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BACKGROUND: X-ray micro-tomography (μCT) is a powerful non-destructive 3D imaging method applied in many scientific fields. In combination with propagation-based phase-contrast, the method is suitable for samples with low absorption contrast. Phase contrast tomography has become available in the lab with the ongoing development of micro-focused tube sources, but it requires sensitive and high-resolution X-ray detectors. The development of novel scintillation detectors, particularly for microscopy, requires more flexibility than available in commercial tomography systems. OBJECTIVE: We aim to develop a compact, flexible, and versatile μCT laboratory setup that combines absorption and phase contrast imaging as well as the option to use it for scintillator characterization. Here, we present details on the design and implementation of the setup. METHODS: We used the setup for μCT in absorption and propagation-based phase-contrast mode, as well as to study a perovskite scintillator. RESULTS: We show the 2D and 3D performance in absorption and phase contrast mode, as well as how the setup can be used for testing new scintillator materials in a realistic imaging environment. A spatial resolution of around 1.3μm is measured in 2D and 3D. CONCLUSIONS: The setup meets the needs for common absorption μCT applications and offers increased contrast in phase contrast mode. The availability of a versatile laboratory μCT setup allows not only for easy access to tomographic measurements, but also enables a prompt monitoring and feedback beneficial for advances in scintillator fabrication.

X-ray microscopy is an essential imaging method in many scientific fields, which can be extended to three-dimensional (3D) using tomography. Recently, metal halide perovskite (MHP) nanomaterials have become a promising candidate for X-ray scintillators, due to their high light yield, high spatial resolution, and easy fabrication. Tomography requires many projections and therefore scintillators with excellent stability. This is challenging for MHPs, which often suffer from fast degradation under X-ray irradiation and ambient conditions. Here, we demonstrate that MHP scintillators of CsPbBr3 nanowires (diameter: 60 nm, length: 5–9 µm) grown in anodized aluminum oxide (CsPbBr3 NW/AAO) have sufficient stability for X-ray micro-tomography. A tomogram was taken with a Cu X-ray source over 41 h (dose 4.2 Gyair). During this period the scintillator brightness fluctuated less than 5%, which enabled a successful reconstruction. A long-term study with 2 weeks of continuous X-ray exposure (37.5 Gyair) showed less than 14% fluctuations in brightness and no long-term degradation, despite variations in the ambient relative humidity from 7.4 %RH to 34.2 %RH. The resolution was stable at (180 ± 20) 1pmm−1, i.e., about 2.8 micron. This demonstrates that CsPbBr3 NW/AAO scintillators are promising candidates for high resolution X-ray imaging detectors.

Vertically aligned metal halide perovskite (MHP) nanowires are promising for various optoelectronic applications, which can be further enhanced by heterostructures. However, present methods to obtain free-standing vertically aligned MHP nanowire arrays and heterostructures lack the scalability needed for applications. We use a low-temperature solution process to prepare free-standing vertically aligned green-emitting CsPbBr

Strain and interactions at grain boundaries during solid-phase crystallization are known to play a significant role in the functional properties of polycrystalline materials. However, elucidating three-dimensional nanoscale grain morphology, kinetics, and strain under realistic conditions is challenging. Here, we image a single-grain growth during the amorphous-to-polycrystalline transition in technologically relevant transparent conductive oxide (TCO) film of In2O3:Zr with in-situ Bragg coherent X-ray diffraction imaging and transmission electron microscopy. We find that the Johnson-Mehl-Avrami-Kolmogorov theory, which describes the average kinetics of polycrystalline films growth, can be applied to the single grains as well. The quantitative analysis stems directly from imaging results. We elucidate the interface-controlled nature of the single-grain growth in thin films and reveal the surface strains which may be a driving force for anisotropic crystallization rates. Our results bring in-situ imaging with coherent X-rays towards understanding and controlling the crystallization processes of TCOs and other polycrystalline materials at the nanoscale.

Nanoscale X-ray detectors could allow higher resolution in imaging and diffraction experiments than established systems but are difficult to design due to the long absorption length of X-rays. Here, we demonstrate X-ray detection in a single nanowire in which the nanowire axis is parallel to the optical axis. In this geometry, X-ray absorption can occur along the nanowire length, while the spatial resolution is limited by the diameter. We use the device to make a high-resolution 3D image of the 88 nm diameter X-ray nanofocus at the Nanomax beamline, MAX IV synchrotron, by scanning the single pixel device in different planes along the optical axis. The images reveal fine details of the beam that are unattainable with established detectors and show good agreement with ptychography.

