Postgrowth Shaping and Transport Anisotropy in Two-Dimensional InAs Nanofins.

We report on the postgrowth shaping of free-standing two-dimensional (2D) InAs nanofins that are grown by selective-area epitaxy and mechanically transferred to a separate substrate for device fabrication. We use a citric acid-based wet etch that enables complex shapes, for example, van der Pauw cloverleaf structures, with patterning resolution down to 150 nm as well as partial thinning of the nanofin to improve local gate response. We exploit the high sensitivity of the cloverleaf structures to transport anisotropy to address the fundamental question of whether there is a measurable transport anisotropy arising from wurtzite/zincblende polytypism in 2D InAs nanostructures. We demonstrate a mobility anisotropy of order 2-4 at room temperature arising from polytypic stacking faults in our nanofins. Our work highlights a key materials consideration for devices featuring self-assembled 2D III-V nanostructures using advanced epitaxy methods.

Impact of invasive metal probes on Hall measurements in semiconductor nanostructures.

Recent advances in bottom-up growth are giving rise to a range of new two-dimensional nanostructures. Hall effect measurements play an important role in their electrical characterization. However, size constraints can lead to device geometries that deviate significantly from the ideal of elongated Hall bars with currentless contacts. Many devices using these new materials have a low aspect ratio and feature metal Hall probes that overlap with the semiconductor channel. This can lead to a significant distortion of the current flow. We present experimental data from InAs 2D nanofin devices with different Hall probe geometries to study the influence of Hall probe length and width. We use finite-element simulations to further understand the implications of these aspects and expand their scope to contact resistance and sample aspect ratio. Our key finding is that invasive probes lead to significant underestimation of measured Hall voltage, typically of the order 40-80%. This in turn leads to a subsequent proportional overestimation of carrier concentration and an underestimation of mobility.

In situ passivation of GaAsSb nanowires for enhanced infrared photoresponse.

Surface passivation of semiconductor nanowires (NWs) is important for their optoelectronic properties and applications. Here, the in situ passivation effect of an epitaxial InP shell and the corresponding photodetector performance is experimentally studied. Compared with the unpassivated GaAs1- x Sb x core-only NWs, the GaAs1- x Sb x /InP core/shell NWs have shown much stronger photoluminescence and cathodoluminescence intensities. Correspondingly, the fabricated single GaAs1- x Sb x /InP core/shell NW photodetector shows a responsivity of 325.1 A W-1 (@ 1.3 µm and 1.5 V) that is significantly enhanced compared to that of single GaAs1- x Sb x core-only NW photodetectors (143.5 A W-1), with a comparable detectivity of 4.7 × 1010 and 5.3 × 1010 cm√Hz/W, respectively. This is ascribed to the enhanced carrier mobility and carrier concentration by the in situ passivation, which lead to both higher photoconductivity and dark-conductivity. Our results show that in situ passivation is an effective approach for performance enhancement of GaAs1-x Sb x NW based optoelectronic devices.

Ballistic InSb Nanowires and Networks via Metal-Sown Selective Area Growth.

Selective area growth is a promising technique to realize semiconductor-superconductor hybrid nanowire networks, potentially hosting topologically protected Majorana-based qubits. In some cases, however, such as the molecular beam epitaxy of InSb on InP or GaAs substrates, nucleation and selective growth conditions do not necessarily overlap. To overcome this challenge, we propose a metal-sown selective area growth (MS SAG) technique, which allows decoupling selective deposition and nucleation growth conditions by temporarily isolating these stages. It consists of three steps: (i) selective deposition of In droplets only inside the mask openings at relatively high temperatures favoring selectivity, (ii) nucleation of InSb under Sb flux from In droplets, which act as a reservoir of group III adatoms, done at relatively low temperatures, favoring nucleation of InSb, and (iii) homoepitaxy of InSb on top of the formed nucleation layer under a simultaneous supply of In and Sb fluxes at conditions favoring selectivity and high crystal quality. We demonstrate that complex InSb nanowire networks of high crystal and electrical quality can be achieved this way. We extract mobility values of 10 000-25 000 cm2 V-1 s-1 consistently from field-effect and Hall mobility measurements across single nanowire segments as well as wires with junctions. Moreover, we demonstrate ballistic transport in a 440 nm long channel in a single nanowire under a magnetic field below 1 T. We also extract a phase-coherent length of ∼8 µm at 50 mK in mesoscopic rings.

