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This article introduces a groundbreaking analytical workflow designed for the holistic characterisation, modelling and physical simulation of device heterostructures. Our innovative workflow autonomously, comprehensively and locally characterises the crystallographic information and 3D orientation of the crystal phases, the elemental composition, and the strain maps of devices from (scanning) transmission electron microscopy data. It converts a manual characterisation process that traditionally takes days into an automatic routine completed in minutes. This is achieved through a physics-guided artificial intelligence model that combines unsupervised and supervised machine learning in a modular way to provide a representative 3D description of the devices, materials structures, or samples under analysis. To culminate the process, we integrate the extracted knowledge to automate the generation of both 3D finite element and atomic models of millions of atoms acting as digital twins, enabling simulations that yield essential physical and chemical insights crucial for understanding the device's behaviour in practical applications. We prove this end-to-end workflow with a state-of-the-art materials platform based on SiGe planar heterostructures for hosting coherent and scalable spin qubits. Our workflow connects representative digital twins of the experimental devices with their theoretical properties to reveal the true impact that every atom in the structure has on their electronic properties, and eventually, into their functional quantum performance. Notably, the versatility of our workflow is demonstrated through its successful application to a wide array of materials systems, device configurations and sample morphologies.

We investigate the disorder properties of two-dimensional hole gases in Ge/SiGe heterostructures grown on Ge wafers, using thick SiGe barriers to mitigate the influence of the semiconductor-dielectric interface. Across several heterostructure field effect transistors we measure an average maximum mobility of $(4.4 \pm 0.2) \times 10^{6}~\mathrm{cm^2/Vs}$ at a saturation density of $(1.72 \pm 0.03) \times 10^{11}~\mathrm{cm^{-2}}$, corresponding to a long mean free path of $(30 \pm 1)~\mathrm{\mu m}$. The highest measured mobility is $4.68 \times 10^{6}~\mathrm{cm^2/Vs}$. We identify uniform background impurities and interface roughness as the dominant scattering mechanisms limiting mobility in a representative device, and we evaluate a percolation-induced critical density of $(4.5 \pm 0.1)\times 10^{9} ~\mathrm{cm^{-2}}$. This low-disorder heterostructure, according to simulations, may support the electrostatic confinement of holes in gate-defined quantum dots.

High kinetic inductance superconductors are gaining increasing interest for the realisation of qubits, amplifiers and detectors. Moreover, thanks to their high impedance, quantum buses made of such materials enable large zero-point fluctuations of the voltage, boosting the coupling rates to spin and charge qubits. However, fully exploiting the potential of disordered or granular superconductors is challenging, as their inductance and, therefore, impedance at high values are difficult to control. Here we have integrated a granular aluminium resonator, having a characteristic impedance exceeding the resistance quantum, with a germanium double quantum dot and demonstrate strong charge-photon coupling with a rate of $g_\text{c}/2\pi= (566 \pm 2)$ MHz. This was achieved due to the realisation of a wireless ohmmeter, which allows \emph{in situ} measurements during film deposition and, therefore, control of the kinetic inductance of granular aluminium films. Reproducible fabrication of circuits with impedances (inductances) exceeding 13 k$\Omega$ (1 nH per square) is now possible. This broadly applicable method opens the path for novel qubits and high-fidelity, long-distance two-qubit gates.