The interest in metal halide perovskites has grown as impressive results have been shown in solar cells, light emitting devices, and scintillators, but this class of materials have a complex crystal structure that is only partially understood. In particular, the dynamics of the nanoscale ferroelastic domains in metal halide perovskites remains difficult to study. An ideal in situ imaging method for ferroelastic domains requires a challenging combination of high spatial resolution and long penetration depth. Here, we demonstrate in situ temperature-dependent imaging of ferroelastic domains in a single nanowire of metal halide perovskite, CsPbBr3. Scanning X-ray diffraction with a 60 nm beam was used to retrieve local structural properties for temperatures up to 140 °C. We observed a single Bragg peak at room temperature, but at 80 °C, four new Bragg peaks appeared, originating in different real-space domains. The domains were arranged in periodic stripes in the center and with a hatched pattern close to the edges. Reciprocal space mapping at 80 °C was used to quantify the local strain and lattice tilts, revealing the ferroelastic nature of the domains. The domains display a partial stability to further temperature changes. Our results show the dynamics of nanoscale ferroelastic domain formation within a single-crystal perovskite nanostructure, which is important both for the fundamental understanding of these materials and for the development of perovskite-based devices.

Axially heterostructured nanowires are a promising platform for next generation electronic and optoelectronic devices. Reports based on theoretical modeling have predicted more complex strain distributions and increased critical layer thicknesses than in thin films, due to lateral strain relaxation at the surface, but the understanding of the growth and strain distributions in these complex structures is hampered by the lack of high-resolution characterization techniques. Here, we demonstrate strain mapping of an axially segmented GaInP-InP 190 nm diameter nanowire heterostructure using scanning X-ray diffraction. We systematically investigate the strain distribution and lattice tilt in three different segment lengths from 45 to 170 nm, obtaining strain maps with about 10−4 relative strain sensitivity. The experiments were performed using the 90 nm diameter nanofocus at the NanoMAX beamline, taking advantage of the high coherent flux from the first diffraction limited storage ring MAX IV. The experimental results are in good agreement with a full simulation of the experiment based on a three-dimensional (3D) finite element model. The largest segments show a complex profile, where the lateral strain relaxation at the surface leads to a dome-shaped strain distribution from the mismatched interfaces, and a change from tensile to compressive strain within a single segment. The lattice tilt maps show a cross-shaped profile with excellent qualitative and quantitative agreement with the simulations. In contrast, the shortest measured InP segment is almost fully adapted to the surrounding GaInP segments.

Semiconductor nanowires in wrapped, gate-all-around transistor geometry are highly favorable for future electronics. The advanced nanodevice processing results in strain due to the deposited dielectric and metal layers surrounding the nanowires, significantly affecting their performance. Therefore, non-destructive nanoscale characterization of complete devices is of utmost importance due to the small feature sizes and three-dimensional buried structure. Direct strain mapping inside heterostructured GaSb-InAs nanowire tunnel field-effect transistor embedded in dielectric HfO2, W metal gate layers, and an organic spacer is performed using fast scanning X-ray nanodiffraction. The effect of 10 nm W gate on a single embedded nanowire with segment diameters down to 40 nm is retrieved. The tensile strain values reach 0.26% in the p-type GaSb segment of the transistor. Supported by the finite element method simulation, we establish a connection between the Ar pressure used during the W layer deposition and the nanowire strain state. Thus, we can benchmark our models for further improvements in device engineering. Our study indicates, how the significant increase in X-ray brightness at 4th generation synchrotron, makes high-throughput measurements on realistic nanoelectronic devices viable.

Metal halide perovskites (MHPs) have been studied intensely as the active material for optoelectronic devices. Lithography methods for perovskites remain limited because of the solubility of perovskites in polar solvents. Here, we demonstrate an electron-beam-lithography process with a poly(methyl methacrylate) resist based on the nonpolar solvents

Nanowire growth enables creation of embedded heterostructures, where one material is completely surrounded by another. Through materials-selective post-growth oxidation it is also possible to combine amorphous oxides and crystalline, e.g. III–V materials. Such oxide-embedded structures pose a challenge for compositional characterization through transmission electron microscopy since the materials will overlap in projection. Furthermore, materials electrically isolated by an embedding oxide are more sensitive to electron beam-induced alterations. Methods that can directly isolate the embedded material, preferably at reduced electron doses, will be required in this situation. Here, we analyse the performance of two such techniques—local lattice parameter measurements from high resolution micrographs and bulk plasmon energy measurements from electron energy loss spectra—by applying them to analyse InP-AlInP segments embedded in amorphous aluminium oxide. We demonstrate the complementarity of the two methods, which show an overall excellent agreement. However, in regions with residual strain, which we analyse through molecular dynamics simulations, the two techniques diverge from the true value in opposite directions.

