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Carole Diederichs

Publications and source records attributed to Carole Diederichs.

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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

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

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

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

Unveiling the Enhancement of Spontaneous Emission at Exceptional Points

Exceptional points (EPs), singularities of non-Hermitian physics where complex spectral resonances degenerate, are one of the most exotic features of nonequilibrium open systems with unique properties. For instance, the emission rate of quantum emitters placed near resonators with EPs is enhanced (compared to the free-space emission rate) by a factor that scales quadratically with the resonance quality factor. Here, we verify the theory of spontaneous emission at EPs by measuring photoluminescence from photonic-crystal slabs that are embedded with a high-quantum-yield active material. While our experimental results verify the theoretically predicted enhancement, it also highlights the practical limitations on the enhancement due to material loss. Our designed structures can be used in applications that require enhanced and controlled emission, such as quantum sensing and imaging.

physics.optics

Ultralow Threshold Polariton Condensate in a Monolayer Semiconductor Microcavity at Room Temperature

Atomically thin transition metal dichalcogenides possess valley dependent functionalities that are usually available only at crogenic temperatures, constrained by various valley depolarization scatterings. The formation of exciton polaritons by coherently superimposing excitons and microcavity photons potentially harnesses the valley polarized polariton polariton interactions for novel valleytronics devices. Robust EPs have been demonstrated at room temperature in TMDs microcavity, however, the coherent polariton lasing and condensation remain elusive. Herein, we demonstrate for the first time the realization of EP condensation in a TMD microcavity at room temperature. The continuous wave pumped EP condensation and lasing with ultralow thresholdsis evidenced by the macroscopic occupation of the ground state, that undergoes a nonlinear increase of the emission and a continuous blueshift, a build up of spatial coherence, and a detuning-controlled threshold. Our work presents a critically important step towards exploiting nonlinear polariton polariton interactions and polaritonic devices with valley functionality at room temperature.

physics.optics

Observation of Exciton Polariton Condensation in a Perovskite Lattice at Room Temperature

Bose-Einstein condensation in strongly correlated lattices provides the possibility to coherently generate macroscopic quantum states, which have attracted tremendous attention as ideal platforms for quantum simulation. Ultracold atoms in optical lattices are one of such promising systems, where their realizations of different phases of matter exhibit promising applications in condensed matter physics, chemistry, and cosmology. Nevertheless, this is only accessible with ultralow temperatures in the nano to micro Kelvin scale set by the typical inverse mass of an atom. Alternative systems such as lattices of trapped ions and superconducting circuit arrays also rely on ultracold temperatures. Exciton polaritons with extremely light effective mass, are regarded as promising alternatives to realize Bose-Einstein condensation in lattices at higher temperatures. Along with the condensation, an efficient exciton polariton quantum simulator would require a strong lattice with robust trapping at each lattice site as well as strong inter-site coupling to allow coherent quantum motion of polaritons within the lattice. However, exciton polaritons in a strong lattice have only been shown to condense at liquid helium temperatures. Here, we report the observation of exciton polariton condensation in a one-dimensional strong lead halide perovskite lattice at room temperature. Modulated by deep periodic potentials, the strong lead halide perovskite lattice exhibits a large forbidden bandgap opening up to 13.3 meV and a lattice band up to 8.5 meV wide, which are at least 10 times larger than previous systems. Above a critical density, we observe exciton polariton condensation into py orbital states with long-range spatial coherence at room temperature. Our result opens the route to the implementation of polariton condensates in quantum simulators at room temperature.

cond-mat.mes-hall

Optical switching of resonance fluorescence from a single germanium vacancy color center in diamond

Scalable quantum photonic networks require coherent excitation of quantum emitters. However, many solid-state systems can undergo a transition to a dark shelving state that inhibits the fluorescence. Here we demonstrate that a controlled gating using a weak non-resonant laser, the resonant excitation can be recovered and amplified for single germanium vacancies (GeVs). Employing the gated resonance excitation, we achieve optically stable resonance fluorescence of GeV centers. Our results are pivotal for the deployment of diamond color centers as reliable building blocks for scalable solid state quantum networks.

cond-mat.mes-hall

Room Temperature Polariton Lasing in All-Inorganic Perovskites

Polariton lasing is the coherent emission arising from a macroscopic polariton condensate first proposed in 1996. Over the past two decades, polariton lasing has been demonstrated in a few inorganic and organic semiconductors in both low and room temperatures. Polariton lasing in inorganic materials significantly relies on sophisticated epitaxial growth of crystalline gain medium layers sandwiched by two distributed Bragg reflectors in which combating the built-in strain and mismatched thermal properties is nontrivial. On the other hand, organic active media usually suffer from large threshold density and weak nonlinearity due to the Frenkel exciton nature. Further development of polariton lasing towards technologically significant applications demand more accessible materials, ease of device fabrication and broadly tunable emission at room temperature. Herein, we report the experimental realization of room-temperature polariton lasing based on an epitaxy-free all-inorganic cesium lead chloride perovskite microcavity. Polariton lasing is unambiguously evidenced by a superlinear power dependence, macroscopic ground state occupation, blueshift of ground state emission, narrowing of the linewidth and the build-up of long-range spatial coherence. Our work suggests considerable promise of lead halide perovskites towards large-area, low-cost, high performance room temperature polariton devices and coherent light sources extending from the ultraviolet to near infrared range.

cond-mat.mtrl-sci

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

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

Ultra-coherent single photon source

We present a novel type of single photon source in solid state, based on the coherent laser light scattering by a single InAs quantum dot. We demonstrate that the coherence of the emitted single photons is tailored by the resonant excitation with a spectral linewidth below the radiative limit. Our ultra-coherent source opens the way for integrated quantum devices dedicated to the generation of single photons with high degrees of indistinguishability.

cond-mat.mes-hall

Optically-gated resonant emission in single quantum dots

We report on the resonant emission in coherently-driven single semiconductor quantum dots. We demonstrate that an ultra-weak non-resonant laser acts as an optical gate for the quantum dot resonant response. We show that the gate laser suppresses Coulomb blockade at the origin of a resonant emission quenching, and that the optically-gated quantum dots systematically behave as ideal two-level systems in both regimes of coherent and incoherent resonant emission.

cond-mat.mes-hall