Whereas ferroelectricity may vanish in ultra-thin ferroelectric films, it is expected to emerge in ultra-thin anti-ferroelectric films, sparking people's interest in using antiferroelectric materials as an alternative to ferroelectric ones for high-density data storage applications. Lead Zirconate (PbZrO3) is considered the prototype material for antiferroelectricity, and indeed previous studies indicated that nanoscale PbZrO3 films exhibit ferroelectricity. The understanding of such phenomena from the microstructure aspect is crucial but still lacking. In this study, we fabricated a PbZrO3 film with thicknesses varying from 5 nm to 80 nm. Using Piezoresponse Force Microscopy, we discovered the film displayed a transition from antiferroelectric behaviour in the thicker areas to ferroelectric behaviour in the thinner ones, with a critical thickness between 10 and 15 nm. In this critical thickness range, a 12 nm PZO thin film was chosen for further study using aberration-corrected scanning transmission electron microscopy. The investigation showed that the film comprises both ferroelectric and ferrielectric phases. The ferroelectric phase is characterized by polarisation along the pseudocubic [011] projection direction. The positions of Pb, Zr, and O were determined using the integrated differential phase contrast method. This allowed us to ascertain that the ferroelectric PbZrO3 unit cell is half the size of that in the antiferroelectric phase on the ab plane. The observed unit cell is different from the electric field-induced ferroelectric rhombohedral phases. Additionally, we identified a ferrielectric phase with a unique up-up-zero-zero dipole configuration. The finding is crucial for understanding the performance of ultrathin antiferroelectric thin films and the subsequent design and development of antiferroelectric devices.

Using high resolution scanning transmission electron microscopy and low-loss electron energy loss spectroscopy, we correlate the local bandgap (Eg), indium concentration, and strain distribution across multiple InxGa1-xAs quantum wells (QWs), on a GaAs substrate, within a metamorphic laser structure. Our findings reveal significant inhomogeneities, particularly near the interfaces, for both the indium and strain distribution, and subtle variations in the Eg across individual QWs. The interplay between strain, composition, and Eg was further explored by density functional theory simulations, indicating that variations in the Eg are predominantly influenced by the indium concentration, with strain playing a minor role. The observed local inhomogeneities suggest that differences between individual QWs may affect the collective emission and performance of the final device. This study highlights the importance of spatially resolved analysis in understanding and optimising the electronic and optical properties for designing of next-generation metamorphic lasers with multiple QWs as the active region.

New approaches such as selective area growth, where crystal growth is lithographically controlled, allow the integration of bottom-up grown semiconductor nanomaterials in large-scale classical and quantum nanoelectronics. This calls for assessment and optimization of the reproducibility between individual components. We quantify the structural and electronic statistical reproducibility within large arrays of nominally identical selective area growth InAs nanowires. The distribution of structural parameters is acquired through comprehensive atomic force microscopy studies and transmission electron microscopy. These are compared to the statistical distributions of the cryogenic electrical properties of 256 individual SAG nanowire field effect transistors addressed using cryogenic multiplexer circuits. Correlating measurements between successive thermal cycles allows distinguishing between the contributions of surface impurity scattering and fixed structural properties to device reproducibility. The results confirm the potential of SAG nanomaterials, and the methodologies for quantifying statistical metrics are essential for further optimization of reproducibility.

The electrical characterisation of classical and quantum devices is a critical step in the development cycle of heterogeneous material stacks for semiconductor spin qubits. In the case of silicon, properties such as disorder and energy separation of conduction band valleys are commonly investigated individually upon modifications in selected parameters of the material stack. However, this reductionist approach fails to consider the interdependence between different structural and electronic properties at the danger of optimising one metric at the expense of the others. Here, we achieve a significant improvement in both disorder and valley splitting by taking a co-design approach to the material stack. We demonstrate isotopically-purified, strained quantum wells with high mobility of 3.14(8)$\times$10$^5$ cm$^2$/Vs and low percolation density of 6.9(1)$\times$10$^{10}$ cm$^{-2}$. These low disorder quantum wells support quantum dots with low charge noise of 0.9(3) $\mu$eV/Hz$^{1/2}$ and large mean valley splitting energy of 0.24(7) meV, measured in qubit devices. By striking the delicate balance between disorder, charge noise, and valley splitting, these findings provide a benchmark for silicon as a host semiconductor for quantum dot qubits. We foresee the application of these heterostructures in larger, high-performance quantum processors.

