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We present the first experimental study into how Au-seeded GaAs nanowire diameter affects the Ga-dependent incubation and As-dependent step-flow processes revealing a dramatic increase of step-flow process time for smaller diameter nanowires.

With the increased demand for controlled deterministic growth of III–V semiconductors at the nanoscale, the impact and interest of understanding defect formation and crystal structure switching becomes increasingly important. Vapor–liquid–solid (VLS) growth of semiconductor nanocrystals is an important mechanism for controlling and studying the formation of individual crystal layers and stacking defects. Using in situ studies, combining atomic resolution of transmission electron microscopy and controlled VLS crystal growth using metal organic chemical vapor deposition, we investigate the simplest achievable change in atomic layer stacking–single twinned layers formed in GaAs. Using Au-assisted GaAs nanowires of various diameters, we study the formation of individual layers with atomic resolution to reveal the growth difference in forming a twin defect. We determine that the formation of a twinned layer occurs significantly more slowly than that of a normal crystal layer. To understand this, we conduct thermodynamic modeling and determine that the propagation of a twin is limited by the energy cost of forming the twin interface. Finally, we determine that the slower propagation of twinned layers increases the probability of additional layers nucleating, such that multiple layers grow simultaneously. This observation challenges the current understanding that continuous uniform epitaxial growth, especially in the case of liquid-metal assisted nanowires, proceeds one single layer at a time and that its progression is limited by the nucleation rate.

The nanowire geometry is favorable for the growth of ternary semiconductor materials, because the composition and properties can be tuned freely without substrate lattice matching. To achieve precise control of the composition in ternary semiconductor nanowires, a deeper understanding of the growth is required. One unknown aspect of seeded nanowire growth is how the composition of the catalyst nanoparticle affects the resulting composition of the growing nanowire. We report the first in situ measurements of the nanoparticle and InxGa1-xAs nanowire compositional relationship using an environmental transmission electron microscopy setup. The compositions were measured and correlated during growth, via X-ray energy dispersive spectroscopy. Contrary to predictions from thermodynamic models, the experimental results do not show a miscibility gap. Therefore, we construct a kinetic model that better predicts the compositional trends by suppressing the miscibility gap. The findings imply that compositional control of InxGa1-xAs nanowires is possible across the entire compositional range.

We explore the energetics of microwaves interacting with a double quantum dot photodiode and show wave-particle aspects in photon-assisted tunneling. The experiments show that the single photon energy sets the relevant absorption energy in a weak-drive limit, which contrasts the strong drive limit where the wave amplitude determines the relevant-energy scale and opens up microwave induced bias triangles. The threshold condition between these two regimes is set by the fine-structure constant of the system. The energetics are determined here with the detuning conditions of the double dot system and stopping-potential measurements that constitute a microwave version of the photoelectric effect., 5 pages 4 figures

The world of environmental microscopy provides the possibility to study and analyze transformations and reactions during realistic conditions to understand the processes better. We report on the design and development of a metal-organic chemical vapor deposition (MOCVD) system integrated with an environmental transmission electron microscope intended for real-time investigations of crystal growth. We demonstrate methods for achieving a wide range of precisely controlled concentrations of precursor gas at the sample, as well as for calibrating the sample partial pressure using the pressure measured elsewhere in the microscope column. The influences of elevated temperature and reactive gas within the pole-piece gap are evaluated with respect to imaging and spectroscopy. We show that X-ray energy-dispersive spectroscopy can be strongly affected by temperatures beyond 500$^{\circ }$C, while the spatial resolution is largely unaffected by heat and microscope pressure for the relevant conditions. Finally, the influence of the electron beam on the investigated processes is discussed. With this work, we aim to provide crucial input in the development of advanced in situ electron microscopy systems for studies of complex reactions in real time under realistic conditions, for instance as used during formation of semiconductor crystals.

Hot electron relaxation and transport in nanostructures involve a multitude of ultrafast processes whose interplay and relative importance are still not fully understood, but which are relevant for future applications in areas such as photocatalysis and optoelectronics. To unravel these processes, their dynamics in both time and space must be studied with high spatiotemporal resolution in structurally well-defined nanoscale objects. We employ time-resolved photoemission electron microscopy to image the relaxation of photogenerated hot electrons within InAs nanowires on a femtosecond time scale. We observe transport of hot electrons to the nanowire surface within 100 fs caused by surface band bending. We find that electron-hole scattering substantially influences hot electron cooling during the first few picoseconds, while phonon scattering is prominent at longer time scales. The time scale of cooling is found to differ between the well-defined wurtzite and zincblende crystal segments of the nanowires depending on excitation light polarization. The scattering and transport mechanisms identified will play a role in the rational design of nanostructures for hot-electron-based applications.