Shape Engineering of InP Nanostructures by Selective Area Epitaxy.

Greater demand for III-V nanostructures with more sophisticated geometries other than nanowires is expected because of the recent intensive investigation of nanowire networks that show great potential in all-optical logic gates, nanoelectronics, and quantum computing. Here, we demonstrate highly uniform arrays of InP nanostructures with tunable shapes, such as membrane-, prism-, and ring-like shapes, which can be simultaneously grown by selective area epitaxy. Our in-depth investigation of shape evolution confirms that the shape is essentially determined by pattern confinement and the minimization of total surface energy. After growth optimization, all of the different InP nanostructures grown under the same growth conditions show perfect wurtzite structure regardless of the geometry and strong and homogeneous photon emission. This work expands the research field in terms of producing nanostructures with the desired shapes beyond the limits of nanowires to satisfy various requirements for nanoelectronics, optoelectronics, and quantum device applications.

The Role of Polarity in Nonplanar Semiconductor Nanostructures.

The lack of mirror symmetry in binary semiconductor compounds turns them into polar materials, where two opposite orientations of the same crystallographic direction are possible. Interestingly, their physical properties (e.g., electronic or photonic) and morphological features (e.g., shape, growth direction, and so forth) also strongly depend on the polarity. It has been observed that nanoscale materials tend to grow with a specific polarity, which can eventually be reversed for very specific growth conditions. In addition, polar-directed growth affects the defect density and topology and might induce eventually the formation of undesirable polarity inversion domains in the nanostructure, which in turn will affect the photonic and electronic final device performance. Here, we present a review on the polarity-driven growth mechanism at the nanoscale, combining our latest investigation with an overview of the available literature highlighting suitable future possibilities of polarity engineering of semiconductor nanostructures. The present study has been extended over a wide range of semiconductor compounds, covering the most commonly synthesized III-V (GaN, GaP, GaAs, GaSb, InN, InP, InAs, InSb) and II-VI (ZnO, ZnTe, CdS, CdSe, CdTe) nanowires and other free-standing nanostructures (tripods, tetrapods, belts, and membranes). This systematic study allowed us to explore the parameters that may induce polarity-dependent and polarity-driven growth mechanisms, as well as the polarity-related consequences on the physical properties of the nanostructures.

Vapor Phase Growth of Semiconductor Nanowires: Key Developments and Open Questions.

Nanowires are filamentary crystals with a tailored diameter that can be obtained using a plethora of different synthesis techniques. In this review, we focus on the vapor phase, highlighting the most influential achievements along with a historical perspective. Starting with the discovery of VLS, we feature the variety of structures and materials that can be synthesized in the nanowire form. We then move on to establish distinct features such as the three-dimensional heterostructure/doping design and polytypism. We summarize the status quo of the growth mechanisms, recently confirmed by in situ electron microscopy experiments and defining common ground between the different synthesis techniques. We then propose a selection of remaining defects, starting from what we know and going toward what is still to be learned. We believe this review will serve as a reference for neophytes but also as an insight for experts in an effort to bring open questions under a new light.

Importance of point defect reactions for the atomic-scale roughness of III-V nanowire sidewalls.

