Spin cross-correlation experiments in an electron entangler.

Correlations are fundamental in describing many-body systems. However, in experiments, correlations are notoriously difficult to assess on a microscopic scale, especially for electron spins. Even though it is firmly established theoretically that the electrons in a Cooper pair1 of a superconductor form maximally spin-entangled singlet states with opposite spin projections2-4, no spin correlation experiments have been demonstrated so far. Here we report the direct measurement of the spin cross-correlations between the currents of a Cooper pair splitter5-13, an electronic device that emits electrons originating from Cooper pairs. We use ferromagnetic split-gates14,15, compatible with nearby superconducting structures, to individually spin polarize the transmissions of the quantum dots in the two electronic paths, which act as tunable spin filters. The signals are detected in standard transport and in highly sensitive transconductance experiments. We find that the spin cross-correlation is negative, consistent with spin singlet emission, and deviates from the ideal value mostly due to the overlap of the Zeeman split quantum dot states. Our results demonstrate a new route to perform spin correlation experiments in nano-electronic devices, especially suitable for those relying on magnetic field sensitive superconducting elements, like triplet or topologically non-trivial superconductors16-18, or to perform Bell tests with massive particles19,20.

Spin-Resolved Magneto-Tunneling and Giant Anisotropic g-Factor in Broken Gap InAs-GaSb Core-Shell Nanowires.

We experimentally and computationally investigate the magneto-conductance across the radial heterojunction of InAs-GaSb core-shell nanowires under a magnetic field, B, up to 30 T and at temperatures in the range 4.2-200 K. The observed double-peak negative differential conductance markedly blue-shifts with increasing B. The doublet accounts for spin-polarized currents through the Zeeman split channels of the InAs (GaSb) conduction (valence) band and exhibits strong anisotropy with respect to B orientation and marked temperature dependence. Envelope function approximation and a semiclassical (WKB) approach allow to compute the magnetic quantum states of InAs and GaSb sections of the nanowire and to estimate the B-dependent tunneling current across the broken-gap interface. Disentangling different magneto-transport channels and a thermally activated valence-to-valence band transport current, we extract the g-factor from the spin-up and spin-down dI/dV branch dispersion, revealing a giant, strongly anisotropic g-factor in excess of 60 (100) for the radial (tilted) field configurations.

Josephson Diode Effect in High-Mobility InSb Nanoflags.

We report nonreciprocal dissipation-less transport in single ballistic InSb nanoflag Josephson junctions. Applying an in-plane magnetic field, we observe an inequality in supercurrent for the two opposite current propagation directions. Thus, these devices can work as Josephson diodes, with dissipation-less current flowing in only one direction. For small fields, the supercurrent asymmetry increases linearly with external field, and then it saturates as the Zeeman energy becomes relevant, before it finally decreases to zero at higher fields. The effect is maximum when the in-plane field is perpendicular to the current vector, which identifies Rashba spin-orbit coupling as the main symmetry-breaking mechanism. While a variation in carrier concentration in these high-quality InSb nanoflags does not significantly influence the supercurrent asymmetry, it is instead strongly suppressed by an increase in temperature. Our experimental findings are consistent with a model for ballistic short junctions and show that the diode effect is intrinsic to this material.

Quantum-Dot Single-Electron Transistors as Thermoelectric Quantum Detectors at Terahertz Frequencies.

Low-dimensional nanosystems are promising candidates for manipulating, controlling, and capturing photons with large sensitivities and low noise. If quantum engineered to tailor the energy of the localized electrons across the desired frequency range, they can allow devising of efficient quantum sensors across any frequency domain. Here, we exploit the rich few-electron physics to develop millimeter-wave nanodetectors employing as a sensing element an InAs/InAs0.3P0.7 quantum-dot nanowire, embedded in a single-electron transistor. Once irradiated with light, the deeply localized quantum element exhibits an extra electromotive force driven by the photothermoelectric effect, which is exploited to efficiently sense radiation at 0.6 THz with a noise equivalent power <8 pWHz-1/2 and almost zero dark current. The achieved results open intriguing perspectives for quantum key distributions, quantum communications, and quantum cryptography at terahertz frequencies.

Impact of electrostatic doping on carrier concentration and mobility in InAs nanowires.

