arXiv subjects

Emmanuel Lhuillier

Publications and source records attributed to Emmanuel Lhuillier.

At least 19 recordsLinked to original sources

arXiv2025

Plasmonic interferences sampled by a diffraction grating generate moir{é} fringes

We report on the formation of moir{é} patterns when observing the diffraction of surface plasmons by periodic gratings of finite extent with an imaging spectrometer that maps the light emission as a function of the wavelength and the propagation distance. This phenomenon results from the formation of standing waves upon the partial reflection of surface plasmons at the far end of the grating and their scattering by the periodic corrugations. The moir{é} fringes are created as a result of the incommensurability between the sampling pitch of the grating and the wavelengthdependent standing waves. We introduce a scalar model that supports these observations and provides physical insight into these results, including a method to estimate the complex Fresnel reflection coefficient of a surface plasmon at the edge of a grating.

physics.optics↗

arXiv2024

Anisotropic Thermal Transport in Tunable Self-Assembled Nanocrystal Supercrystals

Realizing tunable functional materials with built-in nanoscale heat flow directionality represents a significant challenge that could advance thermal management strategies. Here we use spatiotemporally-resolved thermoreflectance to visualize lateral thermal transport anisotropy in self-assembled supercrystals of anisotropic Au nanocrystals. Correlative electron and thermoreflectance microscopy reveal that nano- to meso-scale heat predominantly flows along the long-axis of the anisotropic nanocrystals, and does so across grain boundaries and curved assemblies while voids disrupt heat flow. We finely control the anisotropy via the aspect ratio of constituent nanorods, and it exceeds the aspect ratio for nano-bipyramid supercrystals and certain nanorod arrangements. Finite element simulations and effective medium modeling rationalize the emergent anisotropic behavior in terms of a simple series resistance model, further providing a framework for estimating thermal anisotropy as a function of material and structural parameters. Self-assembly of colloidal nanocrystals promises an interesting route to direct heat flow in a wide range of applications that utilize this important class of materials.

physics.app-ph↗

arXiv2024

Towards robust detection of entangled two-photon absorption

Over the last 50 years entangled photon pairs have received attention for use in lowering the flux in two-photon absorption imaging and spectroscopy. Despite this, evidence for entangled two-photon absorption (ETPA) effects remain highly debated, especially at low-fluxes. Here, we structure the transverse spatial correlations of entangled photon pairs to evidence signs of ETPA at room-temperature in organic and inorganic chromophores, in the low-flux regime. We demonstrate our scheme to be robust to common artifacts that have previously hampered detection of ETPA such as linear absorption and background fluorescence, and show that ETPA scales with transverse correlation area and chromophore two-photon cross-sections. Our results present a step towards verifying ETPA and experimentally exploring entangled light-matter interactions.

quant-ph↗

arXiv2024

Room-temperature efficient single-photon generation from CdSe/ZnS nanoplateletes

In the search for materials for quantum information science applications, colloidal semiconductor nanoplatelets (NPLs) have emerged as a highly promising new class of materials due to their interesting optical properties, such as narrow emission linewidth and fast photoluminescence (PL) lifetimes at room temperature. So far only few works focused on the quantum properties of their emission, however, NPLs, with their atomic-scale thickness and one-dimensional quantum confinement, are promising candidates for single-photon sources. Here, we demonstrate room-temperature single-photon emission from core/shell CdSe/ZnS NPLs, which feature 8$x$20 nm$^2$ surface area and 1 nm shell. The limited surface area ensures effective Auger non-radiative recombination, resulting in highly efficient single-photon generation with values of photon purity as low as $g^{(2)}(τ)=0.04$. The observed long-period blinking and bleaching, typical of such thin shells, can be easily reduced by increasing the shell thickness. This work establishes NPLs as new single-photon sources very well suited for integration into quantum photonic systems.

quant-ph↗

arXiv2024

Optical and X-ray Photo-emission Spectroscopies of Core/Shell Colloidal CdSe/CdS Quantum Dots: Modeling and Experimental Determination of Band Alignment

