arXiv subjects

Sébastien Roux

Publications and source records attributed to Sébastien Roux.

17 recordsLinked to original sources

arXiv2026

Non-radiative energy transfer between boron vacancies in hexagonal boron nitride and other 2D materials

Boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) have emerged as a promising platform for two-dimensional quantum sensors capable of operating at atomic-scale proximity. However, the mechanisms responsible for photoluminescence quenching in thin hBN sensing layers when placed in contact with absorptive materials remain largely unexplored. In this Letter, we investigate non-radiative Förster resonance energy transfer (FRET) between $V_B^-$ centers and either monolayer graphene or 2D semiconductors. Strikingly, we find that the FRET rate is negligible for hBN sensing layers thicker than 3 nm, highlighting the potential of $V_B^-$ centers for integration into ultra-thin quantum sensors within van der Waals heterostructures. Furthermore, we experimentally extract the intrinsic radiative decay rate of $V_B^-$ defects.

cond-mat.mtrl-sci↗

arXiv2026

Gate-tuneable single-photon emitters in WSe2 monolayer created via AFM nanoindentation on rigid SiO2/Si substrates

Single-photon emitters (SPEs) hosted by two-dimensional (2D) semiconducting materials are envisioned for next-generation quantum applications. However, SPE creation in 2D semiconductors on rigid substrates like SiO2/Si via nanoindentation is a technological gap, critical for interfacing SPEs with photonic circuits and cavities. Here, we report a protocol for deterministically creating SPEs in monolayer WSe2 on SiO2/Si substrates using a sharp diamond AFM (atomic force microscope) tip. A displacement-controlled indentation process is developed, allowing indent depths > 150 nm necessary for creating SPEs. Sharp defect peaks (~200 μeV) are observed in cryogenic (4K) photoluminescence (PL) spectrum at nanoindented sites and are stable upto ~ 120K. 76% of sites exhibit sharp defect-bound peaks confirmed by power-dependent, temperature-dependent, and time-resolved PL (TRPL). AFM and PL mapping link these peaks to indent periphery. The peaks show sub-linewidth spectral jitter, no blinking, and single-photon nature in second-order autocorrelation measurements. SPEs can be switched on/off, and background emissions suppressed using electrical gating. Gate-voltage dependent TRPL indicate that SPE dynamics can be tuned, depending on nature of SPE, pointing the way to higher-purity SPEs. Our work is directly applicable to other 2D materials and photonic circuit/cavity compatible rigid substrates and is a significant step for scalable SPE technologies.

cond-mat.mes-hall↗

arXiv2025

High luminescence efficiency of multi-valley excitonic complexes in heavily doped WSe2 monolayer

Monolayers of group-VI transition-metal dichalcogenides (TMDs) are two-dimensional semiconductors that exhibit exceptionally strong light-matter coupling yet typically suffer from low emission quantum yields. In this letter, we investigate the heavily n-doped regime of a WSe$_2$ monolayer and show that multi-particle excitonic complexes produce photoluminescence signals up to two orders of magnitude stronger than in the neutral state. Time-resolved photoluminescence and differential reflectivity measurements reveal that the quantum yield rises with carrier density and exceeds 50% for electron concentrations above 10$^{13}$ cm$^{-2}$. These findings establish TMD monolayers as a platform for exploring excitonic complexes in high-density electron gases and point toward new opportunities for efficient, atomically thin light emitters.

cond-mat.mes-hall↗

arXiv2025

Exciton self-trapping in twisted hexagonal boron nitride homostructures

One of the main interests of 2D materials is their ability to be assembled with many degrees of freedom for tuning and manipulating excitonic properties. There is a need to understand how the structure of the interfaces between atomic layers influences exciton properties. Here we use cathodoluminescence and time-resolved cathodoluminescence experiments to study how excitons interact with the interface between two twisted hexagonal boron nitride (hBN) crystals with various angles. An efficient capture of free excitons by the interface is demonstrated, which leads to a population of long-lived and interface-localized (2D) excitons. Temperature dependent experiments indicate that for high twist angles, these excitons localized at the interface further undergo a selftrapping. It consists in a distortion of the lattice around the exciton on which the exciton traps itself. Our results suggest that this exciton-interface interaction causes the broad 4-eV optical emission of highly twisted hBN-hBN structures. Exciton self-trapping is finally discussed as a common feature of sp2 hybridized boron nitride polytypes and nanostructures due to the ionic nature of the B-N bond and the small size of their excitons.

