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Clement Merckling

Publications and source records attributed to Clement Merckling.

12 recordsLinked to original sources

Stoichiometric Epitaxial Strontium Titanate Thin Films on Silicon by High-Temperature Sr Segregation

Thin-film strontium titanate (SrTiO$_3$, STO) layers grown on silicon require accurate stoichiometry and single-crystalline order to exploit their functional properties optimally. Oxide molecular beam epitaxy can provide an epitaxial interface, but suffers from source oxidation and resulting flux instabilities, yielding only a narrow growth process window for cationic stoichiometry control. Here, we investigate post-growth annealing in oxygen as a pathway to drive the STO layer toward stoichiometry in intentionally Sr-rich epitaxial STO films on silicon (001). Annealing over a broad temperature range revealed two distinct Sr-segregation mechanisms. Below 800 {\deg}C, excess Sr segregates toward the surface, forming SrO outgrowths that progressively sublimate at elevated temperatures. Above 800 {\deg}C, a second mechanism dominates: Sr accumulates within the interfacial SiO$_2$ layer formed by oxygen diffusion at the STO/Si interface. Together, these mechanisms effectively remove excess Sr from the STO lattice, yielding a more stoichiometric perovskite layer. Our results demonstrate that growing slightly Sr-rich STO templates followed by controlled annealing provides a practical route to improve crystalline quality, offering a scalable strategy for high-quality STO integration on silicon.

cond-mat.mtrl-sci

Disorder-driven symmetry suppression by van der Waals planar defects in a magnetic topological insulator

Magnetic topological insulators offer a platform to control electronic topology through magnetic order, yet reliable routes to tune their properties remain limited. Here, we show that ion irradiation allows to modify the magnetic and the topological properties of the van der Waals magnetic topological insulator MnBi$_2$Te$_4$. Using inert ion beams, intrinsic defects are introduced via collision cascades without chemical doping. We identify two distinct regimes. At low fluence, cation antisite disorder leads to a near-complete redistribution of Bi over cation sites while preserving long-range crystallographic order, accompanied by a transition from $p$-type to $n$-type transport. At high fluence, cation-anion intermixing drives the formation of a previously unreported layer-disordered phase characterized by a high density of van der Waals-specific planar defects, including swapped bilayers. Despite significant structural disorder, the system retains partial periodic order up to high displacement levels. Magnetometry and X-ray spectroscopy show that the Mn high-spin state and antiferromagnetic interactions persist, while magnetic anisotropy is strongly reduced. At the same time, the anomalous Hall conductivity is suppressed fivefold, far exceeding the change in magnetization, indicating a direct modification of Berry curvature. These results establish ion irradiation as a means to tune topology through defect engineering and reveal a disorder-driven approach to control symmetry and electronic structure in van der Waals magnetic materials.

cond-mat.mtrl-sci

Cryogenic piezoelectric effects in thin film strontium titanate devices

Next generation quantum technologies will need to rely on efficient transduction between electrical, optical, and mechanical quantum degrees of freedom to generate large-scale entanglement over large distances. The performance of such transducers is fundamentally limited by the cryogenic properties of the underlying materials. Here, we demonstrate that engineering strain in ferroelectric thin-film strontium titanate ($\mathrm{SrTiO_3}$) not only results in an exceptionally large Pockels coefficient, but also in a robust linear piezoelectric response at cryogenic temperatures, surpassing previous thin-film benchmarks. We measure piezoelectric tensor elements of $d_{15} = 151.8 \pm 1.5$ pm/V and $d_{33} = 54.8 \pm 4$ pm/V, and an effective photoelastic coefficient of $p_{\mathrm{eff}}$ = 0.56 at 5~K. Utilizing these enhanced properties, we demonstrate the first $\mathrm{SrTiO_3}$-on-oxide acousto-optic modulator with a voltage-length product ($V_{\pi}L$) of $0.874 \pm 0.084$ V cm, outperforming state-of-the-art unreleased modulators that typically feature a $V_{\pi}L$ of a few V cm. Our results establish thin-film $\mathrm{SrTiO_3}$ as a promising material system for integrated quantum photonics operating at cryogenic temperatures.

