arXiv subjects

Guillaume Cassabois

Publications and source records attributed to Guillaume Cassabois.

At least 19 recordsLinked to original sources

arXiv2026

In-situ Silicon Doped hBN by High-Temperature Molecular Beam Epitaxy Enables Single Photon Emission

Hexagonal boron nitride (hBN) has emerged as a leading host for optically active quantum defects. Yet introduction of specific impurity species other than carbon remains unexplored. Here, we demonstrate an in-situ silicon doping of hBN grown by high-temperature molecular beam epitaxy (HT-MBE). By systematically varying the growth temperature from 900 to 1390 °C under a constant silicon flux, we establish an optimal window for Si incorporation to host a diverse range of emitters from 430-750 nm at room temperature. By transferring silicon-doped hBN film on SiO$_2$ substrate, we verified that single photon emitter activity was sustained in the hBN, demonstrating compatibility with device integration. The plausible origins of the observed optical transitions were discussed, and several potential candidates were proposed. Our results demonstrate a step toward a comprehensive understanding of in-situ doping of hBN and its utilization for quantum photonic applications.

physics.optics↗

arXiv2026

Optical detection of the electron spin resonances of G centers in silicon

Color centers in silicon are emerging as promising platforms for quantum technologies. Among them, the G center has attracted considerable interest owing to its bright telecom O-band single-photon emission and its optically addressable metastable electron-spin triplet state. Here we investigate the spin properties of ensembles of G centers under above-band-gap excitation. We elucidate the spin photo-dynamics giving rise to the optical detected magnetic resonance (ODMR) response of G centers. The optimal pulsed sequence for measuring the ODMR spectrum of the G defects is identified, along with the temperature and optical-power regimes maximizing the spin readout contrast. Through magneto-optical measurements, we detect a level-anticrossing of the G center electron spin states. At last, we demonstrate coherent spin control of the defects, and characterize their spin-coherence properties. Unveiling the spin degree of freedom of the G center opens new avenues for the realization of quantum memories and quantum registers based on silicon color centers.

quant-ph↗

arXiv2026

A single optically detectable tumbling spin in silicon

We demonstrate single spin spectroscopy of a fluorescent tumbling defect in silicon called the G center, behaving as a pseudo-molecule randomly reorienting itself in the crystalline matrix. Using high-resolution spin spectroscopy, we reveal a fine magnetic structure resulting from the spin principal axes jumping between discrete orientations in the crystal. Modeling the atomic reorientation of the defect shows that spin tumbling induces variations in the coupling to the microwave magnetic field, enabling position-dependent Rabi frequencies to be detected in coherent spin control experiments. By virtue of its pseudo-molecule configuration, the G center in silicon is a unique quantum system to investigate the mutual interaction between optical, spin and rotation properties in a highly versatile material.

quant-ph↗

arXiv2025

Growth of hexagonal BN crystals by traveling-solvent floating zone

Large, high-purity single-crystals of hexagonal BN (h-BN) are essential for exploiting its many desirable and interesting properties. Here, we demonstrate via X-ray tomography, X-ray diffraction and scanning electron microscopy that h-BN crystals can be grown by traveling-solvent floating-zone (TSFZ). The diameters of grown boules range from 3 - 5 mm with lengths from 2 - 10 mm. Tomography indicates variable grain sizes within the boules, with the largest having areas of $\approx$ 1 mm $\times$ 2 mm and thickness $\approx$ 0.5 mm. Although the boules contain macroscale flux inclusions, the h-BN lattice itself is of high quality for samples grown under optimized conditions. The currently optimized growth procedure employs an Fe flux, moderate N$_2$ pressure ($P_{N2} \approx$ 6 bar), and a growth rate of 0.1 mm/h. Raman spectroscopy for an optimized sample gives an average linewidth of 7.7(2) cm$^{-1}$ for the E$_{\mathrm{2g}}$ intralayer mode at 1365.46(4) cm$^{-1}$ and 1.0(1) cm$^{-1}$ for the E$_{\mathrm{2g}}$ interlayer shear mode at 51.78(9) cm$^{-1}$. The corresponding photoluminescence spectrum shows sharp phonon-assisted free exciton peaks and minimal signal in the energy range corresponding to carbon-related defects ($E$ = 3.9 4.1 eV). Our work demonstrates the viability of growing h-BN by the TSFZ technique, thereby opening a new route towards larger, high-quality crystals and advancing the state of h-BN related research.