Semiconductor nanowires are promising material systems for coming-of-age nanotechnology. The usage of the vapor–solid–solid (VSS) route, where the catalyst used for promoting axial growth of nanowires is a solid, offers certain advantages compared to the common vapor–liquid–solid (VLS) route (using a liquid catalyst). The VSS growth of group-IV elemental nanowires has been investigated by other groups in situ during growth in a transmission electron microscope (TEM). Though it is known that compound nanowire growth has different dynamics compared to elemental semiconductors, the layer growth dynamics of VSS growth of compound nanowires have not been studied yet. Here we investigate for the first time controlled VSS growth of compound nanowires by in situ microscopy, using Au-seeded GaAs as a model system. The ledge-flow growth kinetics and dynamics at the wire–catalyst interface are studied and compared for liquid and solid catalysts under similar growth conditions. Here the temperature and thermal history of the system are manipulated to control the catalyst phase. In the first experiment discussed here we reduce the growth temperature in steps to solidify the initially liquid catalyst, and compare the dynamics between VLS and VSS growth observed at slightly different temperatures. In the second experiment we exploit thermal hysteresis of the system to obtain both VLS and VSS at the same temperature. The VSS growth rate is comparable or slightly slower than the VLS growth rate. Unlike in the VLS case, during VSS growth we frequently observe that a new layer starts before the previous layer is completely grown, i.e., ‘multilayer growth’. Understanding the VSS growth mode enables better control of nanowire properties by widening the range of usable nanowire growth parameters.

The radius of III-V nanowires is known to have an effect on the resulting crystal structure during particle-assisted growth; however, the causes behind this effect remain under debate. In this work, we use stochastic simulations of nanowire growth to evaluate how the radius (R) affects the growth dynamics and how this in turn affects the crystal structure selection. This is due to the geometry of the growing nanowire: The number of atoms in the seed particle scales with R3, and the number of III-V pairs per layer scales with R2. The influx of growth species to the seed can, for instance, scale with the surface area of the seed particle for direct impingement (?R2) or the perimeter of the nanowire for sidewall diffusion (?R1) or be radius-independent for substrate diffusion in some cases (?R0). These differences in radius dependencies cause the particle composition to change more rapidly for thinner nanowires, which in turn leads to nucleation at higher supersaturations and promotion of the wurtzite structure. In addition, the geometry can also make the influx V/III ratio dependent on the nanowire radius, which can influence the selection of crystal structure in different ways depending on the materials system and growth regime. (Less)

Crystal growth of semiconductor nanowires from a liquid droplet depends on the stability of this droplet's liquid-solid interface. Because of the assisting property of the droplet, growth will be hindered if the droplet is displaced onto the nanowire sidewalls. Using real-time observation of such growth by in situ transmission electron microscopy combined with theoretical analysis of the surface energies involved, we observe a reoccurring truncation at the edge of the droplet-nanowire interface. We demonstrate that creating a truncation widens the parameter range for having a droplet on the top facet, which allows continued nanowire growth. Combining experiment and theory provides an explanation for the previously reported truncation phenomenon of the growth interface based only on droplet wetting dynamics. In addition to determining the fundamental limits of droplet-assisted nanowire growth, this allows experimental estimation of the surface tension and the surface energies of the nanowire such as the otherwise metastable wurtzite GaAs {101̅0} facet.