cond-mat.mtrl-sci↗

arXiv2025

Charge state tuning of spin defects in hexagonal boron nitride

Boron vacancies in hexagonal boron nitride (hBN) are among the most extensively studied optically active spin defects in van der Waals crystals, due to their promising potential to develop two-dimensional (2D) quantum sensors. In this letter, we demonstrate the tunability of the charge state of boron vacancies in ultrathin hBN layers, revealing a transition from the optically active singly negatively charged state to the optically inactive doubly negatively charged state when sandwiched between graphene electrodes. Notably, there is a photoluminescence quenching of a few percent upon the application of a bias voltage between the electrodes. Our findings emphasize the critical importance of considering the charge state of optically active defects in 2D materials, while also showing that the negatively charged boron vacancy remains robust against external perpendicular electric fields. This stability makes it a promising candidate for integration into various van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2024

Optical detection of the sliding ferroelectric switching in hBN with a WSe2 monolayer

When two BN layers are stacked in parallel in an AB or BA arrangement, a spontaneous out-of-plane electric polarization arises due to charge transfer in the out-of-plane B-N bonds. The ferroelectric switching from AB to BA (or BA to AB) can be achieved with a relatively small out-of-plane electric field through the in-plane sliding of one atomic layer over the other. However, the optical detection of such ferroelectric switching in hBN has not yet been demonstrated. In this study, we utilize an adjacent WSe2 monolayer to detect the ferroelectric switching in BN. This dynamic coupling between a 2D ferroelectric and a 2D semiconductor allows for the fundamental investigation of the ferroelectric material using a non-destructive, local optical probe, offering promising applications for compact and non-volatile memory devices.

cond-mat.mtrl-sci↗

arXiv2023

Electron and hole doping of monolayer WSe2 induced by twisted ferroelectric hexagonal boron nitride

For the past few years, 2D ferroelectric materials have attracted strong interest for their potential in future nanoelectronics devices. The recent discovery of 2D ferroelectricity in twisted layers of insulating hexagonal boron nitride, one of the most used 2D materials, has opened the route to its integration into complex van der Waals heterostructures combining hybrid properties. Here we show that opposite polarizations in ferroelectric domains of a folded hBN layer can imprint local n and p doping in a semiconducting transition metal dichalcogenide WSe2 monolayer. We demonstrate that WSe2 can be used as an optical probe of ferroelectricity in hBN and show that the doping density and type can be controlled with the position of the semiconductor with respect to the ferroelectric interface. Our results establish the ferroelectric hBN/WSe2 van der Waals stacking as a promising optoelectronic structure.

cond-mat.mtrl-sci↗

arXiv2023

Surface recombination and out of plane diffusivity of free excitons in hexagonal boron nitride

We present a novel experimental protocol using Cathodoluminescence measurements as a function of the electron incident energy to study both exciton diffusion in a directional way and surface exciton recombination. Our approach overcomes the challenges of anisotropic diffusion and the limited applicability of existing methods to the bulk counterparts of 2D materials. The protocol is then applied at room and at cryogenic temperatures to four bulk hexagonal boron nitride crystals grown by different synthesis routes. The exciton diffusivity depends on the sample quality but not on the temperature, indicating it is limited by defect scattering even in the best quality crystals. The lower limit for the diffusivity by phonon scattering is 0.2 cm$^{2}$.s$^{-1}$. Diffusion lengths were as much as 570 nm. Finally, the surface recombination velocity exceeds 10$^{5}$ cm$^{2}$.s$^{-1}$, at a level similar to silicon or diamond. This result reveals that surface recombination could strongly limit light-emitting devices based on 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Two-photon interference from a quantum emitter in hexagonal boron nitride

Recently discovered quantum emitters in two-dimensional (2D) materials have opened new perspectives of integrated photonic devices for quantum information. Most of these applications require the emitted photons to be indistinguishable, which has remained elusive in 2D materials. Here, we investigate two-photon interference of a quantum emitter generated in hexagonal boron nitride (hBN) using an electron beam. We measure the correlations of zero-phonon-line photons in a Hong-Ou-Mandel (HOM) interferometer under non-resonant excitation. We find that the emitted photons exhibit a partial indistinguishability of $0.44 \pm 0.11$ in a 3 ns time window, which corresponds to a corrected value of $0.56 \pm 0.11$ after accounting for imperfect emitter purity. The dependence of the HOM visibility on the width of the post-selection time window allows us to estimate the dephasing time of the emitter to be $\sim 1.5$ ns, about half the limit set by spontaneous emission. A visibility above 90 % is under reach using Purcell effect with up-to-date 2D material photonics.