The surface morphology of III-V semiconductor nanowires (NWs) protected by an arsenic cap and subsequently evaporated in ultrahigh vacuum is investigated with scanning tunneling microscopy and scanning transmission electron microscopy. We show that the changes of the surface morphology as a function of the NW composition and the nature of the seed particles are intimately related to the formation and reaction of surface point defects. Langmuir evaporation close to the congruent evaporation temperature causes the formation of vacancies which nucleate and form vacancy islands on {110} sidewalls of self-catalyzed InAs NWs. However, for annealing temperatures much smaller than the congruent temperature, a new phenomenon occurs: group III vacancies form and are filled by excess As atoms, leading to surface AsGa antisites. The resulting Ga adatoms nucleate with excess As atoms at the NW edges, producing monoatomic-step islands on the {110} sidewalls of GaAs NWs. Finally, when gold atoms diffuse from the seed particle onto the {110} sidewalls during evaporation of the protective As cap, Langmuir evaporation does not take place, leaving the sidewalls of InAsSb NWs atomically flat.

Selectivity Map for Molecular Beam Epitaxy of Advanced III-V Quantum Nanowire Networks.

Selective-area growth is a promising technique for enabling of the fabrication of the scalable III-V nanowire networks required to test proposals for Majorana-based quantum computing devices. However, the contours of the growth parameter window resulting in selective growth remain undefined. Herein, we present a set of experimental techniques that unambiguously establish the parameter space window resulting in selective III-V nanowire networks growth by molecular beam epitaxy. Selectivity maps are constructed for both GaAs and InAs compounds based on in situ characterization of growth kinetics on GaAs(001) substrates, where the difference in group III adatom desorption rates between the III-V surface and the amorphous mask area is identified as the primary mechanism governing selectivity. The broad applicability of this method is demonstrated by the successful realization of high-quality InAs and GaAs nanowire networks on GaAs, InP, and InAs substrates of both (001) and (111)B orientations as well as homoepitaxial InSb nanowire networks. Finally, phase coherence in Aharonov-Bohm ring experiments validates the potential of these crystals for nanoelectronics and quantum transport applications. This work should enable faster and better nanoscale crystal engineering over a range of compound semiconductors for improved device performance.

Engineering the Side Facets of Vertical [100] Oriented InP Nanowires for Novel Radial Heterostructures.

In addition to being grown on industry-standard orientation, vertical [100] oriented nanowires present novel families of facets and related cross-sectional shapes. These nanowires are engineered to achieve a number of facet combinations and cross-sectional shapes, by varying their growth parameters within ranges that facilitate vertical growth. In situ post-growth annealing technique is used to realise other combinations that are unattainable solely using growth parameters. Two examples of possible novel radial heterostructures grown on these vertical [100] oriented nanowire facets are presented, demonstrating their potential in future applications.

Radial Growth Evolution of InGaAs/InP Multi-Quantum-Well Nanowires Grown by Selective-Area Metal Organic Vapor-Phase Epitaxy.

III-V semiconductor multi-quantum-well nanowires (MQW NWs) via selective-area epitaxy (SAE) is of great importance for the development of nanoscale light-emitting devices for applications such as optical communication, silicon photonics, and quantum computing. To achieve highly efficient light-emitting devices, not only the high-quality materials but also a deep understanding of their growth mechanisms and material properties (structural, optical, and electrical) are extremely critical. In particular, the three-dimensional growth mechanism of MQWs embedded in a NW structure by SAE is expected to be different from that of those grown in a planar structure or with a catalyst and has not yet been thoroughly investigated. In this work, we reveal a distinctive radial growth evolution of InGaAs/InP MQW NWs grown by the SAE metal organic vapor-phase epitaxy (MOVPE) technique. We observe the formation of zinc blende (ZB) QW discs induced by the axial InGaAs QW growth on the wurtzite (WZ) base-InP NW and propose it as the key factor driving the overall structure of radial growth. The role of the ZB-to-WZ change in the driving of the overall growth evolution is supported by a growth formalism, taking into account the formation-energy difference between different facets. Despite a polytypic crystal structure with mixed ZB and WZ phases across the MQW region, the NWs exhibit high uniformity and desirable QW spatial layout with bright room-temperature photoluminescence at an optical communication wavelength of ∼1.3 µm, which is promising for the future development of high-efficiency light-emitting devices.