cond-mat.mtrl-sci↗

arXiv2024

Hopping of the center-of-mass of single G centers in silicon-on-insulator

Among the wealth of single fluorescent defects recently detected in silicon, the G center catches interest for its telecom single-photon emission that could be coupled to a metastable electron spin triplet. The G center is a unique defect where the standard Born-Oppenheimer approximation breaks down as one of its atoms can move between 6 lattice sites under optical excitation. The impact of this atomic reconfiguration on the photoluminescence properties of G centers is still largely unknown, especially in silicon-on-insulator (SOI) samples. Here, we investigate the displacement of the center-of-mass of the G center in silicon. We show that single G defects in SOI exhibit a multipolar emission and zero-phonon line fine structures with splittings up to $\sim1$ meV, both indicating a motion of the defect central atom over time. Combining polarization and spectral analysis at the single-photon level, we evidence that the reconfiguration dynamics are drastically different from the one of the unperturbed G center in bulk silicon. The SOI structure freezes the delocalization of the G defect center-of-mass and as a result, enables to isolate linearly polarized optical lines. Under above-bandgap optical excitation, the central atom of G centers in SOI behaves as if it were in a 6-slot roulette wheel, randomly alternating between localized crystal sites at each optical cycle. Comparative measurements in a bulk silicon sample and ab initio calculations highlight that strain is likely the dominant perturbation impacting the G center geometry. These results shed light on the importance of the atomic reconfiguration dynamics to understand and control the photoluminescence properties of the G center in silicon. More generally, these findings emphasize the impact of strain fluctuations inherent to SOI wafers for future quantum integrated photonics applications based on color centers in silicon.

quant-ph↗

arXiv2024

Layer-by-layer connection for large area single crystal boron nitride multilayer films

Boron nitride (BN) is today considered as one of the most promising materials for many novel applications including bright single photon emission, deep UV opto-electronics, small sized solid-state neutron detector, and high-performance two-dimensional materials, etc. Despite the recent successful fabrication of large-area BN single-crystals (typically <= 5 atomic layers), the scalable growth of thicker single-crystalline BN films still constitutes a great challenge. In this work, we demonstrate an approach to grow large-area multilayer single-crystal BN films by chemical vapor deposition on face-centered cubic Fe-Ni (111) single crystal alloy thin films with different stoichiometric phases. We show that the BN growth is greatly tunable and improved by increasing the Fe content in single-crystal Fe-Ni (111). The formation of pyramid-shaped multilayer BN domains with aligned orientation enables a continuous connection following a layer-by-layer, 'first-meet-first-connect', mosaic stitching mechanism. By means of selected area electron diffraction, micro-photoluminescence spectroscopy in the deep UV and high-resolution transmission electron microscopy, the layer-by-layer connection mechanism is unambiguously evidenced, and the stacking order has been verified to occur as unidirectional AB and ABC stackings, i.e., in the Bernal and rhombohedral BN phase.

cond-mat.mtrl-sci↗

arXiv2024

Genuine and faux single G centers in carbon-implanted silicon

Among the wide variety of single fluorescent defects investigated in silicon, numerous studies have focused on color centers with a zero-phonon line around $1.28 μ$m and identified to a common carbon-complex in silicon, namely the G center. However, inconsistent estimates regarding their quantum efficiency cast doubt on the correct identification of these individual emitters. Through a comparative analysis of their single-photon emission properties, we demonstrate that these single color centers are split in two distinct families of point defects. A first family consists of the genuine single G centers with a well-identified microscopic structure and whose photoluminescence has been investigated on ensemble measurements since the 60's. The remaining defects belong to a new color center, which we will refer to as G$^{\star}$ center, whose atomic configuration has yet to be determined. These results provide a safeguard against future defect misidentifications, which is crucial for further development of quantum technologies relying on G or G$^{\star}$ center quantum properties.