quant-ph↗

arXiv2022

Quantum well confinement and competitive radiative pathways in the luminescence of black phosphorus layers

Black phosphorus (BP) stands out from other 2D materials by the wide amplitude of the band-gap energy (Delta(Eg)) that sweeps an optical window from Visible (VIS) to Infrared (IR) wavelengths, depending on the layer thickness. This singularity made the optical and excitonic properties of BP difficult to map. Specifically, the literature lacks in presenting experimental and theoretical data on the optical properties of BP on an extended thickness range. Here we report the study of an ensemble of photoluminescence spectra from 79 passivated BP flakes recorded at 4 K with thicknesses ranging from 4 nm to 700 nm, obtained by mechanical exfoliation. We observe that the exfoliation steps induce additional defects states that compete the radiative recombination from bound excitons observed in the crystal. We also show that the evolution of the photoluminescence energy versus thickness follows a quantum well confinement model appreciable from a thickness predicted and probed at 25 nm. The BP slabs placed in different 2D heterostructures show that the emission energy is not significantly modulated by the dielectric environment. Introduction Confinement effects

cond-mat.mes-hall↗

arXiv2022

Inverting Regional Sensitivity Analysis to reveal sensitive model behaviors

We address the question of sensitivity analysis for model outputs of any dimension using Regional Sensitivity Analysis (RSA). Classical RSA computes sensitivity indices related to the impact of model inputs variations on the occurrence of a target region of the model output space. In this work, we invert this perspective by proposing to find, for a given target model input, the region whose occurrence is best explained by the variations of this input. When it exists, this region can be seen as a model behavior which is particularly sensitive to the variations of the model input under study. We name this method iRSA (for inverse RSA). iRSA is formalized as an optimization problem using region-based sensitivity indices and solved using dedicated numerical algorithms. Using analytical and numerical examples, including an environmental model producing time series, we show that iRSA can provide a new graphical and interpretable characterization of sensitivity for model outputs of various dimensions.

math.ST↗

arXiv2022

Cathodoluminescence monitoring of quantum emitter activation in hexagonal boron nitride

The ability to locally activate or generate quantum emitters in two-dimensional materials is of major interest for the realization of integrated quantum photonic devices. In particular, hexagonal boron nitride (hBN) has recently been shown to allow a variety of techniques for obtaining quantum emitters at desired locations. Here, we use cathodoluminescence (CL) to monitor in situ the local activation of color centers by an electron beam in hBN. We observe that the CL signal saturates at a given surface dose, independently of the electron current density. Based on photoluminescence and photon correlations, we show that the number of photoactive color centers is proportional to the CL signal, and we estimate the maximum density of quantum emitters that can be generated by our technique. Our results provide insights about the activation mechanism and could help to optimize the controlled generation of single photon sources in hexagonal boron nitride.

physics.app-ph↗

arXiv2022

From the synthesis of hBN crystals to their use as nanosheets for optoelectronic devices

In the wide world of 2D materials, hexagonal boron nitride (hBN) holds a special place due to its excellent characteristics. In addition to its thermal, chemical and mechanical stability, hBN demonstrates high thermal conductivity, low compressibility, and wide band gap around 6 eV, making it promising candidate for many groundbreaking applications and more specifically for optoelectronic devices. Millimeters scale hexagonal boron nitride crystals are obtained through a disruptive dual method (PDC/PCS) consisting in a complementary coupling of the Polymer Derived Ceramics route and a Pressure-Controlled Sintering process. In addition to their excellent chemical and crystalline quality, these crystals exhibit a free exciton lifetime of 0.43 ns, as determined by time-resolved cathodoluminescence measurements, confirming their interesting optical properties. To go further in applicative fields, hBN crystals are then exfoliated, and resulting Boron Nitride NanoSheets (BNNSs) are used to encapsulate transition metal dichalcogenides (TMDs). Such van der Waals heterostructures are tested by optical spectroscopy. BNNSs do not luminesce in the emission spectral range of TMDs and the photoluminescence width of the exciton at 4K is in the range 2-3 meV. All these results demonstrate that these BNNSs are relevant for future opto-electronic applications.