X-ray scintillation detectors based on metal halide perovskites have shown excellent light yield, but they mostly target applications with spatial resolution at the tens of micrometers level. Here, we use a one-step solution method to grow arrays of 15-μm-long single-crystalline CsPbBr3 nanowires (NWs) in an AAO (anodized aluminum oxide) membrane template, with nanowire diameters ranging from 30 to 360 nm. The CsPbBr3 nanowires in AAO (CsPbBr3 NW/AAO) show increasing X-ray scintillation efficiency with decreasing nanowire diameter, with a maximum photon yield of ∼5 300 ph/MeV at 30 nm diameter. The CsPbBr3 NW/AAO composites also display high radiation resistance, with a scintillation-intensity decrease of only ∼20–30% after 24 h of X-ray exposure (integrated dose 162 Gyair) and almost no change after ambient storage for 2 months. X-ray images can distinguish line pairs with a spacing of 2 μm for all nanowire diameters, while slanted edge measurements show a spatial resolution of ∼160 lp/mm at modulation transfer function (MTF) = 0.1. The combination of high spatial resolution, radiation stability, and easy fabrication makes these CsPbBr3 NW/AAO scintillators a promising candidate for high-resolution X-ray imaging applications.

Crystallography is an invaluable tool in materials science, solid state physics and protein science. Understanding crystallography requires grasping the powerful but abstract concept of reciprocal space. Here a simple but insightful experiment using a laser pointer and Au microdisc arrays to explore and illustrate Bragg diffraction and reciprocal space is demonstrated. The Au microdisc arrays were manufactured using standard semiconductor fabrication techniques. The flexibility of the array design allows the demonstration of basic concepts such as lattice and atomic form factor, but also more advanced ones such as quasicrystal and shape function.

Ferroelectric and ferroelastic domains have been predicted to enhance metal halide perovskite (MHP) solar cell performance. While the formation of such domains can be modified by temperature, pressure, or strain, established methods lack spatial control at the level of single domains. Here, we induce the formation of ferroelastic domains in CsPbBr3 nanowires at room temperature using an atomic force microscope (AFM) tip and visualize the domains using nanofocused x-ray diffraction with a 60 nm beam. Regions scanned with a low AFM tip force show orthorhombic 004 reflections along the nanowire axis, while regions exposed to higher forces exhibit 220 reflections. The applied stress locally changes the crystal structure, leading to lattice tilts that define ferroelastic domains, which spread spatially and terminate at {112}-type domain walls. The ability to induce individual ferroelastic domains within MHPs using AFM gives new possibilities for device design and fundamental experimental studies.

Nanofocused X-ray beam induced current (XBIC) is used to quantitatively map the spatially dependent carrier collection probability within single nanowires., Here it is demonstrated how nanofocused X-ray beam induced current (XBIC) can be used to quantitatively map the spatially dependent carrier collection probability within nanostructured solar cells. The photocurrent generated by a 50 nm-diameter X-ray beam was measured as a function of position, bias and flux in single p–i–n doped solar-cell nanowires. The signal gathered mostly from the middle segment decays exponentially toward the p- and n-segments, with a characteristic decay length that varies between 50 nm and 750 nm depending on the flux and the applied bias. The amplitude of the XBIC shows saturation at reverse bias, which indicates that most carriers are collected. At forward bias, the relevant condition for solar cells, the carrier collection is only efficient in a small region. Comparison with finite element modeling suggests that this is due to unintentional p-doping in the middle segment. It is expected that nanofocused XBIC could be used to investigate carrier collection in a wide range of nanostructured solar cells.

First results of in-line holography and holotomography from the NanoMAX beamline at MAX IV are presented., Coherent X-ray imaging techniques, such as in-line holography, exploit the high brilliance provided by diffraction-limited storage rings to perform imaging sensitive to the electron density through contrast due to the phase shift, rather than conventional attenuation contrast. Thus, coherent X-ray imaging techniques enable high-sensitivity and low-dose imaging, especially for low-atomic-number (Z) chemical elements and materials with similar attenuation contrast. Here, the first implementation of in-line holography at the NanoMAX beamline is presented, which benefits from the exceptional focusing capabilities and the high brilliance provided by MAX IV, the first operational diffraction-limited storage ring up to approximately 300 eV. It is demonstrated that in-line holography at NanoMAX can provide 2D diffraction-limited images, where the achievable resolution is only limited by the 70 nm focal spot at 13 keV X-ray energy. Also, the 3D capabilities of this instrument are demonstrated by performing holotomography on a chalk sample at a mesoscale resolution of around 155 nm. It is foreseen that in-line holography will broaden the spectra of capabilities of MAX IV by providing fast 2D and 3D electron density images from mesoscale down to nanoscale resolution.