We fabricate dual-gated electric double layer (EDL) field effect transistors based on InAs nanowires gated with an ionic liquid, and we perform electrical transport measurements in the temperature range from room temperature to 4.2 K. By adjusting the spatial distribution of ions inside the ionic liquid employed as gate dielectric, we electrostatically induce doping in the nanostructures under analysis. We extract low-temperature carrier concentration and mobility in very different doping regimes from the analysis of current-voltage characteristics and transconductances measured exploiting global back-gating. In the liquid gate voltage interval from -2 to 2 V, carrier concentration can be enhanced up to two orders of magnitude. Meanwhile, the effect of the ionic accumulation on the nanowire surface turns out to be detrimental to the electron mobility of the semiconductor nanostructure: the electron mobility is quenched irrespectively to the sign of the accumulated ionic species. The reported results shine light on the effective impact on crucial transport parameters of EDL gating in semiconductor nanodevices and they should be considered when designing experiments in which electrostatic doping of semiconductor nanostructures via electrolyte gating is involved.

Proximitized Josephson junctions in highly-doped InAs nanowires robust to optical illumination.

We have studied the effects of optical-frequency light on proximitized InAs/Al Josephson junctions based on highly n-doped InAs nanowires at varying incident photon flux and at three different photon wavelengths. The experimentally obtained IV curves were modeled using a resistively shunted junction model which takes scattering at the contact interfaces into account. Despite the fact that the InAs weak link is photosensitive, the Josephson junctions were found to be surprisingly robust, interacting with the incident radiation only through heating, whereas above the critical current our devices showed non-thermal effects resulting from photon exposure. Our work indicates that Josephson junctions based on highly-doped InAs nanowires can be integrated in close proximity to photonic circuits. The results also suggest that such junctions can be used for optical-frequency photon detection through thermal processes by measuring a shift in critical current.

Orbital Tuning of Tunnel Coupling in InAs/InP Nanowire Quantum Dots.

We report results on the control of barrier transparency in InAs/InP nanowire quantum dots via the electrostatic control of the device electron states. Recent works demonstrated that barrier transparency in this class of devices displays a general trend just depending on the total orbital energy of the trapped electrons. We show that a qualitatively different regime is observed at relatively low filling numbers, where tunneling rates are rather controlled by the axial configuration of the electron orbital. Transmission rates versus filling are further modified by acting on the radial configuration of the orbitals by means of electrostatic gating, and the barrier transparency for the various orbitals is found to evolve as expected from numerical simulations. The possibility to exploit this mechanism to achieve a controlled continuous tuning of the tunneling rate of an individual Coulomb blockade resonance is discussed.

Morphology control of single-crystal InSb nanostructures by tuning the growth parameters.

Research interest in indium antimonide (InSb) has increased significantly in recent years owing to its intrinsic properties and the consequent opportunities to implement next-generation quantum devices. Hence, the precise, reproducible control over morphology and crystalline quality becomes of paramount importance for a practical quantum-device technology. Here, we investigate the growth of InSb nanostructures with different morphologies on InAs stems without pre-growth efforts (patterning). InSb nanostructures such as nanowires (1D), nanoflags (2D) and nanocubes (3D) have been realized by means of Au-assisted chemical beam epitaxy by tailoring the growth parameters like growth temperature, precursor fluxes, sample rotation and substrate orientation. Through morphological and crystallographic characterization, all the as-grown InSb 2D nanostructures are found to be single-crystalline with zinc blende structure, free from any defects such as stacking faults and twin planes. The existence of two families of 2D nanostructures, characterised by an aperture angle at the base of 145° and 160°, is observed and modelled. This study provides useful guidelines for the controlled growth of high-quality InSb nanostructures with different shape.

Thermoelectric Conversion at 30 K in InAs/InP Nanowire Quantum Dots.

We demonstrate high-temperature thermoelectric conversion in InAs/InP nanowire quantum dots by taking advantage of their strong electronic confinement. The electrical conductance G and the thermopower S are obtained from charge transport measurements and accurately reproduced with a theoretical model accounting for the multilevel structure of the quantum dot. Notably, our analysis does not rely on the estimate of cotunnelling contributions, since electronic thermal transport is dominated by multilevel heat transport. By taking into account two spin-degenerate energy levels we are able to evaluate the electronic thermal conductance K and investigate the evolution of the electronic figure of merit ZT as a function of the quantum dot configuration and demonstrate ZT ≈ 35 at 30 K, corresponding to an electronic efficiency at maximum power close to the Curzon-Ahlborn limit.

Growth dynamics of InAs/InP nanowire heterostructures by Au-assisted chemical beam epitaxy.