Optical properties of multilayer semi-conductor nano-emitters are crucially dependent on the relative energy levelsof their different components. For core/shell quantum dots, the relative energy difference between conduction bandedge of core and shell materials induces, depending on its value, either a confinement of the electron within the coreor a delocalization of its wave function within the whole quantum dot. This results in drastic consequences on theenergy and the oscillator strength of the fundamental transition. Surprisingly, the literature currently lacks a definitivevalue for the energy difference between CdSe and CdS conduction band edges as most of the experimental studiesprovide values corresponding to specific geometries of quantum dots. Here, we develop a full theoretical modelexpressing energy levels considering core/shell interface pressure, ligands and enabling the accurate prediction ofthe bandgap value with the nanocrystal size. It allows to reliably determine the energy difference between theconduction band edge of CdSe and CdS materials, known as the conduction band offset, in such a way that this valuecan later be used to model quantum dots of any geometry. This value is determined using our model and two differentexperimental methods: optical spectroscopy and X-ray photoemission (XPS) experiments.

cond-mat.mtrl-sci↗

arXiv2024

Infrared Imaging using thermally stable HgTe/CdS nanocrystals

Transferring the nanocrystals (NCs) from the laboratory environment toward practical applications has raised new challenges. In the case of NCs for display and lightning, the focus was on reduced Auger recombination and maintaining luminescence at high temperatures. When it comes to infrared sensing, narrow band gap materials are required and HgTe appears as the most spectrally tunable platform. Its low-temperature synthesis reduces the growth energy cost yet also favors sintering. As a result, once coupled to a read-out circuit, the Joule effect aggregates the particles leading to a poorly defined optical edge and dramatically large dark current. Here, we demonstrate that CdS shells bring the expected thermal stability (no redshift upon annealing, reduced tendency to form amalgams and preservation of photoconduction after an atomic layer deposition process). The peculiar electronic structure of these confined particles is unveiled using k.p self-consistent simulations showing a significant exciton biding energy at around 200 meV. After shelling, the material displays a p-type behavior that favors the generation of photoconductive gain. The latter is then used to increase the external quantum

physics.app-ph↗

arXiv2023

Highly photostable Zn-treated halide perovskite nanocrystals for efficient single photon generation

Achieving pure single-photon emission is essential for a range of quantum technologies, from optical quantum computing to quantum key distribution to quantum metrology. Among solid-state quantum emitters, colloidal lead halide perovskite (LHP) nanocrystals (NCs) have garnered significant attention due to their interesting structural and optical properties, which make them appealing single-photon sources (SPSs). However, their practical utilization for quantum technology applications has been hampered by environment-induced instabilities. In this study, we fabricate and characterize in a systematic manner Zn-treated $CsPbBr_3$ colloidal NCs obtained through $Zn^{2+}$ ion doping at the Pb-site, demonstrating improved stability under dilution and illumination. These doped NCs exhibit high single-photon purity, reduced blinking on a sub-millisecond timescale and stability of the bright state for excitation powers well above the saturation levels. Our findings highlight the potential of this synthesis approach to optimize the performance of LHP-based SPSs, opening up interesting prospects for their integration into nanophotonic systems for quantum technology applications.

quant-ph↗

arXiv2022

Unidirectional Rashba Spin Splitting in Single Layer WS$_{2(1-x)}$Se$_{2x}$ alloy