Journal of synchrotron radiation 28(5), 1573 - 1582 (2021). doi:10.1107/S1600577521006159, Using multilayer zone plates (MZPs) as two-dimensional optics, focal spot sizes of less than 10 nm can be achieved, as we show here with a focus of 8.4 nm × 9.6 nm, but the need for order-sorting apertures prohibits practical working distances. To overcome this issue, here an off-axis illumination of a circular MZP is introduced to trade off between working distance and focal spot size. By this, the working distance between order-sorting aperture and sample can be more than doubled. Exploiting a 2D focus of 16 nm × 28 nm, real-space 2D mapping of local electric fields and charge carrier recombination using X-ray beam induced current in a single InP nanowire is demonstrated. Simulations show that a dedicated off-axis MZP can reach sub-10 nm focusing combined with reasonable working distances and low background, which could be used for in operando imaging of composition, carrier collection and strain in nanostructured devices., Published by Wiley-Blackwell, [S.l.]

Metal halide perovskites show great promise for a wide range of optoelectronic applications but are plagued by instability when exposed to air and light. This work presents low-temperature solution growth of vertically aligned CsPbBr3 nanowire arrays in AAO (anodized aluminum oxide) templates with excellent stability, with samples exposed to air for 4 months still exhibiting comparable photoluminescence and UV stability to fresh samples. The single-crystal nanowire length is adjusted from ∼100 nm to 5 μm by adjusting the precursor solution amount and concentration, and we observe length-to-diameter ratios as high as 100. Structural characterization results indicate that large-diameter CsPbBr3 nanowires have an orthorhombic structure, while the 10 nm- and 20 nm-diameter nanowires adopt a cubic structure. Photoluminescence shows a gradual blue-shift in emission with decreasing nanowire diameter and marginal changes under varying illumination power intensity. The CsPbBr3-nanowires/AAO composite exhibits excellent resistance to X-ray radiation and long-term air storage, which makes it promising for future optoelectronic applications such as X-ray scintillators. These results show how physical confinement in AAO can be used to realize CsPbBr3 nanowire arrays and control their morphology and crystal structure.

Bragg coherent diffraction imaging is a powerful strain imaging tool, often limited by beam-induced sample instability for small particles and high power densities. Here, we devise and validate an adapted diffraction volume assembly algorithm, capable of recovering three-dimensional datasets from particles undergoing uncontrolled and unknown rotations. We apply the method to gold nanoparticles which rotate under the influence of a focused coherent x-ray beam, retrieving their three-dimensional shapes and strain fields. The results show that the sample instability problem can be overcome, enabling the use of fourth generation synchrotron sources for Bragg coherent diffraction imaging to their full potential. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under Contract No. 2018-07152, the Swedish Governmental Agency for Innovation Systems under Contract No. 2018-04969, and Formas under Contract No. 2019-02496. This work has also received funding from the ÅForsk Foundation (Contract No. 17-408), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Contract No. 801847), from the Olle Engkvist Foundation, from the Swedish Research council (Contract No. 2018-00234), and from NanoLund.

Propagation-based phase contrast imaging (PB-PCI) with an X-ray lab source is a powerful technique to study low absorption samples, e.g. soft tissue or plastics, on the micrometer scale but is often limited by the low flux and coherence of the source. The setup geometry is essential for the performance since there is a trade-off where a short source distance yields a high contrast-to-noise ratio (CNR) but a low relative fringe contrast. While theoretical optimization strategies based on Fresnel propagation have been reported, there is a need for experimental testing of these models. Here, we systematically investigate this trade-off experimentally using two different setups with high-resolution detectors: a custom-built system with a Cu X-ray source and a commercial system (Zeiss Xradia) with a W source. The fringe contrast, CNR and fringe separation for a low-absorption test sample were measured for 130 different combinations of magnification and overall distances. We find that these figures-of-merit are sensitive to the magnification and that an optimum can be found that is independent of the overall source-detector distance. In general, we find that the theoretical models show excellent agreement with the measurements. However, this requires the complicated X-ray spectrum to be considered, in particular for the broadband W source.

Correction for ‘Strain mapping inside an individual processed vertical nanowire transistor using scanning X-ray nanodiffraction’ by Dmitry Dzhigaev et al., Nanoscale, 2020, 12, 14487–14493, DOI: 10.1039/D0NR02260H.