In this work we demonstrate a two-fold selectivity control of InAs shells grown on crystal phase and morphology engineered GaAs nanowire (NW) core templates. This selectivity occurs driven by differences in surface energies of the NW core facets. The occurrence of the different facets itself is controlled by either forming different crystal phases or additional tuning of the core NW morphology. First, in order to study the crystal phase selectivity, GaAs NW cores with an engineered crystal phase in the axial direction were employed. A crystal phase selective growth of InAs on GaAs was found for high growth rates and short growth times. Secondly, the facet-dependant selectivity of InAs growth was studied on crystal phase controlled GaAs cores which were additionally morphology-tuned by homoepitaxial overgrowth. Following this route, the original hexagonal cores with {110} sidewalls were converted into triangular truncated NWs with ridges and predominantly {112}

Scaling down material synthesis to crystalline structures only few atoms in size and precisely positioned in device configurations remains highly challenging, but is crucial for new applications e.g., in quantum computing. We propose to use the sidewall facets of larger III–V semiconductor nanowires (NWs), with controllable axial stacking of different crystal phases, as templates for site-selective growth of ordered few atoms 1D and 2D structures. We demonstrate this concept of self-selective growth by Bi deposition and incorporation into the surfaces of GaAs NWs to form GaBi structures. Using low temperature scanning tunneling microscopy (STM), we observe the crystal structure dependent self-selective growth process, where ordered 1D GaBi atomic chains and 2D islands are alloyed into surfaces of the wurtzite (Wz) \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\{11{\bar{2}}0\}$$\end{document}{112¯0} crystal facets. The formation and lateral extension of these surface structures are controlled by the crystal structure and surface morphology uniquely found in NWs. This allows versatile high precision design of structures with predicted novel topological nature, by using the ability of NW heterostructure variations over orders of magnitude in dimensions with atomic-scale precision as well as controllably positioning in larger device structures., Site-selected crystal material synthesis at the atomic scale has been a long-standing challenge. Here the authors use nanowire crystal phase heterostructures as templates for self-selective growth of one- and two-dimensional GaBi nanostructures, which allows versatile design with atomic-scale precision.

We study using in situ transmission electron microscopy the birth of GaAs nanowires from liquid Au–Ga catalysts on amorphous substrates. Lattice-resolved observations of the starting stages of growth are reported here for the first time. It reveals how the initial nanostructure evolves into a nanowire growing in a zincblende 〈111〉 or the equivalent wurtzite〈0001〉 direction. This growth direction(s) is what is typically observed in most III–V and II–VI nanowires. However, the reason for this preferential nanowire growth along this direction is still a dilemma. Based on the videos recorded shortly after the nucleation of nanowires, we argue that the lower catalyst droplet-nanowire interface energy of the {111} facet when zincblende (or the equivalent {0001} facet in wurtzite) is the reason for this direction selectivity in nanowires.

Proposals for quantum information applications are frequently based on the coherent manipulation of spins confined to quantum dots. For these applications, $p$-type III-V material systems promise a reduction of the hyperfine interaction while maintaining large $g$ factors and strong spin-orbit interaction. In this Letter, we study bottom-gated device architectures to realize single and serial multiquantum dot systems in Schottky-contacted $p$-type GaSb nanowires. We find that the effect of potentials applied to gate electrodes on the nanowire is highly localized to the immediate vicinity of the gate electrode only, which prevents the formation of double quantum dots with commonly used device architectures. We further study the transport properties of a single quantum dot induced by bottom gating and find large gate-voltage dependent variations of the ${g}^{*}$ factors up to $8.1\ifmmode\pm\else\textpm\fi{}0.2$ as well as spin-orbit energies between 110 and 230 $\ensuremath{\mu}\mathrm{eV}$.

Particle-assisted III-V semiconductor nanowire growth and applications thereof have been studied extensively. However, the stability of nanowires in contact with the particle and the particle chemical composition as a function of temperature remain largely unknown. In this work, we use in situ transmission electron microscopy to investigate the interface between a Au-Ga particle and the top facet of an ?1 1 1 ?-oriented GaAs nanowire grown via the vapor-liquid-solid process. We observed a thermally activated bilayer-by-bilayer removal of the GaAs facet in contact with the liquid particle during annealing between 300 and 420 °C in vacuum. Interestingly, the GaAs-removal rates initially depend on the thermal history of the sample and are time-invariant at later times. In situ X-ray energy dispersive spectroscopy was also used to determine that the Ga content in the particle at any given temperature remains constant over extended periods of time and increases with increasing temperature from 300 to 400 °C. We attribute the observed phenomena to droplet-assisted decomposition of GaAs at a rate that is controlled by the amount of Ga in the droplet. We suggest that the observed transients in removal rates are a direct consequence of time-dependent changes in the Ga content. Our results provide new insights into the role of droplet composition on the thermal stability of GaAs nanowires and complement the existing knowledge on the factors influencing nanowire growth. Moreover, understanding the nanowire stability and decomposition is important for improving processing protocols for the successful fabrication and sustained operation of nanowire-based devices. (Less)