Bottom-up grown nanomaterials play an integral role in the development of quantum technologies. Among these, semiconductor nanowires (NWs) are widely used in proof-of-principle experiments, however, difficulties in parallel processing of conventionally-grown NWs makes scalability unfeasible. Here, we harness selective area growth (SAG) to remove this road-block. We demonstrate large scale integrated SAG NW circuits consisting of 512 channel multiplexer/demultiplexer pairs, incorporating thousands of interconnected SAG NWs operating under deep cryogenic conditions. Multiplexers enable a range of new strategies in quantum device research and scaling by increase the device count while limiting the number of connections between room-temperature control electronics and the cryogenic samples. As an example of this potential we perform a statistical characterization of large arrays of identical SAG quantum dots thus establishing the feasibility of applying cross-bar gating strategies for efficient scaling of future SAG quantum circuits., Comment: Main text and Supplementary Information

Morphological control at the nanoscale paves the way to fabricate nanostructures with desired plasmonic properties. We report the nanoengineering of plasmon resonances in 1D hollow nanostructures of two different AuAg nanotubes; completely hollow nanotubes and hybrid nanotubes comprising solid Ag and hollow AuAg segments. Spatially resolved plasmon mapping by electron energy loss spectroscopy (EELS) revealed the presence of high order resonator-like modes and localized surface plasmon resonance (LSPR) modes in both nanotubes. Experimental findings are accurately correlated with boundary element method (BEM) simulations, where both experiments and simulations revealed that the plasmon resonances are intensely present inside the nanotubes due to plasmon hybridization. Based on the experimental and simulated results reported, we show that the novel hybrid AuAg nanotubes possess two significant coexisting features: (i) LSPRs have been generated distinctively from the hollow and solid parts of the hybrid AuAg nanotube, which opens the way to control a broad range of plasmon resonances with one single nanostructure and (ii) the periodicity of the high-order modes are disrupted due to the plasmon hybridization by the interaction of solid and hollow parts, resulting in an asymmetrical plasmon distribution in 1D nanostructures. The asymmetry could be modulated/engineered leading to control coded plasmonic nanotubes.

Hybrid semiconductor/superconductor nanowires constitute a pervasive platform for studying gate-tunable superconductivity and the emergence of topological behavior. Their low-dimensionality and crystal structure flexibility facilitate novel heterostructure growth and efficient material optimization; crucial prerequisites for accurately constructing complex multi-component quantum materials. Here, we present an extensive optimization of Sn growth on InSb, InAsSb and InAs nanowires. We demonstrate how the growth conditions and the crystal structure/symmetry of the semiconductor drive the formation of either semi-metallic $\mathrm{\alpha-Sn}$ or superconducting $\mathrm{\beta-Sn}$. For InAs nanowires, we obtain phase-pure, superconducting $\mathrm{\beta-Sn}$ shells. However, for InSb and InAsSb nanowires, an initial epitaxial $\mathrm{\alpha-Sn}$ phase evolves into a polycrystalline shell of coexisting $\mathrm{\alpha}$ and $\mathrm{\beta}$ phases, where the $\beta/\alpha$ volume ratio increases with Sn shell thickness. Whether these nanowires exhibit superconductivity or not critically relies on the $\mathrm{\beta-Sn}$ content. Therefore, this work provides key insights into Sn phase control on a variety of semiconductors, with consequences for the yield of superconducting hybrids suitable for generating topological systems., Comment: 12 pages, 5 figures

In the archetypal antiferroelectric PbZrO3, antiparallel electric dipoles cancel each other, resulting in zero spontaneous polarisation at the macroscopic level. Yet in actual hysteresis loops, the cancellation is rarely perfect and some remnant polarization is often observed, suggesting the metastability of polar phases in this material. In this work, using aberration-corrected scanning transmission electron microscopy methods on a PbZrO3 single crystal, we uncover the coexistence of the common antiferroelectric phase and a ferrielectric phase featuring an electric dipole pattern of "up down up". This dipole arrangement, predicted by Aramberri et al. (2021) to be the ground state of PbZrO3 at 0K, appears at room temperature in the form of translational boundaries that aggregate to form wider stripe domains of the polar phase embedded within the antiferroelectric matrix.