Metal halide perovskites attract significant interest due to their remarkable performance in optoelectronic devices. However, the gap in understanding the relationship between their nanoscale structure and properties limits their application towards novel devices. In this work, twinned ferroelastic domains in single 500 nm CsPbBr3 particles are studied with 3D Bragg coherent x-ray diffraction imaging. A preferential double-domain structure is revealed in four identical particles, with one domain oriented along the [110] and the other along the [002] direction. The particles exhibit similar scattering volume ratios of 0.12 ± 0.026 between twin phases, suggesting the possibility of a deterministic formation process. The domains exhibit a difference in lattice tilt of 0.59 degrees, in excellent agreement with calculations of the lattice mismatch at the (112) twin boundary. These results provide important insights both for the fundamental understanding of ferroelastic nanoscale materials and for the performance improvement of perovskite-based devices. Moreover, this work paves the way towards real-time imaging of the domain dynamics in ferroic systems.

Time-resolved finite-element modelling is used to study the sample heating from intense X-ray irradiation., Recent developments in synchrotron brilliance and X-ray optics are pushing the flux density in nanofocusing experiments to unprecedented levels, which increases the risk of different types of radiation damage. The effect of X-ray induced sample heating has been investigated using time-resolved and steady-state three-dimensional finite-element modelling of representative nanostructures. Simulations of a semiconductor nanowire indicate that the heat generated by X-ray absorption is efficiently transported within the nanowire, and that the temperature becomes homogeneous after about 5 ns. The most important channel for heat loss is conduction to the substrate, where the heat transfer coefficient and the interfacial area are limiting the heat transport. While convective heat transfer to air is significant, the thermal radiation is negligible. The steady-state average temperature in the nanowire is 8 K above room temperature at the reference parameters. In the absence of heat transfer to the substrate, the temperature increase at the same flux reaches 55 K in air and far beyond the melting temperature in vacuum. Reducing the size of the X-ray focus at constant flux only increases the maximum temperature marginally. These results suggest that the key strategy for reducing the X-ray induced heating is to improve the heat transfer to the surrounding.

We have investigated strained GaAs-GaInP core-shell nanowires using transmission electron microscopy and nanofocused scanning X-ray diffraction. Nominally identical growth conditions for each sample were achieved by using nanoimprint lithography to create wafer-scale arrays of Au seed particles. However, we observe large individual differences, with neighboring nanowires showing either straight, bent, or twisted morphology. Using scanning X-ray diffraction, we reconstructed and quantified the bending and twisting of the nanowires in three dimensions. In one nanowire, we find that the shell lattice is tilted with respect to the core lattice, with an angle that increases from 2° at the base to 5° at the top. Furthermore, the azimuthal orientation of the tilt changes by 30° along the nanowire axis. Our results demonstrate how strained core-shell nanowire growth can lead to a rich interplay of composition, lattice mismatch, bending and lattice tilt, with additional degrees of complexity compared with thin films.

The coherence of polaritons plays a fundamental role in numerous recent experimental observations, from strong coupling to Bose-Einstein condensation, but accessing the coherence of polaritons is a difficult task due to the high energy of plasmons and excitons. However, surface phonon polaritons offer similar promises at much lower energy. Here, we demonstrate the possibility to use visible ultrafast lasers to generate and time resolve coherent surface phonon polaritons in nanowires. We show that these modes are generated through the ultrafast screening of the surface depletion field. By comparing experiments and FDTD simulations, we show that this method allows the simultaneous generation of dark and bright mode. Our observations open the way to deeper investigations of the role of coherence in the rich polariton physics.

The long absorption length of hard X-rays makes them ideal tools for investigating electronic and optoelectronic devices in realistic operational conditions. Modern X-ray optics reach the relevant length scales for single nanoelectronic devices. Here, methods to investigate single nanowire devices with nanofocused X-rays are discussed. The X-rays are used both as pump and probe of semiconductor nanowire devices. Nanofocused X-ray diffraction was used to quantify bending and lattice tilt in strained core-shell nanowires as well as electrically biased nanowire devices. The carrier collection in single solar cell nanowires was probed with X-ray beam induced current. X-ray fluorescence mapping at 50 nm spatial resolution of Zn doping in solar cell nanowires revealed background doping and long gradients. The demonstrated methods are relevant for a wide range of nanoscale semiconductor devices.