The steady-state chemical composition of the In/Au alloy nanoparticles (NPs) during isothermal growth of Au-assisted InAs and InP nanowires (NWs) is different for the two materials. Therefore, when switching from one material to the other, to grow axial NW heterostructures, transient effects dominate during the time period of the NP reconfiguration. As a consequence, the precise control of the thickness of thin InP and InAs segments, which is fundamental for the realization of quantum dot (QD) structures and superlattices, can be very challenging. In this work, we present a study of the thickness/diameter dependence of two InP barriers and of the InAs short segment in between (QD), inserted into InAs NWs grown by means of Au-assisted chemical beam epitaxy. We found a broad variability of the InP segment thickness within the same as-grown sample, resulting in InAs NWs with asymmetric and non-homogeneous InP barriers. We explain the results by considering the NP reconfiguration dynamics which dominates at the early stages of the growth in both growth sequences. Moreover, we propose a strategy to control the growth rate and the dynamics of the barriers, by forcing the NP reconfiguration before starting the InP growth. This allows for the realization of InAs/InP NW heterostructures of different diameters, all having symmetric InP barriers with well controlled thickness, which are crucial parameters for the realization of advanced electronic quantum devices.

Highly symmetric and tunable tunnel couplings in InAs/InP nanowire heterostructure quantum dots.

We present a comprehensive electrical characterization of an InAs/InP nanowire (NW) heterostructure, comprising of two InP barriers forming a quantum dot (QD), two adjacent lead segments and two metallic contacts. We demonstrate how to extract valuable quantitative information of the QD. The QD shows very regular Coulomb blockade resonances over a large gate voltage range. By analyzing the resonance line shapes, we map the evolution of the tunnel couplings from the few to the many electron regime, with electrically tunable tunnel couplings from <1 µeV to >600 µeV, and a transition from the temperature to the lifetime broadened regime. The InP segments form tunnel barriers with almost fully symmetric tunnel couplings and a barrier height of ∼350 meV. All of these findings can be understood in great detail based on the deterministic material composition and geometry. Our results demonstrate that integrated InAs/InP QDs provide a promising platform for electron tunneling spectroscopy in InAs NWs, which can readily be contacted by a variety of superconducting materials to investigate subgap states in proximitized NW regions, or be used to characterize thermoelectric nanoscale devices in the quantum regime.

Conductometric Sensing with Individual InAs Nanowires.

In this work, we isolate individual wurtzite InAs nanowires and fabricate electrical contacts at both ends, exploiting the single nanostructures as building blocks to realize two different architectures of conductometric sensors: (a) the nanowire is drop-casted onto-supported by-a SiO2/Si substrate, and (b) the nanowire is suspended at approximately 250 nm from the substrate. We test the source-drain current upon changes in the concentration of humidity, ethanol, and NO2, using synthetic air as a gas carrier, moving a step forward towards mimicking operational environmental conditions. The supported architecture shows higher response in the mid humidity range (50% relative humidity), with shorter response and recovery times and lower detection limit with respect to the suspended nanowire. These experimental pieces of evidence indicate a minor role of the InAs/SiO2 contact area; hence, there is no need for suspended nanostructures to improve the sensing performance. Moreover, the sensing capability of single InAs nanowires for detection of NO2 and ethanol in the ambient atmosphere is reported and discussed.

Nanoparticle Stability in Axial InAs-InP Nanowire Heterostructures with Atomically Sharp Interfaces.

The possibility to expand the range of material combinations in defect-free heterostructures is one of the main motivations for the great interest in semiconductor nanowires. However, most axial nanowire heterostructures suffer from interface compositional gradients and kink formation, as a consequence of nanoparticle-nanowire interactions during the metal-assisted growth. Understanding such interactions and how they affect the growth mode is fundamental to achieve a full control over the morphology and the properties of nanowire heterostructures for device applications. Here we demonstrate that the sole parameter affecting the growth mode (straight or kinked) of InP segments on InAs nanowire stems by the Au-assisted method is the nanoparticle composition. Indeed, straight InAs-InP nanowire heterostructures are obtained only when the In/Au ratio in the nanoparticles is low, typically smaller than 1.5. For higher In content, the InP segments tend to kink. Tailoring the In/Au ratio by the precursor fluxes at a fixed growth temperature enables us to obtain straight and radius-uniform InAs-InP nanowire heterostructures (single and double) with atomically sharp interfaces. We present a model that is capable of describing all the experimentally observed phenomena: straight growth versus kinking, the stationary nanoparticle compositions in pure InAs and InAs-InP nanowires, the crystal phase trends, and the interfacial abruptness. By taking into account different nanowire/nanoparticle interfacial configurations (forming wetting or nonwetting monolayers in vertical or tapered geometry), our generalized model provides the conditions of nanoparticle stability and abrupt heterointerfaces for a rich variety of growth scenarios. Therefore, our results provide a powerful tool for obtaining high quality InAs-InP nanowire heterostructures with well-controlled properties and can be extended to other material combinations based on the group V interchange.

