resonant excitation spectroscopy

We investigate experimentally and theoretically the resonant emission of single InAs/GaAs quantum dots in a planar microcavity. Due to the presence of at least one residual charge in the quantum dots, the resonant excitation of the neutral exciton is blocked. The influence of the residual doping on the initial quantum dots charge state is analyzed, and the resonant emission quenching is interpreted as a Coulomb blockade effect. The use of an additional non-resonant laser in a specific low power regime leads to the carrier draining in quantum dots and allows an efficient optical gating of the exciton resonant emission. A detailed population evolution model, developed to describe the carrier draining and the optical gate effect, perfectly fits the experimental results in the steady state and dynamical regimes of the optical gate with a single set of parameters. We deduce that ultra-slow Auger- and phonon-assisted capture processes govern the carrier draining in quantum dots with relaxation times in the 1 - 100 microsecond range. We conclude that the optical gate acts as a very sensitive probe of the quantum dots population relaxation in an unprecedented slow-capture regime.

cond-mat.mes-hall