Simultaneous Selective-Area and Vapor-Liquid-Solid Growth of InP Nanowire Arrays.

Selective-area epitaxy is highly successful in producing application-ready size-homogeneous arrays of III-V nanowires without the need to use metal catalysts. Previous works have demonstrated excellent control of nanowire properties but the growth mechanisms remain rather unclear. Herein, we report a detailed growth study revealing that fundamental growth mechanisms of pure wurtzite InP ⟨111⟩A nanowires can indeed differ significantly from the simple picture of a facet-limited selective-area growth process. A dual growth regime with and without metallic droplet is found to coexist under the same growth conditions for different diameter nanowires. Incubation times and highly nonmonotonous growth rate behaviors are revealed and explained within a dedicated kinetic model.

Doping-enhanced radiative efficiency enables lasing in unpassivated GaAs nanowires.

Nanolasers hold promise for applications including integrated photonics, on-chip optical interconnects and optical sensing. Key to the realization of current cavity designs is the use of nanomaterials combining high gain with high radiative efficiency. Until now, efforts to enhance the performance of semiconductor nanomaterials have focused on reducing the rate of non-radiative recombination through improvements to material quality and complex passivation schemes. Here we employ controlled impurity doping to increase the rate of radiative recombination. This unique approach enables us to improve the radiative efficiency of unpassivated GaAs nanowires by a factor of several hundred times while also increasing differential gain and reducing the transparency carrier density. In this way, we demonstrate lasing from a nanomaterial that combines high radiative efficiency with a picosecond carrier lifetime ready for high speed applications.

Twin-Induced InSb Nanosails: A Convenient High Mobility Quantum System.

Ultra narrow bandgap III-V semiconductor nanomaterials provide a unique platform for realizing advanced nanoelectronics, thermoelectrics, infrared photodetection, and quantum transport physics. In this work we employ molecular beam epitaxy to synthesize novel nanosheet-like InSb nanostructures exhibiting superior electronic performance. Through careful morphological and crystallographic characterization we show how this unique geometry is the result of a single twinning event in an otherwise pure zinc blende structure. Four-terminal electrical measurements performed in both the Hall and van der Pauw configurations reveal a room temperature electron mobility greater than 12,000 cm(2)·V(-1)·s(-1). Quantized conductance in a quantum point contact processed with a split-gate configuration is also demonstrated. We thus introduce InSb "nanosails" as a versatile and convenient platform for realizing new device and physics experiments with a strong interplay between electronic and spin degrees of freedom.

Room temperature GaAsSb single nanowire infrared photodetectors.

Antimonide-based ternary III-V nanowires (NWs) allow for a tunable bandgap over a wide range, which is highly interesting for optoelectronics applications, and in particular for infrared photodetection. Here we demonstrate room temperature operation of GaAs0.56Sb0.44 NW infrared photodetectors grown by metal organic vapor phase epitaxy. These GaAs0.56Sb0.44 NWs have uniform axial composition and show p-type conductivity with a peak field-effect mobility of ∼12 cm(2) V(-1) s(-1)). Under light illumination, single GaAs0.56Sb0.44 NW photodetectors exhibited typical photoconductor behavior with an increased photocurrent observed with the increase of temperature owing to thermal activation of carrier trap states. A broadband infrared photoresponse with a long wavelength cutoff at ∼1.66 µm was obtained at room temperature. At a low operating bias voltage of 0.15 V a responsivity of 2.37 (1.44) A/W with corresponding detectivity of 1.08 × 10(9) (6.55 × 10(8)) cm√Hz/W were achieved at the wavelength of 1.3 (1.55) µm, indicating that ternary GaAs0.56Sb0.44 NWs are promising photodetector candidates for small footprint integrated optical telecommunication systems.

Tunable Polarity in a III-V Nanowire by Droplet Wetting and Surface Energy Engineering.