Atomically thin two-dimensional (2D) layered semiconductors such as transition metal dichalcogenides (TMDs) have attracted considerable attention due to their tunable band gap, intriguing spin-valley physics, piezoelectric effects and potential device applications. Here we study the electronic properties of a single layer WS$_{1.4}$Se$_{0.6}$ alloys. The electronic structure of this alloy, explored using angle resolved photoemission spectroscopy, shows a clear valence band structure anisotropy characterized by two paraboloids shifted in one direction of the k-space by a constant in-plane vector. This band splitting is a signature of a unidirectional Rashba spin splitting with a related giant Rashba parameter of 2.8 0.7 eV . The combination of angle resolved photoemission spectroscopy with piezo force microscopy highlights the link between this giant unidirectional Rashba spin splitting and an in-plane polarization present in the alloy. These peculiar anisotropic properties of the WS$_{1.4}$Se$_{0.6}$ alloy can be related to local atomic orders induced during the growth process due the different size and electronegativity between S and Se atoms. This distorted crystal structure combined to the observed macroscopic tensile strain, as evidenced by photoluminescence, displays electric dipoles with a strong in-plane component, as shown by piezoelectric microscopy. The interplay between semiconducting properties, in-plane spontaneous polarization and giant out-of-plane Rashba spin-splitting in this two-dimensional material has potential for a wide range of applications in next-generation electronics, piezotronics and spintronics devices.

cond-mat.mtrl-sci↗

arXiv2022

Anomalous Absorption in Arrays of Metallic Nanoparticles: A Powerful Tool for Quantum Dot Optoelectronics

Periodic arrays of noble metal nanoparticles are emblematic nanostructures in photonics. Their ability to sustain localized surface plasmon resonances has been used throughout the years to demonstrate a variety of passive and active functionalities such as enhanced luminescence in dipolar media and LEDs as well as higher responsivities in photoconductive detectors. Here, we show that additional magnetic resonances, associated with inductive current loops between the nanoparticles and accessible with transverse electric waves, emerge in the limit of dense arrays with subwavelength periods. Moreover, their interplay with the plasmons of the system results in spectrally sharp analogues of electromagnetically induced absorption (EIA). We use these metasurfaces to induce changes and enhancements in the emission, absorption, photoconduction, and polarization properties of active layers of PbS nanocrystals, illustrating the potential of EIA beyond the passive functionalities demonstrated so far in literature.

physics.optics↗

arXiv2022

Evidence for Highly p-type doping and type II band alignment in large scale monolayer WSe2 /Se-terminated GaAs heterojunction grown by Molecular beam epitaxy

Two-dimensional materials (2D) arranged in hybrid van der Waals (vdW) heterostructures provide a route toward the assembly of 2D and conventional III-V semiconductors. Here, we report the structural and electronic properties of single layer WSe2 grown by molecular beam epitaxy on Se-terminated GaAs(111)B. Reflection high-energy electron diffraction images exhibit sharp streaky features indicative of a high-quality WSe2 layer produced via vdW epitaxy. This is confirmed by in-plane x-ray diffraction. The single layer of WSe2 and the absence of interdiffusion at the interface are confirmed by high resolution X-ray photoemission spectroscopy and high-resolution transmission microscopy. Angle-resolved photoemission investigation revealed a well-defined WSe2 band dispersion and a high p-doping coming from the charge transfer between the WSe2 monolayer and the Se-terminated GaAs substrate. By comparing our results with local and hybrid functionals theoretical calculation, we find that the top of the valence band of the experimental heterostructure is close to the calculations for free standing single layer WSe2. Our experiments demonstrate that the proximity of the Se-terminated GaAs substrate can significantly tune the electronic properties of WSe2. The valence band maximum (VBM, located at the K point of the Brillouin zone) presents an upshifts of about 0.56 eV toward the Fermi level with respect to the VBM of WSe2 on graphene layer, which is indicative of high p-type doping and a key feature for applications in nanoelectronics and optoelectronics.

cond-mat.mes-hall↗

arXiv2022

Hybridization and localized flat band in the WSe2/MoSe2 heterobilayer grown by molecular beam epitaxy