The opportunity to engineer III-V nanowires in wurtzite and zinc blende crystal structure allows for exploring properties not conventionally available in the bulk form as well as opening the opportunity for use of additional degrees of freedom in device fabrication. However, the fundamental understanding of the nature of polytypism in III-V nanowire growth is still lacking key ingredients to be able to connect the results of modeling and experiments. Here we show InP nanowires of both pure wurtzite and pure zinc blende grown simultaneously on the same InP [100]-oriented substrate. We find wurtzite nanowires to grow along [Formula: see text] and zinc blende counterparts along [Formula: see text]. Further, we discuss the nucleation, growth, and polytypism of our nanowires against the background of existing theory. Our results demonstrate, first, that the crystal growth conditions for wurtzite and zinc blende nanowire growth are not mutually exclusive and, second, that the interface energies predominantly determine the crystal structure of the nanowires.

Simultaneous Bragg diffraction and coherent small-angle scattering of a single solar cell nanowire is demonstrated, using a nanofocused hard X-ray beam and two detectors., Simultaneous scanning Bragg contrast and small-angle ptychographic imaging of a single solar cell nanowire are demonstrated, using a nanofocused hard X-ray beam and two detectors. The 2.5 µm-long nanowire consists of a single-crystal InP core of 190 nm diameter, coated with amorphous SiO2 and polycrystalline indium tin oxide. The nanowire was selected and aligned in real space using the small-angle scattering of the 140 × 210 nm X-ray beam. The orientation of the nanowire, as observed in small-angle scattering, was used to find the correct rotation for the Bragg condition. After alignment in real space and rotation, high-resolution (50 nm step) raster scans were performed to simultaneously measure the distribution of small-angle scattering and Bragg diffraction in the nanowire. Ptychographic reconstruction of the coherent small-angle scattering was used to achieve sub-beam spatial resolution. The small-angle scattering images, which are sensitive to the shape and the electron density of all parts of the nanowire, showed a homogeneous profile along the nanowire axis except at the thicker head region. In contrast, the scanning Bragg diffraction microscopy, which probes only the single-crystal InP core, revealed bending and crystalline inhomogeneity. Both systematic and non-systematic real-space movement of the nanowire were observed as it was rotated, which would have been difficult to reveal only from the Bragg scattering. These results demonstrate the advantages of simultaneously collecting and analyzing the small-angle scattering in Bragg diffraction experiments.

International audience; The properties of semiconductors can be controlled using doping, making it essential for electronic and optoelectronic devices. However, with shrinking device sizes it becomes increasingly difficult to quantify doping with sufficient sensitivity and spatial resolution. Here, we demonstrate how X-ray fluorescence mapping with a nanofocused beam, nano-XRF, can quantify Zn doping within in situ doped III-V nanowires, by using large area detectors and high-efficiency focusing optics. The spatial resolution is defined by the focus size to 50 nm. The detection limit of 7 ppm (2.8 X 10(17) cm(-3)), corresponding to about 150 Zn atoms in the probed volume, is bound by a background signal. In solar cell InP nanowires with a p-i-n doping profile, we use nano-XRF to observe an unintentional Zn doping of 5 x 10(17) cm(-3) in the middle segment. We investigated the dynamics of in situ Zn doping in a dedicated multisegment nanowire, revealing significantly sharper gradients after turning the Zn source off than after turning the source on. Nano-XRF could be used for quantitative mapping of a wide range of dopants in many types of nanostructures.

International audience; We demonstrate x-ray absorption fine structure spectroscopy (XAFS) detected by x-ray beam induced current (XBIC) in single n(+)i-n(+) doped nanowire devices. Spatial scans with the 65 nm diameter beam show a peak of the XBIC signal in the middle segment of the nanowire. The XBIC and the x-ray fluorescence signals were detected simultaneously as a function of the excitation energy near the Ga K absorption edge at 10.37 keV. The spectra show similar oscillations around the edge, which shows that the XBIC is limited by the primary absorption. Our results reveal the feasibility of the XBIC detection mode for the XAFS investigation in nanostructured devices.

Measuring lifetime of photogenerated charges in semiconductor nanowires (NW) is important for understanding light-induced processes in these materials and is relevant for their photovoltaic and photodetector applications. In this paper, we investigate the dynamics of photogenerated charge carriers in a series of as-grown InP NW with different levels of sulfur (S) doping. We observe that photoluminescence (PL) decay time as well as integrated PL intensity decreases with increasing S doping. We attribute these observations to hole trapping with the trap density increased due to S-doping level followed by nonradiative recombination of trapped charges. This assignment is proven by observation of the trap saturation in three independent experiments: via excitation power and repetition rate PL lifetime dependencies and by PL pump-probe experiment.