Controllable axial switching of polarity in GaAs nanowires with minimal tapering and perfect twin-free ZB structure based on the fundamental understanding of nanowire growth and kinking mechanism is presented. The polarity of the bottom segment is confirmed to be (111)A by atomically resolved scanning transmission electron microscopy.

Formation of long single quantum dots in high quality InSb nanowires grown by molecular beam epitaxy.

We report on realization and transport spectroscopy study of single quantum dots (QDs) made from InSb nanowires grown by molecular beam epitaxy (MBE). The nanowires employed are 50-80 nm in diameter and the QDs are defined in the nanowires between the source and drain contacts on a Si/SiO2 substrate. We show that highly tunable QD devices can be realized with the MBE-grown InSb nanowires and the gate-to-dot capacitance extracted in the many-electron regimes is scaled linearly with the longitudinal dot size, demonstrating that the devices are of single InSb nanowire QDs even with a longitudinal size of ∼700 nm. In the few-electron regime, the quantum levels in the QDs are resolved and the Landég-factors extracted for the quantum levels from the magnetotransport measurements are found to be strongly level-dependent and fluctuated in a range of 18-48. A spin-orbit coupling strength is extracted from the magnetic field evolutions of a ground state and its neighboring excited state in an InSb nanowire QD and is on the order of ∼300 µeV. Our results establish that the MBE-grown InSb nanowires are of high crystal quality and are promising for the use in constructing novel quantum devices, such as entangled spin qubits, one-dimensional Wigner crystals and topological quantum computing devices.

In(x)Ga(1-x)As nanowires with uniform composition, pure wurtzite crystal phase and taper-free morphology.

Obtaining compositional homogeneity without compromising morphological or structural quality is one of the biggest challenges in growing ternary alloy compound semiconductor nanowires. Here we report growth of Au-seeded InxGa1-xAs nanowires via metal-organic vapour phase epitaxy with uniform composition, morphology and pure wurtzite (WZ) crystal phase by carefully optimizing growth temperature and V/III ratio. We find that high growth temperatures allow the InxGa1-xAs composition to be more uniform by suppressing the formation of typically observed spontaneous In-rich shells. A low V/III ratio results in the growth of pure WZ phase InxGa1-xAs nanowires with uniform composition and morphology while a high V/III ratio allows pure zinc-blende (ZB) phase to form. Ga incorporation is found to be dependent on the crystal phase favouring higher Ga concentration in ZB phase compared to the WZ phase. Tapering is also found to be more prominent in defective nanowires hence it is critical to maintain the highest crystal structure purity in order to minimize tapering and inhomogeneity. The InP capped pure WZ In0.65Ga0.35As core-shell nanowire heterostructures show 1.54 µm photoluminescence, close to the technologically important optical fibre telecommunication wavelength, which is promising for application in photodetectors and nanoscale lasers.

Controlling the morphology, composition and crystal structure in gold-seeded GaAs(1-x)Sb(x) nanowires.

While III-V binary nanowires are now well controlled and their growth mechanisms reasonably well understood, growing ternary nanowires, including controlling their morphology, composition and crystal structure remains a challenge. However, understanding and control of ternary alloys is of fundamental interest and critical to enable a new class of nanowire devices. Here, we report on the progress in understanding the complex growth behaviour of gold-seeded GaAs1-xSbx nanowires grown by metalorganic vapour phase epitaxy. The competition between As and Sb atoms for incorporation into the growing crystal leads to a tunability of the Sb content over a broad range (x varies from 0.09 to 0.6), solely by changing the AsH3 flow. In contrast, changing TMSb flow is more effective in affecting the morphology and crystal structure of the nanowires. Inclined faults are found in some of these nanowires and directly related to the kinking of the nanowires and controlled by TMSb flow. Combined with the observed sharp increase of wetting angle between the Au seed and nanowire, the formation of inclined faults are attributed to the Au seed being dislodged from the growth front to wet the sidewalls of the nanowires, and are related to the surfactant role of Sb. The insights provided by this study should benefit future device applications relying on taper- and twin-free ternary antimonide III-V nanowire alloys and their heterostructures.