physics.optics

RTNinja: A generalized machine learning framework for analyzing random telegraph noise signals in nanoelectronic devices

Random telegraph noise is a prevalent variability phenomenon in nanoelectronic devices, arising from stochastic carrier exchange at defect sites and critically impacting device reliability and performance. Conventional analysis techniques often rely on restrictive assumptions or manual interventions, limiting their applicability to complex, noisy datasets. Here, we introduce RTNinja, a generalized, fully automated machine learning framework for the unsupervised analysis of random telegraph noise signals. RTNinja deconvolves complex signals to identify the number and characteristics of hidden individual sources without requiring prior knowledge of the system. The framework comprises two modular components: LevelsExtractor, which uses Bayesian inference and model selection to denoise and discretize the signal, and SourcesMapper, which infers source configurations through probabilistic clustering and optimization. To evaluate performance, we developed a Monte Carlo simulator that generates labeled datasets spanning broad signal-to-noise ratios and source complexities; across 7000 such datasets, RTNinja consistently demonstrated high-fidelity signal reconstruction and accurate extraction of source amplitudes and activity patterns. Our results demonstrate that RTNinja offers a robust, scalable, and device-agnostic tool for random telegraph noise characterization, enabling large-scale statistical benchmarking, reliability-centric technology qualification, predictive failure modeling, and device physics exploration in next-generation nanoelectronics.

cs.LG

Epitaxial growth of BaBiO3 thin films on SrTiO3(001) and MgO(001) substrates using molecular beam epitaxy and controlling their crystal orientations competition

BaBiO3 has lately gained high research attention as a parent material for an interesting family of alloyed compositions with multiple technological applications. In order to grow a variety of structures, a versatile deposition tool such as molecular beam epitaxy has to be employed. In this work, molecular beam epitaxy growth of BaBiO3 on SrTiO3(001) and MgO(001) substrates is studied. When grown by molecular beam epitaxy on SrTiO3(001) or MgO(001) substrates, BaBiO3 is known to have two competing orientations namely, (001) and (011). Characterization of the thin film is carried out by X-ray diffraction, X-ray reflectivity, atomic force microscopy, Rutherford backscattering, and transmission electron microscopy. Pathways to block the growth of BaBiO3(011) and only grow the technologically relevant BaBiO3(001) are described for both substrates. Understanding of the enabler mechanism of the co-growth is established from epitaxy point of view. This can be beneficially utilized for growth of the different compositions of BaBiO3 material family in a more controlled manner.

cond-mat.mtrl-sci

Structural transformation for BaBiO3-{\delta} thin films grown on SrTiO3-buffered Si(001) induced by an in-situ Molecular Beam Epitaxy cooldown process

Oxygen loss is one of the common defect types in perovskite oxides whose formation can be caused by a low oxygen background pressure during growth or by straining the thin film. Crystalline BaBiO3-{\delta} thin films are grown by molecular beam epitaxy on SrTiO3 buffered Si(001) substrates. Adsorption-controlled regime governs the epitaxy, as the sticking coefficient of bismuth is boosted by supplying activated oxygen at plasma power of 600 W during epitaxy. Even though activated oxygen is supplied during the growth process, large amount of oxygen vacancies is found to be created in the thin film depending on the cooldown process. Perovskite structure is obtained when the cooldown process includes an extended period of time during which activated oxygen at plasma power of 600 W is supplied. Another way for inducing the structural transformation is enabled via an ex-situ 600{\deg}C anneal step at molecular oxygen for the sample which includes oxygen vacancy channels. The transformation into perovskite structure BaBiO3 is manifested as reconstructed octahedra based on transmission electron microscopy, Raman spectroscopy, and photoluminescence. Additionally, smaller out-of-plane lattice constant as well as increased monoclinicity are observed for the perovskite phase supported by X-ray diffraction data. In this paper, thermal mismatch and multivalency-facilitated tensile strain exerted on the layers by the underlying Si substrates are presented as the driving force behind the creation of oxygen vacancies.

