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Nicolas Grandjean

Publications and source records attributed to Nicolas Grandjean.

At least 19 recordsLinked to original sources

Depth Control of Room-Temperature Quantum Emitters in Gallium Nitride

Bright quantum emitters are key components for quantum communication systems. Radiative point defects in gallium nitride (GaN) are promising candidates for room-temperature single-photon emission, operating from the visible to the telecom O-band. Despite their potential, their integration into photonic structures has remained limited in the literature, with experimental photon extraction efficiencies far below simulated predictions. To identify the origin of this limitation, we investigate visible and near-infrared quantum emitters in GaN epilayers grown on $c$-plane sapphire substrates exhibiting narrow linewidths ($\sim$4 nm), high photon count rates ($ > $2 MHz), and strong antibunching, reaching $g^{(2)}(0)$ values as low as 0.06 at room temperature. We find that these emitters are located near the GaN/substrate interface, explaining their limited coupling to optical modes. Building on this observation, we show that the insertion of a thin low-temperature GaN interlayer enables the formation of quantum emitters at arbitrary depths with sub-60 nm accuracy, independent of the substrate. The intentionally introduced emitters retain optical properties comparable to naturally occurring ones, including narrow linewidths ($\sim$6 nm), saturation count rates exceeding 1.5 MHz, high Debye-Waller factors (0.69-0.98), and strong antibunching. The resulting epilayer fully coalesces within less than 250 nm ensuring compatibility with GaN-based cavity fabrication and enabling emitter placement within intrinsic regions of p-i-n diode architectures. These results mark a decisive step toward efficient emitter-cavity coupling, enabling the realization of cavity-enhanced quantum emission in GaN.

cond-mat.mes-hall

When heat goes astray -- non-local heating in a semiconductor

Heating of semiconductor devices limits their performance and lifetime, which must be addressed by thermal management starting at the heat source. It is a common assumption that the heat source and the resulting heat spot locally coincide, if their size exceeds the mean free paths of the main heat carriers, the phonons. We show that this paradigm of heat locality breaks down on length scales spanning several micrometers. As a consequence, non-local heating occurs in contradiction to Fourier's law. Therefore, we heat laterally structured semiconductor membranes that feature a rising number of interfaces with a well-focussed laser and map-out lattice temperatures by Raman thermometry. Remarkably, the non-local heating can exceed the laser-induced local heating, which we attribute to ballistic phonon transport far above cryogenic temperatures.

cond-mat.mes-hall

Three-Octave Supercontinuum Generation in Thick Crystalline Aluminum Nitride Waveguides

We report an efficient extension of supercontinuum generation through dispersion engineering of crystalline aluminum nitride (AlN)-on-sapphire waveguides. Using a tailored epitaxial regrowth of AlN epilayers and an optimized fabrication protocol, the dispersion sensitivity to the waveguide cross-section was enhanced allowing for a significant reach extension of both short and long dispersive wave with optimized pumping conditions, reaching down to 550 nm in the visible and up to 4.5 {\mu}m in the mid-infrared.

physics.optics

Sputtered AlN buffer layer for low-loss crystalline AlN-on-sapphire integrated photonics

In recent years, aluminum nitride (AlN) has emerged as an attractive material for integrated photonics due to its low propagation losses, wide transparency window, and presence of both second- and third-order optical nonlinearities. However, most of the research led on this platform has primarily focused on applications, rather than material optimization, although the latter is equally important to ensure its technological maturity. In this work, we show that voids, which are commonly found in crystalline AlN-on-sapphire epilayers, have a detrimental role in related photonic structures, as they can lead to propagation losses exceeding 30 dB cm$^{-1}$ at 1550 nm. Their impact on light propagation is further quantified through finite-difference time-domain simulations that reveal that void-related scattering losses are strongly dependent on their size and density in the layer. As a possible solution, we demonstrate that when introducing a thin sputtered AlN buffer layer prior to initiating AlN epitaxial growth, void-free layers are obtained. They exhibit intrinsic quality factors in microring resonators as high as $2.0\times 10^6$, corresponding to propagation losses lower than 0.2 dB cm$^{-1}$ at 1550 nm. These void-free layers are further benchmarked for high-power applications through second-harmonic and supercontinuum generation in dispersion-engineered waveguides. Such layers are highly promising candidates for short-wavelength photonic integrated circuit applications, particularly given the strong potential of AlN for visible photonics. Given that volumetric scattering losses scale as $\lambda^{-4}$, the platform quality becomes increasingly critical in the visible and ultraviolet range, where our improved layers are expected to deliver enhanced performance.