Nearly localized moire flat bands in momentum space, arising at particular twist angles, are the key to achieve correlated effects in transition-metal dichalcogenides. Here, we use angle-resolved photoemission spectroscopy (ARPES) to visualize the presence of a flat band near the Fermi level of van der Waals (vdW) WSe2/MoSe2 heterobilayer grown by molecular beam epitaxy. This flat band is localized near the K point of the Brillouin zone and has a width of several hundred meVs. By combining ARPES measurements with density functional theory (DFT) calculations, we confirm the coexistence of different domains, namely the reference 2H stacking without layer misorientation and regions with arbitrary twist angles. For the 2H-stacked heterobilayer, our ARPES results show strong interlayer hybridization effects, further confirmed by complementary micro- Raman spectroscopy measurements. The spin-splitting of the valence band at K is determined to be 470 meV. The valence band maximum (VBM) position of the heterobilayer is located at the Gamma point. The energy difference between the VBM at Gamma and the K point is of -60 meV, which is a stark difference compared to individual 1L WSe2 and 1L WSe2, showing both a VBM at K.

cond-mat.mtrl-sci↗

arXiv2021

Identification of Two Regimes of Carrier Thermalization in PbS Nanocrystal Assemblies

We bring fresh insight into the ensemble properties of PbS colloidal quantum dots with a critical review of the literature on semiconductors followed by systematic comparisons between steady-state photocurrent and photoluminescence measurements. Our experiments, performed with sufficiently low powers to neglect nonlinear effects, indicate that the photoluminescence spectra have no other noticeable contribution beside the radiative recombination of thermalized photocarriers (i.e. photocarriers in thermodynamic quasi-equilibrium). A phenomenological model based on the local Kirchhoff law is proposed that makes it possible to identify the nature of the thermalized photocarriers and to extract their temperatures from the measurements. Two regimes are observed: for highly compact assemblies of PbS quantum dots stripped from organic ligands, the thermalization concerns photocarriers distributed over a wide energy range. With PbS quantum dots cross-linked with 1,2-ethanedithiol or longer organic ligand chains, the thermalization concerns solely the fundamental exciton and can quantitatively explain all the observations, including the precise Stokes shift between the absorbance and luminescence maxima.

cond-mat.mtrl-sci↗

arXiv2021

Spontaneous Emission of Vector Vortex Beams

Harnessing the spontaneous emission of incoherent quantum emitters is one of the hallmarks of nano-optics. Yet, an enduring challenge remains-making them emit vector beams, which are complex forms of light associated with fruitful developments in fluorescence imaging, optical trapping and high-speed telecommunications. Vector beams are characterized by spatially varying polarization states whose construction requires coherence properties that are typically possessed by lasers-but not by photons produced by spontaneous emission. Here, we show a route to weave the spontaneous emission of an ensemble of colloidal quantum dots into vector beams. To this end, we use holographic nanostructures that impart the necessary spatial coherence, polarization and topological properties to the light originating from the emitters. We focus our demonstration on vector vortex beams, which are chiral vector beams carrying non-zero orbital angular momentum, and argue that our approach can be extended to other forms of vectorial light.

physics.optics↗

arXiv2020

Indirect to direct band gap crossover in two-dimensional WS2(1-x)Se2x alloys

In atomically thin transition metal dichalcogenide semiconductors, there is a crossover from indirect to direct bandgap as the thickness drops to one monolayer, which comes with a fast increase of the photoluminescence signal. Here, we show that for different alloy compositions of WS2(1-x)Se2x this trend may be significantly affected by the alloy content and we demonstrate that the sample with the highest Se ratio presents a strongly reduced effect. The highest micro-PL intensity is found for bilayer WS2(1-x)Se2x (x = 0.8) with a decrease of its maximum value by only a factor of 2 when passing from mono- to bi-layer. To better understand this factor and explore the layer-dependent band structure evolution of WS2(1-x)Se2x, we performed a nano-angle resolved photoemission spectroscopy study coupled with first-principles calculations. We find that the high micro-PL value for bilayer WS2(1-x)Se2x (x = 0.8) is due to the overlay of direct and indirect optical transitions. This peculiar high PL intensity in WS2(1-x)Se2x opens the way for spectrally tunable light-emitting devices.

cond-mat.mes-hall↗

arXiv2020

Highly photo-stable Perovskite nanocubes: towards integrated single photon sources based on tapered nanofibers