Growing GaAs nanowires with well-defined crystal structures is a challenging task, but may be required for the fabrication of future devices. In terms of crystal phase selection, the connection between theory and experiment is limited, leaving experimentalists with a trial and error approach to achieve the desired crystal structures. In this work, we present a modeling approach designed to provide the missing connection, combining classical nucleation theory, stochastic simulation, and mass transport through the seed particle. The main input parameters for the model are the flows of the growth species and the temperature of the process, giving the simulations the same flexibility as experimental growth. The output of the model can also be directly compared to experimental observables, such as crystal structure of each bilayer throughout the length of the nanowire and the composition of the seed particle. The model thus enables for observed experimental trends to be directly explored theoretically. Here, we use the model to simulate nanowire growth with varying As flows, and our results match experimental trends with a good agreement. By analyzing the data from our simulation, we find theoretical explanations for these experimental results, providing new insights into how the crystal structure is affected by the experimental parameters available for growth.

Tunneling Field-Effect Transistors (TFET) are one of the most promising candidates for future low-power CMOS applications including mobile and Internet of Things (IoT) products. A vertical gate-all-around (VGAA) architecture with a core shell (C-S) structure is the leading contender to meet CMOS footprint requirements while simultaneously delivering high current drive for high performance specifications and subthreshold swing below the Boltzmann limit for low power operation. In this work, VGAA nanowire GaSb/InAs C-S TFETs are demonstrated experimentally for the first time with key device properties of subthreshold swing S = 40 mV/dec (Vd = 10 mV) and current drive up to 40 μA/wire (Vd = 0.3 V, diameter d = 50 nm) while dimensions including core diameter d, shell thickness and gate length are scaled towards CMOS requirements. The experimental data in conjunction with TCAD modeling reveal interface trap density requirements to reach industry standard off-current specifications.

The electronic band structure of complex nanostructured semiconductors has a considerable effect on the final electronic and optical properties of the material and, ultimately, on the functionality of the devices incorporating them. Valence electron energy-loss spectroscopy (VEELS) in the transmission electron microscope (TEM) provides the possibility of measuring this property of semiconductors with high spatial resolution. However, it still represents a challenge for narrow-bandgap semiconductors, since an electron beam with low energy spread is required. Here we demonstrate that by means of monochromated VEELS we can study the electronic band structure of narrow-gap materials GaSb and InAs in the form of heterostructured nanowires, with bandgap values down to 0.5 eV, especially important for newly developed structures with unknown bandgaps. Using complex heterostructured InAs-GaSb nanowires, we determine a bandgap value of 0.54 eV for wurtzite InAs. Moreover, we directly compare the bandgaps of wurtzite and zinc blende polytypes of GaSb in a single nanostructure, measured here as 0.84 and 0.75 eV, respectively. This allows us to solve an existing controversy in the band alignment between these structures arising from theoretical predictions. The findings demonstrate the potential of monochromated VEELS to provide a better understanding of the band alignment at the heterointerfaces of narrow-bandgap complex nanostructured materials with high spatial resolution. This is especially important for semiconductor device applications where even the slightest variations of the electronic band structure at the nanoscale can play a crucial role in their functionality.

We engineer a system of two strongly confined quantum dots to gain reproducible electrostatic control of the even-electron spin at zero magnetic field. Coupling the dots in a tight ring-shaped potential with two tunnel barriers, we demonstrate that an electric field can switch the electron ground state between a singlet and a triplet configuration. Comparing our experimental cotunneling spectroscopy data to a full many-body treatment of interacting electrons in a double-barrier quantum ring, we find excellent agreement in the evolution of many-body states with electric and magnetic fields. The calculations show that the singlet-triplet energy crossover, not found in conventionally coupled quantum dots, is made possible by the ring-shaped geometry of the confining potential.