cond-mat.mtrl-sci

Engineering high Pockels coefficients in thin-film strontium titanate for cryogenic quantum electro-optic applications

Materials which exhibit the Pockels effect are notable for their strong electro-optic interaction and rapid response times and are therefore used extensively in classical electro-optic components for data and telecommunication applications. Yet many materials optimized for room-temperature operation see their Pockels coefficients at cryogenic temperatures significantly reduced - a major hurdle for emerging quantum technologies which have even more rigorous demands than their classical counterpart. A noted example is $\mathrm{BaTiO_3}$, which features the strongest effective Pockels coefficient at room temperature, only to see it reduced to a third (i.e. $\mathrm{r_{eff}} \approx$ 170 pm/V) at a few Kelvin. Here, we show that this behaviour is not inherent and can even be reversed: Strontium titanate ($\mathrm{SrTiO_3}$), a material normally not featuring a Pockels coefficient, can be engineered to exhibit an $\mathrm{r_{eff}}$ of 345 pm/V at cryogenic temperatures - a record value in any thin-film electro-optic material. By adjusting the stoichiometry, we can increase the Curie temperature and realise a ferroelectric phase that yields a high Pockels coefficient, yet with limited optical losses - on the order of decibels per centimetre. Our findings position $\mathrm{SrTiO_3}$ as one of the most promising materials for cryogenic quantum photonics applications.

physics.optics

Stoichiometry and Thickness of Epitaxial SrTiO$_{3}$ on Silicon (001): an Investigation of Physical, Optical and Electrical Properties

Strontium titanate (SrTiO$_{3}$, STO) stands out as a promising material for various electronic applications thanks to its exceptional dielectric properties. Molecular beam epitaxy is one of the few techniques which allows epitaxial growth of STO directly on industry-relevant silicon substrates. However, maintaining precise stoichiometry and high crystalline quality in this process remains a significant challenge. Establishing this is essential to obtain STO with bulk-like dielectric properties and to minimize leakage current and optical absorbance. In this study, the importance of cationic stoichiometry and the effect of thickness are investigated for STO thin films epitaxially grown on silicon. We employed real-time reflection high-energy electron diffraction (RHEED) as a feedback loop mechanism to counteract Sr source oxidation and maintain a constant flux. Additionally, high-temperature post-growth annealing treatments in O$_{2}$ were investigated to promote layer relaxation and reduce oxygen vacancy concentration, thereby improving the physical, electrical, and optical properties of stoichiometric STO. As a result, high-quality STO thin films exceeding 100 nm were successfully fabricated featuring a bulk-like out-of-plane lattice parameter and refractive index, as well as rocking curve full width at half maximum below 0.2{\deg}, smooth surface (R$_{q}$ < 0.2 nm) and a leakage current density below 1E-7 A/cm$^{2}$.

cond-mat.mtrl-sci

Observation of the radiative decay of the ${}^{229}\mathrm{Th}$ nuclear clock isomer

The nucleus of the radioisotope thorium-229 (${}^{229}$Th) features an isomer with an exceptionally low excitation energy that enables direct laser manipulation of nuclear states. For this reason, it is a leading candidate for use in next-generation optical clocks. This nuclear clock will be a unique tool, amongst others, for tests of fundamental physics. While first indirect experimental evidence for the existence of such an extraordinary nuclear state is significantly older, the proof of existence has been delivered only recently by observing the isomer's electron conversion decay and its hyperfine structure in a laser spectroscopy study, revealing information on the isomer's excitation energy, nuclear spin and electromagnetic moments. Further studies reported the electron conversion lifetime and refined the isomer's energy. In spite of recent progress, the isomer's radiative decay, a key ingredient for the development of a nuclear clock, remained unobserved. In this Letter, we report the detection of the radiative decay of this low-energy isomer in thorium-229 (${}^{229\mathrm{m}}$Th). By performing vacuum-ultraviolet spectroscopy of ${}^{229\mathrm{m}}$Th incorporated into large-bandgap CaF${}_2$ and MgF${}_2$ crystals at the ISOLDE facility at CERN, the photon vacuum wavelength of the isomer's decay is measured as 148.71(42) nm, corresponding to an excitation energy of 8.338(24) eV. This value is in agreement with recent measurements, and decreases the uncertainty by a factor of seven. The half-life of ${}^{229\mathrm{m}}$Th embedded in MgF${}_2$ is determined to be 670(102) s. The observation of the radiative decay in a large-bandgap crystal has important consequences for the design of a future nuclear clock and the improved uncertainty of the energy eases the search for direct laser excitation of the atomic nucleus.