cond-mat.mtrl-sci↗

arXiv2021

Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride

Single photon emitters (SPEs) in low-dimensional layered materials have recently gained a large interest owing to the auspicious perspectives of integration and extreme miniaturization offered by this class of materials. However, accurate control of both the spatial location and the emission wavelength of the quantum emitters is essentially lacking to date, thus hindering further technological steps towards scalable quantum photonic devices. Here, we evidence SPEs in high purity synthetic hexagonal boron nitride (hBN) that can be activated by an electron beam at chosen locations. SPE ensembles are generated with a spatial accuracy better than the cubed emission wavelength, thus opening the way to integration in optical microstructures. Stable and bright single photon emission is subsequently observed in the visible range up to room temperature upon non-resonant laser excitation. Moreover, the low-temperature emission wavelength is reproducible, with an ensemble distribution of width 3 meV, a statistical dispersion that is more than one order of magnitude lower than the narrowest wavelength spreads obtained in epitaxial hBN samples. Our findings constitute an essential step towards the realization of top-down integrated devices based on identical quantum emitters in 2D materials.

physics.optics↗

arXiv2021

Radiative lifetime of free excitons in hexagonal boron nitride

Using a new time-resolved cathodoluminescence system dedicated to the UV spectral range, we present a first estimate of the radiative lifetime of free excitons in hBN at room temperature. This is carried out from a single experiment giving both the absolute luminescence intensity under continuous excitation and the decay time of free excitons in the time domain. The radiative lifetime of indirect excitons in hBN is equal to 27 ns, which is much shorter than in other indirect bandgap semiconductors. This is explained by the close proximity of the electron and the hole in the exciton complex, and also by the small energy difference between indirect and direct excitons. The unusually high luminescence efficiency of hBN for an indirect bandgap is therefore semi-quantitatively understood.

cond-mat.mtrl-sci↗

arXiv2020

Optical brain imaging using a semi-transparent organic light-emitting diode

We report optical brain imaging using a semi-transparent organic light-emitting diode (OLED) based on the orange light-emitting polymer (LEP) Livilux PDO-124. The OLED serves as a compact, extended light source which is capable of uniformly illuminating the cortical surface when placed across a burr hole in the skull. Since all layers of the OLED are substantially transparent to photons with energies below the optical gap of the LEP, light emitted or reflected by the cortical surface may be efficiently transmitted through the OLED and into the objective lens of a low magnification microscope ('macroscope'). The OLED may be placed close to the cortical surface, providing efficient coupling of incident light into the brain cavity; furthermore, the macroscope may be placed close to the upper surface of the OLED, enabling efficient collection of reflected/emitted light from the cortical surface. Hence the use of a semi-transparent OLED simplifies the optical setup, while at the same time maintaining high sensitivity. The OLED is applied here to one of the most demanding forms of optical brain imaging, namely extrinsic optical imaging involving a voltage sensitive dye (VSD). Specifically, we carry out functional imaging of the primary visual cortex (V1) of a rat, using the voltage sensitive dye RH-1691 as a reporter. Imaging through the OLED light-source, we are able to resolve small (~ 0.1 %) changes in the fluorescence intensity of the dye due to changes in the neuronal membrane potential following a visual stimulus. Results are obtained on a single trial basis -- i.e. without averaging over multiple measurements -- with a time-resolution of ten milliseconds.

physics.optics↗

arXiv2010

The Local Field Potential Reflects Surplus Spike Synchrony

The oscillatory nature of the cortical local field potential (LFP) is commonly interpreted as a reflection of synchronized network activity, but its relationship to observed transient coincident firing of neurons on the millisecond time-scale remains unclear. Here we present experimental evidence to reconcile the notions of synchrony at the level of neuronal spiking and at the mesoscopic scale. We demonstrate that only in time intervals of excess spike synchrony, coincident spikes are better entrained to the LFP than predicted by the locking of the individual spikes. This effect is enhanced in periods of large LFP amplitudes. A quantitative model explains the LFP dynamics by the orchestrated spiking activity in neuronal groups that contribute the observed surplus synchrony. From the correlation analysis, we infer that neurons participate in different constellations but contribute only a fraction of their spikes to temporally precise spike configurations, suggesting a dual coding scheme of rate and synchrony. This finding provides direct evidence for the hypothesized relation that precise spike synchrony constitutes a major temporally and spatially organized component of the LFP. Revealing that transient spike synchronization correlates not only with behavior, but with a mesoscopic brain signal corroborates its relevance in cortical processing.

q-bio.NC↗