The interface between wurtzite and zinc blende InP has been identified as type-II, where electrons gather on the zinc blende side and holes on the wurtzite side of the interface. The photoluminescence resulting from recombination across the interface is expected to be long-lived and to exhibit non-exponential decay of emission intensity after pulsed excitation. We verify this prediction using time-resolved photoluminescence spectroscopy on nanowires containing a single heterostructure between a single segment of wurtzite and zinc blende. We find that a significant intensity of type-II emission remains even more than 30 ns after excitation. The decay of the emission intensity is also non-exponential and considerably longer than the exponential decay of the wurtzite InP segment (260 ps). Our results are consistent with the expected photoluminescence characteristics of a type-II interface between the two polytypes. We also find that the lifetime becomes shorter if we create an electron gas at the interface by n-type doping the entire wurtzite segment of the nanowire. This is expected since there are many electrons that a given hole can recombine with, in contrast to the undoped case.

It is now possible to synthesize the wurtzite crystal phase of most III-V semiconductors in the form of nanowires. This sparks interest for fundamental research and adds extra degrees of freedom for designing novel devices. However, the understanding of many properties, such as phonon dispersion, of these wurtzite semiconductors is not yet complete, despite the extensive number of studies published. The

A new environmental transmission electron microscope has been installed in Lund in order to investigate the growth of III–V semiconductor nanowires by metal-organic chemical vapour deposition. We report here on the concepts behind the design of the facility and on details of the operation, and we refer to early results to highlight the new information that can be accessed from in situ studies. The installation includes a gas handling system that delivers the precursors to III–V semiconductor growth under controlled conditions. The core microscope is a Hitachi HF-3300S 300 kV transmission electron microscope with additional pumping that can handle up to 6 Pa of gas injected into the specimen area, or up to 400 Pa if an apertured lid is fitted to the holder. Various custom specimen holders incorporate precursor gas lines, a heating chip or a double tilt mechanism. The polepiece gap has been expanded to accommodate the holders, while the combination of an imaging aberration corrector and a cold field emission gun delivers a point resolution of 86 pm. Single images with atomic level detail are collected by one camera while another camera provides real-time video recording. A scanning unit offers high angle annular dark field and secondary electron images, and compositional microanalysis is performed with energy dispersive spectroscopy. In summary, III–V nanowires have been grown successfully in situ across a range of controlled conditions such as substrate temperature and precursor partial pressures. Atomic resolution images and movies, and spectroscopy data taken during this growth allow detailed measurements of structures, compositions and growth rates—data that are otherwise hard or impossible to obtain from ex situ studies—and further our understanding of the mechanisms of crystal growth.

Subgap states in semiconducting-superconducting nanowire hybrid devices are controversially discussed as potential topologically nontrivial quantum states. One source of ambiguity is the lack of an energetically and spatially well defined tunnel spectrometer. Here, we use quantum dots directly integrated into the nanowire during the growth process to perform tunnel spectroscopy of discrete subgap states in a long nanowire segment. In addition to subgap states with a standard magnetic field dependence, we find topologically trivial subgap states that are independent of the external magnetic field, i.e., that are pinned to a constant energy as a function of field. We explain this effect qualitatively and quantitatively by taking into account the strong spin-orbit interaction in the nanowire, which can lead to a decoupling of Andreev bound states from the field due to a spatial spin texture of the confined eigenstates. This result constitutes an important step forward in the research on superconducting subgap states in nanowires, such as Majorana bound states.

The integration of III–V semiconductors with Si in device fabrication is facilitated by the use of nanoscale structures such as nanowires. Nanowires are predominantly grown using Au seed particles; however, the seed material is known to affect the nanowire growth and properties. Here we present growth of GaAs nanowires using three different seed particle materials: Au, Ag, and a AgAu alloy. By comparing the results from the different seeds, we found that the growths of Au- and AgAu-seeded nanowires were in general very similar, with homogeneous and vertical nanowires observed in both cases. The Ag-seeded growths instead revealed a lower yield of vertical nanowires with large variations in lengths. Different Ga-concentrations were measured in the different seed particles, which suggested that the Au and the AgAu seed particles were liquid during growth, whereas Ag particles were solid. The chemical potential of Ga was however found to be similar for all three seed materials. We propose that the Ga concentr...