nucl-ex

Epitaxy of new layered materials: 2D chalcogenides and challenges of weak van der Waals interactions

The application of new materials in nanotechnology opens new perspectives and enables ground-breaking innovations. Two-dimensional van der Waals materials and more specific, 2D chalcogenides are a promising class of new materials awaiting their usage in the semiconductor industry. However, the integration of van der Waals materials relying on industry-compatible manufacturing processes is still a major challenge. This is currently restricting the application of these new materials to the research laboratories environment only. The large-area and single-crystalline growth of van der Waals materials is one of the most important requirements to meet the challenging demands implied by the semiconductor industry. This review contributes to a more generalized understanding on the integration of van der Waals materials - and in more specific 2D chalcogenides - through the growth process of epitaxy. This, can pursue further the aspiration of large-area, single-crystalline and defect-free epitaxial integration of (quasi) van der Waals homo- and heterostructures into the great world of the semiconductor industry.

cond-mat.mtrl-sci

Towards twin-free molecular beam epitaxy of 2D chalcogenides explained by stronger interlayer van der Waals coupling

Defect-free epitaxial growth of 2D materials is one of the holy grails for a successful integration of van der Waals (vdW) materials in the semiconductor industry. The large-area (quasi-)vdW epitaxy of layered 2D chalcogenides is consequently carefully being researched since these materials hold very promising properties for future nanoelectronic applications. The formation of defects such as stacking faults like 60o twins and consequently 60o grain boundaries is still of major concern for the defect-free epitaxial growth of 2D chalcogenides. Although growth strategies to overcome the occurrence of these defects are currently being considered, more fundamental understanding on the origin of these defects at the initial stages of the growth is highly essential. Therefore this work focuses on the understanding of 60o twin formation in (quasi-)vdW epitaxy of 2D chalcogenides relying on systematic molecular beam epitaxy (MBE) experiments supported by density functional theory (DFT) calculations. The MBE experiments reveal the striking difference in 60o twin formation between WSe2 and Bi2Se3 in both quasi-vdW heteroepitaxy and vdW homoepitaxy, which from our DFT calculations links to the difference in interlayer vdW coupling strength. The stronger interlayer vdW coupling in Bi2Se3 compared to WSe2 results in a striking enhanced control on twin formation and hence shows significantly more promise for defect-free epitaxial integration. This interesting aspect of (quasi-)vdW epitaxy reveals that the strength of interlayer vdW coupling is key for functional 2D materials and opens perspectives for other vdW materials sharing strong interlayer interactions.

cond-mat.mtrl-sci

Room Temperature InP DFB Laser Array Directly Grown on (001) Silicon

Fully exploiting the silicon photonics platform requires a fundamentally new approach to realize high-performance laser sources that can be integrated directly using wafer-scale fabrication methods. Direct band gap III-V semiconductors allow efficient light generation but the large mismatch in lattice constant, thermal expansion and crystal polarity makes their epitaxial growth directly on silicon extremely complex. Here, using a selective area growth technique in confined regions, we surpass this fundamental limit and demonstrate an optically pumped InP-based distributed feedback (DFB) laser array grown on (001)-Silicon operating at room temperature and suitable for wavelength-division-multiplexing applications. The novel epitaxial technology suppresses threading dislocations and anti-phase boundaries to a less than 20nm thick layer not affecting the device performance. Using an in-plane laser cavity defined by standard top-down lithographic patterning together with a high yield and high uniformity provides scalability and a straightforward path towards cost-effective co-integration with photonic circuits and III-V FINFET logic.

physics.optics