The co-integration of spin, superconducting, and topological systems is emerging as an exciting pathway for scalable and high-fidelity quantum information technology. High-mobility planar germanium is a front-runner semiconductor for building quantum processors with spin-qubits, but progress with hybrid superconductor-semiconductor devices is hindered because obtaining a superconducting gap free of subgap states (hard gap) has proven difficult. Here we solve this challenge by developing a low-disorder, oxide-free interface between high-mobility planar germanium and a germanosilicide parent superconductor. This superconducting contact is formed by the thermally-activated solid phase reaction between a metal (Pt) and the semiconductor heterostructure (Ge/SiGe). Electrical characterization reveals near-unity transparency in Josephson junctions and, importantly, a hard induced superconducting gap in quantum point contacts. Furthermore, we demonstrate phase control of a Josephson junction and study transport in a gated two-dimensional superconductor-semiconductor array towards scalable architectures. These results expand the quantum technology toolbox in germanium and provide new avenues for exploring monolithic superconductor-semiconductor quantum circuits towards scalable quantum information processing.

Hybrid semiconductor-superconductor devices hold great promise for realizing topological quantum computing with Majorana zero modes (MZMs). However, multiple claims of Majorana detection, based on either tunneling or Coulomb blockade (CB) spectroscopy, remain disputed. Here we devise an experimental protocol that allows to perform both types of measurements on the same hybrid island by adjusting its charging energy via tunable junctions to the normal leads. This method reduces ambiguities of Majorana detections by checking the consistency between CB spectroscopy and zero bias peaks (ZBPs) in non-blockaded transport.Specifically, we observe junction-dependent, even-odd modulated, single-electron CB peaks in InAs/Al hybrid nanowires (NWs) without concomitant low-bias peaks in tunneling spectroscopy. We provide a theoretical interpretation of the experimental observations in terms of low-energy, longitudinally-confined island states rather than overlapping Majorana modes. Our results highlight the importance of combined measurements on the same device for the identification of topological MZMs.

Selective area growth (SAG) of nanowires and networks promise a route toward scalable electronics, photonics and quantum devices based on III-V semiconductor materials. The potential of high-mobility SAG nanowires however is not yet fully realized, since interfacial roughness, misfit dislocations at the nanowire/substrate interface and non-uniform composition due to material intermixing all scatter electrons. Here, we explore SAG of highly lattice-mismatched InAs nanowires on insulating GaAs(001) substrates and address these key challenges. Atomically smooth nanowire/substrate interfaces are achieved with the use of atomic hydrogen (a-H) as an alternative to conventional thermal annealing for the native oxide removal. The problem of high lattice mismatch is addressed through an In$_x$Ga$_{1-x}$As buffer layer introduced between the InAs transport channel and the GaAs substrate. The Ga-In material intermixing observed in both the buffer layer and the channel is inhibited via careful tuning of the growth temperature. Performing scanning transmission electron microscopy and x-ray diffraction analysis along with low-temperature transport measurements we show that optimized In-rich buffer layers promote high quality InAs transport channels with the field-effect electron mobility over~10000~cm$^2$V$^{-1}$s$^{-1}$. This is twice as high as for non-optimized samples and among the highest reported for InAs selective area grown nanostructures., Comment: Main text: 9 pages, 5 figures Supporting Information is available at https://erda.ku.dk/archives/d3b11c9d399dd9a715c5e2c84870e3c4/published-archive.html

Hole gases in planar germanium can have high mobilities in combination with strong spin-orbit interaction and electrically tunable g-factors, and are therefore emerging as a promising platform for creating hybrid superconductor-semiconductor devices. A key challenge towards hybrid Ge-based quantum technologies is the design of high-quality interfaces and superconducting contacts that are robust against magnetic fields. In this work, by combining the assets of aluminum, which provides good contact to the Ge, and niobium, which has a significant superconducting gap, we demonstrate highly transparent low-disordered JoFETs with relatively large \IcRn \ products that are capable of withstanding high magnetic fields. We furthermore demonstrate the ability of phase-biasing individual JoFETs, opening up an avenue to explore topological superconductivity in planar Ge. The persistence of superconductivity in the reported hybrid devices beyond 1.8 Tesla paves the way towards integrating spin qubits and proximity-induced superconductivity on the same chip.