physics.optics

Thermal analysis of GaN-based photonic membranes for optoelectronics

Semiconductor membranes find their widespread use in various research fields targeting medical, biological, environmental, and optical applications. Often such membranes derive their functionality from an inherent nanopatterning, which renders the determination of their, e.g., optical, electronic, mechanical, and thermal properties a challenging task. In this work we demonstrate the non-invasive, all-optical thermal characterization of around 800-nm-thick and 150-$\mu$m-wide membranes that consist of wurtzite GaN and a stack of In$_{0.15}$Ga$_{0.85}$N quantum wells as a built-in light source. Due to their application in photonics such membranes are bright light emitters, which challenges their non-invasive thermal characterization by only optical means. As a solution, we combine two-laser Raman thermometry with (time-resolved) photoluminescence measurements to extract the in-plane (i.e., $c$-plane) thermal conductivity $\kappa_{\text{in-plane}}$ of our membranes. Based on this approach, we can disentangle the entire laser-induced power balance during our thermal analysis, meaning that all fractions of reflected, scattered, transmitted, and reemitted light are considered. As a result of our thermal imaging via Raman spectroscopy, we obtain $\kappa_{\text{in-plane}}\,=\,165^{+16}_{-14}\,$Wm$^{-1}$K$^{-1}$ for our best membrane, which compares well to our simulations yielding $\kappa_{\text{in-plane}}\,=\,177\,$Wm$^{-1}$K$^{-1}$ based on an ab initio solution of the linearized phonon Boltzmann transport equation. Our work presents a promising pathway towards thermal imaging at cryogenic temperatures, e.g., when aiming to elucidate experimentally different phonon transport regimes via the recording of non-Fourier temperature distributions.

physics.optics

Optical and thermal characterization of a group-III nitride semiconductor membrane by microphotoluminescence spectroscopy and Raman thermometry

We present the simultaneous optical and thermal analysis of a freestanding photonic semiconductor membrane made from wurtzite III-nitride material. By linking micro-photoluminescence ($μ$PL) spectroscopy with Raman thermometry, we demonstrate how a robust value for the thermal conductivity $κ$ can be obtained using only optical, non-invasive means. For this, we consider the balance of different contributions to thermal transport given by, e.g., excitons, charge carriers, and heat carrying phonons. Further complication is given by the fact that this membrane is made from direct bandgap semiconductors, designed to emit light based on an In$_{x}$Ga$_{1-x}$N ($x=0.15$) quantum well embedded in GaN. To meet these challenges, we designed a novel experimental setup that enables the necessary optical and thermal characterizations in parallel. We perform micro-Raman thermometry, either based on a heating laser that acts as a probe laser (1-laser Raman thermometry), or based on two lasers, providing the heating and the temperature probe separately (2-laser Raman thermometry). For the latter technique, we obtain temperature maps over tens of micrometers with a spatial resolution less than $1\,μ\text{m}$, yielding $κ\,=\,95^{+11}_{-7}\,\frac{\text{W}}{\text{m}\cdot \text{K}}$ for the $\textit{c}$-plane of our $\approx\,250\text{-nm}$-thick membrane at around room temperature, which compares well to our $\textit{ab initio}$ calculations applied to a simplified structure. Based on these calculations, we explain the particular relevance of the temperature probe volume, as quasi-ballistic transport of heat-carrying phonons occurs on length scales beyond the penetration depths of the heating laser and even its focus spot radius. The present work represents a significant step towards non-invasive, highly spatially resolved, and still quantitative thermometry performed on a photonic membrane.

physics.optics

Excitonic interplay between surface polar III-nitride quantum wells and MoS$_2$ monolayer