quant-ph↗

arXiv2023

Purcell enhancement of silicon W centers in circular Bragg grating cavities

Generating single photons on demand in silicon is a challenge to the scalability of silicon-on-insulator integrated quantum photonic chips. While several defects acting as artificial atoms have recently demonstrated an ability to generate antibunched single photons, practical applications require tailoring of their emission through quantum cavity effects. In this work, we perform cavity quantum electrodynamics experiments with ensembles of artificial atoms embedded in silicon-on-insulator microresonators. The emitters under study, known as W color centers, are silicon tri-interstitial defects created upon self-ion implantation and thermal annealing. The resonators consist of circular Bragg grating cavities, designed for moderate Purcell enhancement ($F_p=12.5$) and efficient luminescence extraction ($η_{coll}=40\%$ for a numerical aperture of 0.26) for W centers located at the mode antinode. When the resonant frequency mode of the cavity is tuned with the zero-phonon transition of the emitters at 1218 nm, we observe a 20-fold enhancement of the zero-phonon line intensity, together with a two-fold decrease of the total relaxation time in time-resolved photoluminescence experiments. Based on finite-difference time-domain simulations, we propose a detailed theoretical analysis of Purcell enhancement for an ensemble of W centers, considering the overlap between the emitters and the resonant cavity mode. We obtain a good agreement with our experimental results assuming a quantum efficiency of $65 \pm 10 \%$ for the emitters in bulk silicon. Therefore, W centers open promising perspectives for the development of on-demand sources of single photons, harnessing cavity quantum electrodynamics in silicon photonic chips.

physics.optics↗

arXiv2022

Detection of single W-centers in silicon

Controlling the quantum properties of individual fluorescent defects in silicon is a key challenge towards advanced quantum photonic devices prone to scalability. Research efforts have so far focused on extrinsic defects based on impurities incorporated inside the silicon lattice. Here we demonstrate the detection of single intrinsic defects in silicon, which are linked to a tri-interstitial complex called W-center, with a zero-phonon line at 1.218$μ$m. Investigating their single-photon emission properties reveals new information about this common radiation damage center, such as its dipolar orientation and its photophysics. We also identify its microscopic structure and show that although this defect does not feature electronic states in the bandgap, Coulomb interactions lead to excitonic radiative recombination below the silicon bandgap. These results could set the stage for numerous quantum perspectives based on intrinsic luminescent defects in silicon, such as quantum integrated photonics, quantum communications and quantum sensing.

quant-ph↗

arXiv2022

Single G centers in silicon fabricated by co-implantation with carbon and proton

We report the fabrication of G centers in silicon with an areal density compatible with single photon emission at optical telecommunication wavelengths. Our sample is made from a silicon-on-insulator wafer which is locally implanted with carbon ions and protons at various fluences. Decreasing the implantation fluences enables to gradually switch from large ensembles to isolated single defects, reaching areal densities of G centers down to $\sim$0.2 $μ$m$^{-2}$. Single defect creation is demonstrated by photon antibunching in intensity-correlation experiments, thus establishing our approach as a reproducible procedure for generating single artificial atoms in silicon for quantum technologies.

physics.app-ph↗

arXiv2021

Band gap measurements of monolayer h-BN and insights into carbon-related point defects