We use co-tunneling spectroscopy to investigate spin-, orbital-, and spin-orbital Kondo transport in a strongly confined system of InAs double quantum dots (QDs) parallel-coupled to source and drain. In the one-electron transport regime, the higher symmetry spin-orbital Kondo effect manifests at orbital degeneracy and no external magnetic field. We then proceed to show that the individual Kondo contributions can be isolated and studied separately; either by orbital detuning in the case of spin-Kondo transport, or by spin splitting in the case of orbital Kondo transport. By varying the inter-dot tunnel coupling, we show that lifting of the spin degeneracy is key to confirming the presence of an orbital degeneracy, and to detecting a small orbital hybridization gap. Finally, in the two-electron regime, we show that the presence of a spin-triplet ground state results in spin-Kondo transport at zero magnetic field., 8 pages, 6 figures

It has recently become possible to grow GaAs in the wurtzite crystal phase. This ability allows interesting tests of band-structure theory. Wurtzite GaAs has two closely spaced direct conduction bands as well as three nondegenerate valence bands. The energies of the band edges are not well known, in particular not as a function of temperature. In order to improve the accuracy we have studied the temperature dependence of the conduction band minimum as well as of the second valence band maximum using resonant Raman scattering (of up to 3LO Raman lines). We find that the temperature dependence of the bandgap in wurtzite GaAs is very similar to that in zinc blende GaAs. Our results show that they have the same band gaps not only at 7 K but also at room temperature to within 5 meV. This is in some discrepancy with previous work. We find that the energy difference between the first two Γ9V and Γ7V valence bands is constant, around 100 meV, over the investigated temperature range, 7 K to 300 K. Due to a fortuitous spacing of the energy bands we find a very unexpected and strong quadruple resonance in the resonant Raman scattering.

There exists a demand for production of metal nanoparticles for today's emerging nanotechnology. Aerosol-generated metal nanoparticles can oxidize during particle formation due to impurities in the carrier gas. One method to produce unoxidized metal nanoparticles is to first generate metal oxides and then reduce them during sintering. Here, we propose to instead prevent oxidation by introducing the reducing agent already at particle formation. We show that by mixing 5% hydrogen into the nitrogen carrier gas, we can generate single crystalline metal nanoparticles by spark discharge from gold, cobalt, bismuth, and tin electrodes. The non-noble nanoparticles exhibit signs of surface oxidation likely formed post-deposition when exposed to air. Nanoparticles generated without hydrogen are found to be primarily polycrystalline and oxidized. To demonstrate the advantages of supplying the reducing agent at generation, we compare to nanoparticles that are generated in nitrogen and sintered in a hydrogen mixture. For bismuth and tin, the crystal quality of the particles after sintering is considerably higher when hydrogen is introduced at particle generation compared to at sintering, whereas for cobalt it is equally effective to only add hydrogen at sintering. We propose that hydrogen present at particle generation prevents the formation of oxide primary particles, thus improving the ability to sinter the nanoparticles to compact and single crystals of metal. This method is general and can be applied to other aerosol generation systems, to improve the generation of size-controlled nanoparticles of non-noble metals with a suitable reducing agent. (Less)

We use crystal-phase tuning during epitaxial growth of InAs nanowires to create quantum dots with very strong confinement. A set of gate electrodes are used to reproducibly split the quantum dots into even smaller pairs for which we can control the populations down to the last electron. The double quantum dots, which are parallel-coupled to source and drain, show clear and stable odd-even level pairing due to spin degeneracy and the strong confinement. The combination of hard-wall barriers to source and drain, shallow interdot tunnel barriers, and very high single-particle excitation energies allow an order of magnitude tuning of the strength for the first intramolecular bond. We show examples for nanowires with different facet orientations, and suggest possible mechanisms behind the reproducible double-dot formation.

Over the past decade, III-V heterostructure nanowires have attracted a surge of attention for their application in novel semiconductor devices such as tunneling field-effect transistors (TFETs). The functionality of such devices critically depends on the specific atomic arrangement at the semiconductor heterointerfaces. However, most of the currently available characterization techniques lack sufficient spatial resolution to provide local information on the atomic structure and composition of these interfaces. Atomic-resolution spectrum imaging by means of electron energy-loss spectroscopy (EELS) in the scanning transmission electron microscope (STEM) is a powerful technique with the potential to resolve structure and chemical composition with sub-angstrom spatial resolution and to provide localized information about the physical properties of the material at the atomic scale. Here, we demonstrate the use of atomic-resolution EELS to understand the interface atomic arrangement in three-dimensional heterostructures in semiconductor nanowires. We observed that the radial interfaces of GaSb-InAs heterostructure nanowires are atomically abrupt, while the axial interface in contrast consists of an interfacial region where intermixing of the two compounds occurs over an extended spatial region. The local atomic configuration affects the band alignment at the interface and, hence, the charge transport properties of devices such as GaSb-InAs nanowire TFETs. STEM-EELS thus represents a very promising technique for understanding nanowire physical properties, such as differing electrical behavior across the radial and axial heterointerfaces of GaSb-InAs nanowires for TFET applications.