III-nitride wide bandgap semiconductors exhibit large exciton binding energies, preserving strong excitonic effects at room temperature. On the other hand, semiconducting two-dimensional (2D) materials, including MoS$_2$, also exhibit strong excitonic effects, attributed to enhanced Coulomb interactions. This study investigates excitonic interactions between surface GaN quantum well (QW) and 2D MoS$_2$ in van der Waals heterostructures by varying the spacing between these two excitonic systems. Optical property investigation first demonstrates the effective passivation of defect states at the GaN surface through MoS$_2$ coating. Furthermore, a strong interplay is observed between MoS$_2$ monolayers and GaN QW excitonic transitions. This highlights the interest of the 2D material/III-nitride QW system to study near-field interactions, such as Förster resonance energy transfer, which could open up novel optoelectronic devices based on such hybrid excitonic structures.

cond-mat.mes-hall

Polariton lasing in AlGaN microring with GaN/AlGaN quantum wells

Microcavity polaritons are strongly interacting hybrid light-matter quasiparticles, which are promising for the development of novel light sources and active photonic devices. Here, we report polariton lasing in the UV spectral range in microring resonators based on GaN/AlGaN slab waveguides, with experiments carried out from 4 K up to room temperature. Stimulated polariton relaxation into multiple ring resonator modes is observed, which exhibit threshold-like dependence of the emission intensity with pulse energy. The strong exciton-photon coupling regime is confirmed by the significant reduction of the free spectral range with energy and the blueshift of the exciton-like modes with increasing pulse energy. Importantly, the exciton emission shows no broadening with power, further confirming that lasing is observed at electron-hole densities well below the Mott transition. Overall, our work paves the way towards development of novel UV devices based on the high-speed slab waveguide polariton geometry operating up to room temperature with potential to be integrated into complex photonic circuits.

physics.optics

Near ultraviolet photonic integrated lasers based on silicon nitride

Low phase noise lasers based on the combination of III-V semiconductors and silicon photonics are well established in the near-infrared spectral regime. Recent advances in the development of low-loss silicon nitride-based photonic integrated resonators have allowed to outperform bulk external diode and fiber lasers in both phase noise and frequency agility in the 1550 nm-telecommunication window. Here, we demonstrate for the first time a hybrid integrated laser composed of a gallium nitride (GaN) based laser diode and a silicon nitride photonic chip-based microresonator operating at record low wavelengths as low as 410 nm in the near-ultraviolet wavelength region suitable for addressing atomic transitions of atoms and ions used in atomic clocks, quantum computing, or for underwater LiDAR. Using self-injection locking to a high Q (0.4 $\times$ 10$^6$) photonic integrated microresonator we observe a phase noise reduction of the Fabry-Pérot laser at 461 nm by a factor greater than 100$\times$, limited by the device quality factor and back-reflection.

physics.optics

Single photon emission and recombination dynamics in self-assembled GaN/AlN quantum dots

III-nitride quantum dots (QDs) are a promising system actively studied for their ability to maintain single photon emission up to room temperature. Here, we report on the evolution of the emission properties of self-assembled GaN/AlN QDs for temperatures ranging from 5 to 300K. We carefully track the photoluminescence of a single QD and measure an optimum single photon purity of g(2)(0) = 0.05+-0.02 at 5 K and 0.17+-0.8 at 300 K. We complement this study with temperaturedependent time-resolved photoluminescence measurements (TRPL) performed on a QD ensemble to further investigate the exciton recombination dynamics of such polar zero-dimensional nanostructures. By comparing our results to past reports, we emphasize the complexity of recombination processes in this system. Instead of the more conventional mono-exponential decay typical of exciton recombination, TRPL transients display a bi-exponential feature with short- and long-lived components that persist in the low excitation regime. From the temperature insensitivity of the long-lived excitonic component, we first discard the interplay of dark-to-bright state refilling in the exciton recombination process. Besides, this temperature-invariance also highlights the absence of nonradiative exciton recombinations, a likely direct consequence of the strong carrier confinement observed in GaN/AlN QDs up to 300K. Overall, our results support the viability of these dots as a potential single-photon source for quantum applications at room temperature.

physics.optics

Ultrafast-nonlinear ultraviolet pulse modulation in an AlInGaN polariton waveguide operating up to room temperature