Catalyst Composition Tuning: The Key for the Growth of Straight Axial Nanowire Heterostructures with Group III Interchange.

Au-catalyzed III-V nanowire heterostructures based on the group III interchange usually grow straight only in one of the two growth sequences, whereas the other sequence produces kinked geometries; thus, the realization of double heterostructures remains challenging. Here, we investigate the growth of Au-assisted InAs-GaAs and GaAs-InAs axial nanowire heterostructures. A detailed study of the heterostructure morphology as a function of growth parameters and chemical composition of the catalyst nanoparticle is performed by means of scanning electron microscopy, transmission electron microscopy, and energy-dispersive X-ray analysis. Our results clearly demonstrate that the nanoparticle composition, rather than other growth parameters, as postulated so far, controls the growth mode and the resulting nanowire morphology. Although GaAs easily grows straight on InAs, straight growth of InAs on GaAs is achieved only if the nanoparticle composition is properly tuned. We find that straight InAs segments on GaAs require high group III-to-Au ratios in the nanoparticle (greater than 0.8); otherwise, the droplet wets the sidewalls and the nanowire kinks. We discuss the observed behavior within a theoretical model that relates the nanoparticle stability to the group III-to-Au ratio. Based on this finding, we demonstrate the growth of straight nanowire heterostructures for both sequences. The proposed strategy can be extended to other III-V nanowire heterostructures based on the group III interchange, allowing for straight morphology regardless of the growth sequence, and ultimately for designing nanowire heterostructures with the required properties for different applications.

Zincblende InAsxP1-x/InP Quantum Dot Nanowires for Telecom Wavelength Emission.

InAsxP1-x quantum dots (QDs) in InP nanowires (NWs) have been realized as a platform for emission at telecom wavelengths. These QDs are typically grown in NWs with the wurtzite crystal phase, but in this case, ultrathin diameters are required to achieve defect-free heterostructures, making the structures less robust. In this work, we demonstrate the growth of pure zincblende InAsxP1-x QDs in InP NWs, which enabled an increase in NW diameters to about 45 nm, achieved by employing Au-assisted vapor liquid solid growth in a chemical beam epitaxy system. We studied the growth of InP/InAsxP1-x heterostructures with different compositions to control the straight growth along the ⟨100⟩ direction and to tune the emission wavelength. Interestingly, we found that the growth mechanism for pure InAs QDs is different compared to that for InAsxP1-x alloy QDs. This allowed us to optimize different growth protocols to achieve straight growth of the final QD NWs. We successfully obtained the growth of InAsxP1-x QDs with a composition in the range of x = 0.24-1.00. By means of microphotoluminescence measurements, we demonstrate the tunability of the emission in dependence of the InAsxP1-x QD composition and morphology, remarkably observing an emission at the telecom O-band for a 10 nm thick QD with 80% of As content.

GaAs/GaP superlattice nanowires: growth, vibrational and optical properties.

Nanowire geometry allows semiconductor heterostructures to be obtained that are not achievable in planar systems, as in, for example, axial superlattices made of large lattice mismatched materials. This provides a great opportunity to explore new optical transitions and vibrational properties resulting from the superstructure. Moreover, superlattice nanowires are expected to show improved thermoelectric properties, owing to the dominant role of surfaces and interfaces that can scatter phonons more effectively, reducing the lattice thermal conductivity. Here, we show the growth of long (up to 100 repetitions) GaAs/GaP superlattice nanowires with different periodicities, uniform layer thicknesses, and sharp interfaces, realized by means of Au-assisted chemical beam epitaxy. By optimizing the growth conditions, we obtained great control of the nanowire diameter, growth rate, and superlattice periodicity, offering a valuable degree of freedom for engineering photonic and phononic properties at the nanoscale. As a proof of concept, we analyzed a single type of superlattice nanowire with a well-defined periodicity and we observed room temperature optical emission and new phonon modes. Our results prove that high-quality GaAs/GaP superlattice nanowires have great potential for phononic and optoelectronic studies and applications.