As semiconductor electronics keep shrinking, functionality depends on individual atomic scale surface and interface features that may change as voltages are applied. In this work we demonstrate a novel device platform that allows scanning tunneling microscopy (STM) imaging with atomic scale resolution across a device simultaneously with full electrical operation. The platform presents a significant step forward as it allows STM to be performed everywhere on the device surface and high temperature processing in reactive gases of the complete device. We demonstrate the new method through proof of principle measurements on both InAs and GaAs nanowire devices with variable biases up to 4 V. On InAs nanowires we observe a surprising removal of atomic defects and smoothing of the surface morphology under applied bias, in contrast to the expected increase in defects and electromigration-related failure. As we use only standard fabrication and scanning instrumentation our concept is widely applicable and opens up the possibility of fundamental investigations of device surface reliability as well as new electronic functionality based on restructuring during operation.

Growth of III–V semiconductor nanowires is generally assisted by a liquid particle in order to get a highly anisotropic crystallization. The thermodynamic stability of the particle is therefore of importance for control and understanding of the nanowire growth process. In this report we explore the particle stability by manipulating its properties, specifically its surface tension and volume, by accumulating indium in the particle during nanowire growth. We demonstrate a droplet displacement, from the top to one of the nanowire side facets, when exceeding the stability limit for a gold particle wetting an [0001]-oriented InAs nanowire. This particle displacement is attributed to a lowered surface tension and a truncation of the top facet. In addition, our results indicate reversibility of the displacement, showing that the (111/0001) facet is the most favorable for a droplet to wet during common growth conditions. The stability condition for InAs growth is determined experimentally, and the understan...

Although zinc-blende (ZB) and wurtzite (WZ) structures differ only in the atomic stacking sequence, mixing of crystal phases can strongly affect the electronic properties, a problem particularly common to bottom up-grown nanostructures. A lack of understanding of the nature of electronic transport at crystal phase junctions thus severely limits our ability to develop functional nanowire devices. In this work we investigated electron transport in InAs nanowires with designed mixing of crystal structures, ZB/WZ/ZB, by temperature-dependent electrical measurements. The WZ inclusion gives rise to an energy barrier in the conduction band. Interpreting the experimental result in terms of thermionic emission and using a drift-diffusion model, we extracted values for the WZ/ZB band offset, 135 ± 10 meV, and interface sheet polarization charge density on the order of 10–3 C/m2. The extracted polarization charge density is 1–2 orders of magnitude smaller than previous experimental results, but in good agreement wit...

We here investigate the growth mechanism of Sn-seeded GaSb nanowires and demonstrate how the seed particle and its dynamics at the growth interface of the nanowire determine the polarity, as well as the formation of structural defects. We use aberration-corrected scanning transmission electron microscopy imaging methodologies to study the interrelationship between the structural properties, i.e. polarity, growth mechanism, and formation of inclined twin boundaries in pairs. Moreover, the optical properties of the Sn-seeded GaSb nanowires are examined. Their photoluminescence response is compared with one of their Au-seeded counterparts, suggesting the incorporation of Sn atoms from the seed particles into the nanowires.

Emerging theoretical concepts for quantum technologies have driven a continuous search for structures where a quantum state, such as spin, can be manipulated efficiently. Central to many concepts is the ability to control a system by electric and magnetic fields, relying on strong spin-orbit interaction and a large g-factor. Here, we present a mechanism for spin and orbital manipulation using small electric and magnetic fields. By hybridizing specific quantum dot states at two points inside InAs nanowires, nearly perfect quantum rings form. Large and highly anisotropic effective g-factors are observed, explained by a strong orbital contribution. Importantly, we find that the orbital contributions can be efficiently quenched by simply detuning the individual quantum dot levels with an electric field. In this way, we demonstrate not only control of the effective g-factor from 80 to almost 0 for the same charge state, but also electrostatic change of the ground state spin., Quantum technology concepts rely on efficient control of the system state, such as the electron spin. Here the authors present a mechanism for spin and orbital manipulation based on hybridizing quantum dot states at two points inside InAs nanowires, resulting in tunable quantum rings with giant controllable g-factors.