Ultrafast nonlinear photonics enables a host of applications in advanced on-chip spectroscopy and information processing. These rely on a strong intensity dependent (nonlinear) refractive index capable of modulating optical pulses on sub-picosecond timescales and on length scales suitable for integrated photonics. Currently there is no platform that can provide this for the UV spectral range where broadband spectra generated by nonlinear modulation can pave the way to new on-chip ultrafast (bio-) chemical spectroscopy devices. We demonstrate the giant nonlinearity of UV hybrid light-matter states (exciton-polaritons) up to room temperature in an AlInGaN waveguide. We experimentally measure ultrafast nonlinear spectral broadening of UV pulses in a compact 100 $μ$m long device and deduce a nonlinearity 1000 times that in common UV nonlinear materials and comparable to non-UV polariton devices. Our demonstration promises to underpin a new generation of integrated UV nonlinear light sources for advanced spectroscopy and measurement.

physics.optics

Imaging non-radiative point defects buried in quantum wells using cathodoluminescence

Crystallographic point defects (PDs) can dramatically decrease the efficiency of optoelectronic semiconductor devices, many of which are based on quantum well (QW) heterostructures. However, spatially resolving individual non-radiative PDs buried in such QWs has so far not been demonstrated. Here, using high-resolution cathodoluminescence (CL) and a specific sample design, we spatially resolve, image, and analyse non-radiative PDs in InGaN/GaN QWs. We identify two different types of PD by their contrasting behaviour with temperature, and measure their densities from $10^{14}$ cm$^{-3}$ to as high as $10^{16}$ cm$^{-3}$. Our CL images clearly illustrate the interplay between PDs and carrier dynamics in the well: increasing PD concentration severely limits carrier diffusion lengths, while a higher carrier density suppresses the non-radiative behaviour of PDs. The results in this study are readily interpreted directly from CL images, and represent a significant advancement in nanoscale PD analysis.

cond-mat.mtrl-sci

Doubly resonant second-harmonic generation of a vortex beam from a bound state in the continuum

Second harmonic generation in nonlinear materials can be greatly enhanced by realizing doubly-resonant cavities with high quality factors. However, fulfilling such doubly resonant condition in photonic crystal (PhC) cavities is a long-standing challenge, because of the difficulty in engineering photonic bandgaps around both frequencies. Here, by implementing a second-harmonic bound state in the continuum (BIC) and confining it with a heterostructure design, we show the first doubly-resonant PhC slab cavity with $2.4\times10^{-2}$ W$^{-1}$ conversion efficiency under continuous wave excitation. We also report the confirmation of highly normal-direction concentrated far-field emission pattern with radial polarization at the second harmonic frequency. These results represent a solid verification of previous theoretical predictions and a cornerstone achievement, not only for nonlinear frequency conversion but also for vortex beam generation and prospective nonclassical sources of radiation.

physics.optics

Towards bright and pure single photon emitters at 300 K based on GaN quantum dots on silicon

Quantum dots (QDs) based on III-nitride semiconductors are promising for single photon emission at non-cryogenic temperatures due to their large exciton binding energies. Here, we demonstrate GaN QD single photon emitters operating at 300 K with $g^{(2)}(0) = 0.17 \pm 0.08$ under continuous wave excitation. At this temperature, single photon emission rates up to $6\times10^6 \, \text{s}^{-1}$ are reached while $g^{(2)}(0) \leq 0.5$ is maintained. Our results are achieved for GaN QDs embedded in a planar AlN layer grown on silicon, representing a promising pathway for future interlinkage with optical waveguides and cavities. These samples allow exploring the limiting factors to key performance metrics for single photon sources, such as brightness and single photon purity. While high brightness is assured by large exciton binding energies, the single photon purity is mainly affected by the spectral overlap with the biexcitonic emission. Thus, the performance of a GaN QD as a single photon emitter depends on the balance between the emission linewidth and the biexciton binding energy. We identify small GaN QDs with an emission energy in excess of 4.2 eV as promising candidates for future room temperature applications, since the biexciton binding energy becomes comparable to the average emission linewidth of around 55 meV.

cond-mat.mes-hall

Probing alloy formation using different excitonic species: The particular case of InGaN