Multilayer zone plates can be used for holographic imaging without an order-sorting aperture., This article describes holographic imaging experiments using a hard X-ray multilayer zone plate (MZP) with an outermost zone width of 10 nm at a photon energy of 18 keV. An order-sorting aperture (OSA) is omitted and emulated during data analysis by a ‘software OSA’. Scanning transmission X-ray microscopy usually carried out in the focal plane is generalized to the holographic regime. The MZP focus is characterized by a three-plane phase-retrieval algorithm to an FWHM of 10 nm.

Radiative recombination in degenerately n-doped InP nanowires is studied for excitation above and below the Fermi energy of the electron gas, using photoluminescence. Laser-induced electron heating is observed, which allows absorption below the Fermi energy. We observe photon upconversion where photo-excited holes recombine with high |k| electrons. This can be attributed to hole scattering to high |k|-values, and the temperature dependence of this process is measured. We show that hole relaxation via phonon scattering can be observed in continuous wave excitation luminescence measurements.

We report on electrical and optical properties of p+-i-n+ photodetectors/solar cells based on square millimeter arrays of InP nanowires (NWs) grown on InP substrates. The study includes a sample series where the p+-segment length was varied between 0 and 250 nm, as well as solar cells with 9.3% efficiency with similar design. The electrical data for all devices display clear rectifying behavior with an ideality factor between 1.8 and 2.5 at 300 K. From spectrally resolved photocurrent measurements, we conclude that the photocurrent generation process depends strongly on the p+-segment length. Without a p+-segment, photogenerated carriers funneled from the substrate into the NWs contribute strongly to the photocurrent. Adding a p+-segment decouples the substrate and shifts the depletion region, and collection of photogenerated carriers, to the NWs, in agreement with theoretical modeling. In optimized solar cells, clear spectral signatures of interband transitions in the zinc blende and wurtzite InP layers of the mixed-phase i-segments are observed. Complementary electroluminescence, transmission electron microscopy (TEM), as well as measurements of the dependence of the photocurrent on angle of incidence and polarization, support our interpretations.

We have performed near-field x-ray imaging with simultaneous object and probe reconstruction. By an advanced ptychographic algorithm based on longitudinal and lateral translations, full-field images of nanoscale objects are reconstructed with quantitative contrast values, along with the extended wavefronts used to illuminate the objects. The imaging scheme makes idealizing assumptions on the probe obsolete, and efficiently disentangles phase shifts related to the object from the imperfections in the illumination. We validate this approach by comparison to the conventional reconstruction scheme without simultaneous probe retrieval, based on the contrast transfer function algorithm. To this end, a set of semiconductor nanowires with controlled chemical composition (InP core, insulating SiO2 layer, and indium tin oxide cover) is imaged using the quasi-point source illumination realized by the hard x-ray nanofocus (26 nm×39 nm spot size) of the ID16A Nano-Imaging beamline at the European Synchrotron Radiation Facility.

The advent of nanofocused X-ray beams has allowed the study of single nanocrystals and complete nanoscale devices in a nondestructive manner, using techniques such as scanning transmission X-ray microscopy (STXM), X-ray fluorescence (XRF) and X-ray diffraction (XRD). Further insight into semiconductor devices can be achieved by combining these techniques with simultaneous electrical measurements. Here, we present a system for electrical biasing and current measurement of single nanostructure devices, which has been developed for the NanoMAX beamline at the fourth-generation synchrotron, MAX IV, Sweden. The system was tested on single InP nanowire devices. The mechanical stability was sufficient to collect scanning XRD and XRF maps with a 50 nm diameter focus. The dark noise of the current measurement system was about 3 fA, which allowed fly scan measurements of X-ray beam induced current (XBIC) in single nanowire devices.

Realizing photon upconversion in nanostructures is important for many next-generation applications such as biological labelling, infrared detectors and solar cells. In particular nanowires are attractive for optoelectronics because they can easily be electrically contacted. Here we demonstrate photon upconversion with a large energy shift in highly n-doped InP nanowires. Crucially, the mechanism responsible for the upconversion in our system does not rely on multi-photon absorption via intermediate states, thus eliminating the need for high photon fluxes to achieve upconversion. The demonstrated upconversion paves the way for utilizing nanowires—with their inherent flexibility such as electrical contactability and the ability to position individual nanowires—for photon upconversion devices also at low photon fluxes, possibly down to the single photon level in optimised structures. Open image in new window

Improving Nanowire Photovoltaics In principle, solar cells based on arrays of nanowires made from compound inorganic semiconductors, such as indium phosphide (InP), should decrease materials and fabrication costs compared with planar junctions. In practice, device efficiencies tend to be low because of poor light absorption and increased rates of unproductive charge recombination in the surface region. Wallentin et al. (p. 1057 , published online 17 January) now report that arrays of p-i-n InP nanowires (that switch from positive to negative doping), grown to millimeter lengths, can be optimized by varying the nanowire diameter and length of the n-doped segment. Efficiencies as high as 13.8% were achieved, which are comparable to the best planar InP photovoltaics.