Being a flexible wide band gap semiconductor, hexagonal boron nitride (h-BN) has great potential for technological applications like efficient deep ultraviolet light sources, building block for two-dimensional heterostructures and room temperature single photon emitters in the ultraviolet and visible spectral range. To enable such applications, it is mandatory to reach a better understanding of the electronic and optical properties of h-BN and the impact of various structural defects. Despite the large efforts in the last years, aspects such as the electronic band gap value, the exciton binding energy and the effect of point defects remained elusive, particularly when considering a single monolayer. Here, we directly measured the density of states of a single monolayer of h-BN epitaxially grown on highly oriented pyrolytic graphite, by performing low temperature scanning tunneling microscopy (STM) and spectroscopy (STS). The observed h-BN electronic band gap on defect-free regions is $(6.8\pm0.2)$ eV. Using optical spectroscopy to obtain the h-BN optical band gap, the exciton binding energy is determined as being of $(0.7\pm0.2)$ eV. In addition, the locally excited cathodoluminescence and photoluminescence show complex spectra that are typically associated to intragap states related to carbon defects. Moreover, in some regions of the monolayer h-BN we identify, using STM, point defects which have intragap electronic levels around 2.0 eV below the Fermi level.

cond-mat.mes-hall↗

arXiv2019

InAs quantum dot in a needlelike tapered InP nanowire: a telecom band single photon source monolithically grown on silicon

Realizing single photon sources emitting in the telecom band on silicon substrates is essential to reach complementary-metal-oxide-semiconductor (CMOS) compatible devices that secure communications over long distances. In this work, we propose the monolithic growth of needlelike tapered InAs/InP quantum dot-nanowires (QD-NWs) on silicon substrates with a small taper angle and a nanowire diameter tailored to support a single mode waveguide. Such a NW geometry is obtained by a controlled balance over axial and radial growths during the gold-catalyzed growth of the NWs by molecular beam epitaxy. This allows us to investigate the impact of the taper angle on the emission properties of a single InAs/InP QD-NW. At room temperature, a Gaussian far-field emission profile in the telecom O-band with a 30° beam divergence angle is demonstrated from a single InAs QD embedded in a 2° tapered InP NW. Moreover, single photon emission is observed at cryogenic temperature for an off-resonant excitation and the best result, $g^2(0) = 0.05$, is obtained for a 7° tapered NW. This all-encompassing study paves the way for the monolithic growth on silicon of an efficient single photon source in the telecom band based on InAs/InP QD-NWs.

physics.app-ph↗

arXiv2019

Spontaneous emission of color centers at 4eV in hexagonal boron nitride under hydrostatic pressure

The light emission properties of color centers emitting in 3.3-4 eV region are investigated for hydrostatic pressures ranging up to 5GPa at liquid helium temperature. The light emission energy decreases with pressure less sensitively than the bandgap. This behavior at variance from the shift of the bandgap is typical of deep traps. Interestingly, hydrostatic pressure reveals the existence of levels that vary differently under pressure (smaller increase of the emission wavelength compared to the rest of the levels in this energy region or even decrease of it) with pressure. This discovery enriches the physics of the color centers operating in the UV in hBN.

cond-mat.mtrl-sci↗

arXiv2018

Van der Waals epitaxy of two-dimensional single-layer h-BN on graphite by molecular beam epitaxy: Electronic properties and band structure

We report on the controlled growth of h-BN/graphite by means of molecular beam epitaxy (MBE). X-ray photoelectron spectroscopy (XPS) suggests an interface without any reaction or intermixing, while the angle resolved photoemission spectroscopy (ARPES) measurements show that the h-BN layers are epitaxially aligned with graphite. A well-defined band structure is revealed by ARPES measurement, reflecting the high quality of the h-BN films. The measured valence band maximum (VBM) located at 2.8 eV below the Fermi level reveals the presence of undoped h-BN films (band gap ~ 6 eV). These results demonstrate that, although only weak van der Waals interactions are present between h-BN and graphite, a long range ordering of h-BN can be obtained even on polycrystalline graphite via van der Waals epitaxy, offering the prospect of large area, single layer h-BN.

cond-mat.mtrl-sci↗

arXiv2014

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↗

arXiv2013

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↗

arXiv2011

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↗

arXiv2011

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↗