Since the early 1960s, alloys are commonly grouped into two classes, featuring bound states in the bandgap (I) or additional, non-discrete band states (II). Microscopic material parameters for class I alloys can directly be extracted from photoluminescence (PL) spectra, whereas any conclusions drawn for class II alloys usually remain indirect and limited to macroscopic assertions. Nonetheless, here, we present a spectroscopic study on exciton localization in a so-called mixed crystal alloy (class II) that allows us to access microscopic alloy parameters. We study bulk In$_x$Ga$_{1-x}$N epilayers at the onset of alloy formation (0 $\leq$ $x$ $\leq$ 2.4%) in order to understand the material's particular robustness to defects. Based on an in-depth PL analysis it is demonstrated how different excitonic complexes (free, bound, and complex bound excitons) can serve as a probe to monitor the dilute limit of class II alloys. From an $x$-dependent linewidth analysis we extract the length scales at which excitons become increasingly localized, meaning that they convert from a free to a bound particle upon alloy formation. Already at x = 2.4% the average exciton diffusion length is reduced to 5.7 $\pm$ 1.3 nm at a temperature of 12 K, thus, detrimental exciton transfer mechanisms towards non-radiative defects are suppressed. In addition, the associated low temperature PL data suggests that a single indium atom does not suffice in order to permanently capture an exciton. Micro-PL spectra even give access to a forthright probing of silicon bound excitons embedded in a particular environment of indium atoms, thanks to the emergence of a hierarchy of individual, energetically sharp emission lines (full width at half maximum $\approx$ 300 $μ$eV). Consequently, the present study allows us to extract first microscopic alloy properties formerly only accessible for class I alloys.

cond-mat.mes-hall

On thresholdless lasing features in high-$β$ nitride nanobeam cavities: a quantum optical study

Exploring the limits of spontaneous emission coupling is not only one of the central goals in the development of nanolasers, it is also highly relevant regarding future large-scale photonic integration requiring energy-efficient coherent light sources with a small footprint. These studies are accompanied by a vivid debate on how to prove and interpret lasing in the high-$β$ regime. We investigate close-to-ideal spontaneous emission coupling in GaN nanobeam lasers grown on silicon. Due to their high optical quality, such nanobeam cavities allow for efficient funneling of spontaneous emission from the quantum well gain material into the laser mode. By performing a comprehensive optical and quantum-optical characterization, supported by microscopic modeling of the nanolasers, we identify high-$β$ lasing at room temperature and show a lasing transition in the absence of a threshold nonlinearity at 156 K. This peculiar characteristic is explained in terms of a temperature and excitation power dependent interplay between 0D and 2D gain contributions.

cond-mat.mes-hall

Propagating Polaritons in III-Nitride Slab Waveguides

We report on III-nitride waveguides with c-plane GaN/AlGaN quantum wells in the strong light-matter coupling regime supporting propagating polaritons. They feature a normal mode splitting as large as 60 meV at low temperatures thanks to the large overlap between the optical mode and the active region, a polariton decay length up to 100 $μ$m for photon-like polaritons and lifetime of 1-2 ps; with the latter values being essentially limited by residual absorption occurring in the waveguide. The fully lattice-matched nature of the structure allows for very low disorder and high in-plane homogeneity; an important asset for the realization of polaritonic integrated circuits that could support nonlinear polariton wavepackets up to room temperature thanks to the large exciton binding energy of 40 meV.

cond-mat.mes-hall

Efficient continuous-wave nonlinear frequency conversion in high-Q Gallium Nitride photonic crystal cavities on Silicon

We report on nonlinear frequency conversion from the telecom range via second harmonic generation (SHG) and third harmonic generation (THG) in suspended gallium nitride slab photonic crystal (PhC) cavities on silicon, under continuous-wave resonant excitation. Optimized two-dimensional PhC cavities with augmented far-field coupling have been characterized with quality factors as high as 4.4$\times10^{4}$, approaching the computed theoretical values. The strong enhancement in light confinement has enabled efficient SHG, achieving normalized conversion efficiency of 2.4$\times10^{-3}$ $W^{-1}$, as well as simultaneous THG. SHG emission power of up to 0.74 nW has been detected without saturation. The results herein validate the suitability of gallium nitride for integrated nonlinear optical processing.

physics.optics