Heat-Driven Iontronic Nanotransistors.

Thermoelectric polyelectrolytes are emerging as ideal material platform for self-powered bio-compatible electronic devices and sensors. However, despite the nanoscale nature of the ionic thermodiffusion processes underlying thermoelectric efficiency boost in polyelectrolytes, to date no evidence for direct probing of ionic diffusion on its relevant length and time scale has been reported. This gap is bridged by developing heat-driven hybrid nanotransistors based on InAs nanowires embedded in thermally biased Na+ -functionalized (poly)ethyleneoxide, where the semiconducting nanostructure acts as a nanoscale probe sensitive to the local arrangement of the ionic species. The impact of ionic thermoelectric gating on the nanodevice electrical response is addressed, investigating the effect of device architecture, bias configuration and frequency of the heat stimulus, and inferring optimal conditions for the heat-driven nanotransistor operation. Microscopic quantities of the polyelectrolyte such as the ionic diffusion coefficient are extracted from the analysis of hysteretic behaviors rising in the nanodevices. The reported experimental platform enables simultaneously the ionic thermodiffusion and nanoscale resolution, providing a framework for direct estimation of polyelectrolytes microscopic parameters. This may open new routes for heat-driven nanoelectronic applications and boost the rational design of next-generation polymer-based thermoelectric materials.

GaAs/GaP Superlattice Nanowires for Tailoring Phononic Properties at the Nanoscale: Implications for Thermal Engineering.

The possibility to tune the functional properties of nanomaterials is key to their technological applications. Superlattices, i.e., periodic repetitions of two or more materials in one or more dimensions, are being explored for their potential as materials with tailor-made properties. Meanwhile, nanowires offer a myriad of possibilities to engineer systems at the nanoscale, as well as to combine materials that cannot be put together in conventional heterostructures due to the lattice mismatch. In this work, we investigate GaAs/GaP superlattices embedded in GaP nanowires and demonstrate the tunability of their phononic and optoelectronic properties by inelastic light scattering experiments corroborated by ab initio calculations. We observe clear modifications in the dispersion relation for both acoustic and optical phonons in the superlattices nanowires. We find that by controlling the superlattice periodicity, we can achieve tunability of the phonon frequencies. We also performed wavelength-dependent Raman microscopy on GaAs/GaP superlattice nanowires, and our results indicate a reduction in the electronic bandgap in the superlattice compared to the bulk counterpart. All of our experimental results are rationalized with the help of ab initio density functional perturbation theory (DFPT) calculations. This work sheds fresh insights into how material engineering at the nanoscale can tailor phonon dispersion and open pathways for thermal engineering.

Understanding the Morphological Evolution of InSb Nanoflags Synthesized in Regular Arrays by Chemical Beam Epitaxy.

InSb nanoflags are grown by chemical beam epitaxy in regular arrays on top of Au-catalyzed InP nanowires synthesized on patterned SiO2/InP(111)B substrates. Two-dimensional geometry of the nanoflags is achieved by stopping the substrate rotation in the step of the InSb growth. Evolution of the nanoflag length, thickness and width with the growth time is studied for different pitches (distances in one of the two directions of the substrate plane). A model is presented which explains the observed non-linear time dependence of the nanoflag length, saturation of their thickness and gradual increase in the width by the shadowing effect for re-emitted Sb flux. These results might be useful for morphological control of InSb and other III-V nanoflags grown in regular arrays.

Selective-Area Epitaxy of InGaAsP Buffer Multilayer for In-Plane InAs Nanowire Integration.

In order to use III-V compound semiconductors as active channel materials in advanced electronic and quantum devices, it is important to achieve a good epitaxial growth on silicon substrates. As a first step toward this, we report on the selective-area growth of GaP/InGaP/InP/InAsP buffer layer nanotemplates on GaP substrates which are closely lattice-matched to silicon, suitable for the integration of in-plane InAs nanowires. Scanning electron microscopy reveals a perfect surface selectivity and uniform layer growth inside 150 and 200 nm large SiO2 mask openings. Compositional and structural characterization of the optimized structure performed by transmission electron microscopy shows the evolution of the major facet planes and allows a strain distribution analysis. Chemically uniform layers with well-defined heterointerfaces are obtained, and the topmost InAs layer is free from any dislocation. Our study demonstrates that a growth sequence of thin layers with progressively increasing lattice parameters is effective to efficiently relax the strain and eventually obtain high quality in-plane InAs nanowires on large lattice-mismatched substrates.