The interest in perovskite nanocrystals (NCs) such as CsPbBr$_3$ for quantum applications is rapidly raising, as it has been demonstrated that they can behave as very efficient single photon emitters. The main problem to tackle in this context is their photo-stability under optical excitation. In this article, we present a full analysis of the optical and quantum properties of highly efficient perovskite nanocubes synthesized with an established method, which is used for the first time to produce quantum emitters, and is shown to ensure an increased photostability. These emitters exhibit reduced blinking together with a strong photon antibunching. Remarkably these features are hardly affected by the increase of the excitation intensity well above the emission saturation levels. Finally, we achieve for the first time the coupling of a single perovskite nanocube with a tapered optical nanofiber in order to aim for a compact integrated single photon source for future applications.

physics.app-ph↗

arXiv2020

Infrared narrow band gap nanocrystals: recent progresses relative to imaging and active detection

Current technologies for infrared detection have been based on epitaxially grown semiconductors. Here we review some of the recent developments relative to colloidal nanocrystals and their use as building blocks for the design of low-cost infrared sensors. We focus on HgTe nanocrystals which appear as the only material leading to infrared photoconductivity and ultra-broad spectral tunability: from the visible to the long-wave infrared. We review some of the important results which demonstrated that colloidal nanocrystals can be compatible with air stable operations, fast detection, and strong absorption. We discuss the recent progresses relative to multipixel devices and show results obtained by coupling short-wave infrared nanoparticles with CMOS circuits to achieve video rate VGA format imaging. In particular we present that nanocrystals are a promising material for long range (>150 m) active detection in both continuous wave and pulsed mode with a time resolution down to 10 ns.

physics.app-ph↗

arXiv2019

Nanophotonic approaches for integrated quantum photonics

Photons for quantum technologies have been identified early on as a very good candidate for carrying quantum information encoded onto them, either by polarization encoding, time encoding or spatial encoding. Quantum cryptography, quantum communications, quantum networks in general and quantum computing are some of the applications targeted by what is now called quantum photonics. Nevertheless, it was pretty clear at an early stage that bulk optics for handling quantum states of light with photons would not be able to deliver what is needed for these technologies. More recently, single photons, entangled photons and quantum optics in general have been coupled to more integrated approaches coming from classical optics in order to meet the requirements of scalability, reliablility and efficiency for quantum technologies. In this article, we develop our recent advances in two different nanophotonic platforms for quantum photonics using elongated optical fibers and integrated glass waveguides made by the so-called ion-exchange technique. We also present our latest results on quantum nanoemitters that we plan to couple and incorporate with our photonics platforms. These nanoemitters are of two kinds: nanocrystals made of perovskites as well as silicon-vacancy defect centers in nanodiamonds. Some of their properties are developed in this work. We will then give the general steps necessary in order to couple these nanoemitters efficiently with our platforms in the near future.

quant-ph↗

arXiv2019

Spin-Orbit induced phase-shift in Bi$_{2}$Se$_{3}$ Josephson junctions

The transmission of Cooper pairs between two weakly coupled superconductors produces a superfluid current and a phase difference; the celebrated Josephson effect. Because of time-reversal and parity symmetries, there is no Josephson current without a phase difference between two superconductors. Reciprocally, when those two symmetries are broken, an anomalous supercurrent can exist in the absence of phase bias or, equivalently, an anomalous phase shift $φ_0$ can exist in the absence of a superfluid current. We report on the observation of an anomalous phase shift $φ_0$ in hybrid Josephson junctions fabricated with the topological insulator Bi$_2$Se$_3$ submitted to an in-plane magnetic field. This anomalous phase shift $φ_0$ is observed directly through measurements of the current-phase relationship in a Josephson interferometer. This result provides a direct measurement of the spin-orbit coupling strength and open new possibilities for phase-controlled Josephson devices made from materials with strong spin-orbit coupling.

cond-mat.supr-con↗