Control of the crystallization process is central to developing novel materials with atomic precision to meet the demands of electronic and quantum technology applications. Semiconductor nanowires grown by the vapor-liquid-solid process are a promising material system in which the ability to form components with structure and composition not achievable in bulk is well-established. Here we use in situ TEM imaging of GaAs nanowire growth to understand the processes by which the growth dynamics are connected to the experimental parameters. We find that two sequential steps in the crystallization process - nucleation and layer growth - can occur on similar time scales and can be controlled independently using different growth parameters. Importantly, the layer growth process contributes significantly to the growth time for all conditions, and will play a major role in determining material properties. The results are understood through theoretical simulations correlating the growth dynamics, liquid droplet and experimental parameters., Differences in comparison to previous version: 1) Title- To avoid unlikely but possible confusion of the term 'step-flow' we call it layer growth in this new version. 2) The data and interpretations are mostly the same as in previous version, but presented in a modified perspective. 3) The simulation was refined further

Tunneling field-effect transistors (TFET) based on a vertical gate-all-around (VGAA) nanowire (NW) architecture with a core-shell (CS) structure have been explored for future CMOS applications. Performance predictions based on a tight-binding mode-space NEGF technique include a drive current $\mathrm{I}_{\mathrm{o}\mathrm{n}}$ of $6.7\ \mu \mathrm{A}$ (NW diameter $\mathrm{d}= 10.2\ \mathrm{nm}$ ) at $\mathrm{V}_{\mathrm{dd}}=0.3\ \mathrm{V}$ under low power (LP) conditions $(\mathrm{I}_{\mathrm{off}}=1 \mathrm{pA})$ for an InAs/GaSb CS TFET. This compares to Si nMOSFET $\mathrm{I}_{\mathrm{on}} =2.3\ \mu \mathrm{A}$ at $\mathrm{V}_{\mathrm{dd}}=0.55\ \mathrm{V}(\mathrm{d}=6\ \mathrm{nm})$ . On the experimental side, scaling of vertical CS NWs resulted in smallest dimensions of $\mathrm{d}_{\mathrm{c}}= 17$ nm (GaSb core) and $\mathrm{t}_{\mathrm{sh}}=3$ nm (InAs shell) for a total diameter of 23 nm. VGAA CS nFETs demonstrated drive current of up to $40\ \mu \mathrm{A} (\mathrm{V}_{\mathrm{d}}=0.3\ \mathrm{V})$ and subthreshold swing $\mathrm{SS}=40\mathrm{mV}/\mathrm{dec}(\mathrm{V}_{\mathrm{d}}=10\mathrm{mV})$ for NW diameters between 35 – 50 nm. Although key TFET properties such as current drive and subthermal SS have been demonstrated using a VGAA CS architecture for the first time, experimental results still lag predictions. An intrinsic relationship between band-to band-tunneling (BTBT) and $\mathrm{D}_{\mathrm{it}}$ related trap assisted tunneling (TAT) was found which imposes challenging $\mathrm{D}_{\mathrm{it}}$ requirements, in particular for LP $\mathrm{I}_{\mathrm{off}}$ specifications. Complexity of fabrication and a material system foreign to CMOS manufacturing further impact prospects of TFET technology.

Semiconductor nanowires offer the opportunity to incorporate novel structures and functionality into electronic and optoelectronic devices. A clear understanding of the nanowire growth mechanism is essential for well-controlled growth of structures with desired properties, but the understanding is currently limited by a lack of empirical measurements of important parameters during growth, such as catalyst particle composition. However, this is difficult to accurately determine by investigating post-growth. We report direct in situ measurement of the catalyst composition during nanowire growth for the first time. We study Au-seeded GaAs nanowires inside an electron microscope as they grow and measure the catalyst composition using X-ray energy dispersive spectroscopy. The Ga content in the catalyst during growth increases with both temperature and Ga precursor flux., Semiconductor nanowires are promising materials for miniaturized devices, but a thorough understanding of their growth mechanism is necessary for controlled synthesis. Here, the authors use in situ spectroscopy and microscopy to measure the composition of the catalyst droplet as a function of different growth parameters during Au-seeded GaAs nanowire growth.