Spin qubits are considered to be among the most promising candidates for building a quantum processor. GroupIV hole spin qubits have moved into the focus of interest due to the ease of operation and compatibility with Si technology. In addition, Ge offers the option for monolithic superconductor-semiconductor integration. Here we demonstrate a hole spin qubit operating at fields below 10 mT, the critical field of Al, by exploiting the large out-of-plane hole g-factors in planar Ge and by encoding the qubit into the singlet-triplet states of a double quantum dot. We observe electrically controlled g-factor-difference-driven and exchange-driven rotations with tunable frequencies exceeding 100 MHz and dephasing times of 1 $\mu$s which we extend beyond 150 $\mu$s with echo techniques. These results demonstrate that Ge hole singlet-triplet qubits are competing with state-of-the art GaAs and Si singlet-triplet qubits. In addition, their rotation frequencies and coherence are on par with Ge single spin qubits, but they can be operated at much lower fields underlining their potential for on chip integration with superconducting technologies.

Phonon surface scattering has been at the core of heat transport engineering in nanoscale structures and devices. Herein, we demonstrate that this phonon pathway can be the sole mechanism only below a characteristic, size-dependent temperature. Above this temperature, the lattice phonon scattering co-exist along with surface effects. By artificially controlling mass disorder and lattice dynamics at the atomic-level in nanowires without affecting morphology, crystallinity, chemical composition, and electronic properties, the temperature-thermal conductivity-diameter triple parameter space is mapped, and the main phonon scattering mechanisms are disentangled. This led to the identification of the critical temperature at which the effect of lattice mass-disorder on thermal conductivity is suppressed to an extent that phonon transport becomes governed entirely by the surface. This behavior is discussed based on Landauer-Dutta-Lundstrom near-equilibrium transport model. The established framework provides the necessary input to further advance the design and modelling of phonon and heat transport in semiconductor nanoscale systems., Comment: 12 pages text, 4 Figures, 13 pages Supplementary Information

Nanowires can serve as flexible substrates for hybrid epitaxial growth on selected facets, allowing for design of heterostructures with complex material combinations and geometries. In this work we report on hybrid epitaxy of semiconductor - ferromagnetic insulator - superconductor (InAs/EuS/Al) nanowire heterostructures. We study the crystal growth and complex epitaxial matching of wurtzite InAs / rock-salt EuS interfaces as well as rock-salt EuS / face-centered cubic Al interfaces. Because of the magnetic anisotropy originating from the nanowire shape, the magnetic structure of the EuS phase are easily tuned into single magnetic domains. This effect efficiently ejects the stray field lines along the nanowires. With tunnel spectroscopy measurements of the density of states, we show the material has a hard induced superconducting gap, and magnetic hysteretic evolution which indicates that the magnetic exchange fields are not negligible. These hybrid nanowires fulfil key material requirements for serving as a platform for spin-based quantum applications, such as scalable topological quantum computing., Comment: 15 pages, 5 figures

Hybrid semiconductor-ferromagnetic insulator heterostructures are interesting due to their tunable electronic transport, self-sustained stray field and local proximitized magnetic exchange. In this work, we present lattice matched hybrid epitaxy of semiconductor - ferromagnetic insulator InAs/EuS heterostructures and analyze the atomic-scale structure as well as their electronic and magnetic characteristics. The Fermi level at the InAs/EuS interface is found to be close to the InAs conduction band and in the bandgap of EuS, thus preserving the semiconducting properties. Both neutron and X-ray reflectivity measurements show that the ferromagnetic component is mainly localized in the EuS thin film with a suppression of the Eu moment in the EuS layer nearest the InAs. Induced moments in the adjacent InAs layers were not detected although our ab initio calculations indicate a small exchange field in the InAs layer. This work presents a step towards realizing high quality semiconductor - ferromagnetic insulator hybrids, which is a critical requirement for development of various quantum and spintronic applications without external magnetic fields.