Scattering of photons by phonons, or Brillouin scattering, enables manipulation and control of light and has led to revolutionary applications, from slow light to saser and cooling of micromechanical resonators. Recently, enhanced light and sound interaction has been demonstrated in waveguides. However, the design of the waveguide geometry tunes and alters the phonon and photon dispersion simultaneously. Here we investigate, through femtosecond pump-probe spectroscopy and theoretical modeling, the light and sound interaction in a bottom-up fabricated vertical nanowire photonic crystal. In such a system, the phonon dispersion can be tuned by varying the geometry of the constituent nanowires. In contrast, the placement of the nanowires in the photonic crystal can be used for tuning optical array modes, without altering the phonon dispersion. We demonstrate the forward and backward scattering, by acoustic phonons in the nanowires, of (1) such optical array modes and (2) guided modes of the constituent nanowires. Furthermore, our results reveal an enhanced interaction of array modes with phonons that we attribute to the specific scattering mechanism. Our results enable the design of a photonic crystal with separately tailored photon and phonon dispersion for Brillouin scattering. We anticipate these advances to be a starting point for enhanced control of light at the nanoscale.

Position controlled nanowire growth is important for nanowire-based optoelectronic components which rely on light emission or light absorption. For solar energy harvesting applications, dense arrays of nanowires are needed; however, a major obstacle to obtaining dense nanowire arrays is seed particle displacement and coalescing during the annealing stage prior to nanowire growth. Here, we explore three different strategies to improve pattern preservation of large-area catalyst particle arrays defined by nanoimprint lithography for nanowire growth. First, we see that heat treating the growth substrate prior to nanoimprint lithography improves pattern preservation. Second, we explore the possibility of improving pattern preservation by fixing the seed particles in place prior to annealing by modifying the growth procedure. And third, we show that a SiNx growth mask can fully prevent seed particle displacement. We show how these strategies allow us to greatly improve the pattern fidelity of grown InP nanowire arrays with dimensions suitable for solar cell applications, ultimately achieving 100% pattern preservation over the sampled area. The generic nature of these strategies is supported through the synthesis of GaAs and GaP nanowires. [Figure not available: see fulltext.] (Less)

Using both synchrotron-based photoemission electron microscopy/spectroscopy and scanning tunneling microscopy/spectroscopy, we obtain a complete picture of the surface composition, morphology, and electronic structure of InP nanowires. Characterization is done at all relevant length scales from micrometer to nanometer. We investigate nanowire surfaces with native oxide and molecular adsorbates resulting from exposure to ambient air. Atomic hydrogen exposure at elevated temperatures which leads to the removal of surface oxides while leaving the crystalline part of the wire intact was also studied. We show how surface chemical composition will seriously influence nanowire electronic properties. However, opposite to, for example, Ge nanowires, water or sulfur molecules adsorbed on the exterior oxidized surfaces are of less relevance. Instead, it is the final few atomic layers of the oxide which plays the most significant role by strongly negatively doping the surface. The InP nanowires in air are rather insensitive to their chemical surroundings in contrast to what is often assumed for nanowires. Our measurements allow us to draw a complete energy diagram depicting both band gap and differences in electron affinity across an axial nanowire p-n junction. Our findings thus give a robust set of quantitative values relating surface chemical composition to specific electronic properties highly relevant for simulating the performance of nanoscale devices.

Semiconductor III-V nanowires are promising components of future electronic and optoelectronic devices, but they typically show a mixed wurtzite-zinc blende crystal structure. Here we show, theoretically and experimentally, that the crystal structure dominates the conductivity in such InP nanowires. Undoped devices show very low conductivities and mobilities. The zincblende segments are quantum wells orthogonal to the current path and our calculations indicate that an electron concentration of up to 4.6 × 10(18) cm(-3) can be trapped in these. The calculations also show that the room temperature conductivity is controlled by the longest zincblende segment, and that stochastic variations in this length lead to an order of magnitude variation in conductivity. The mobility shows an unexpected decrease for low doping levels, as well as an unusual temperature dependence that bear resemblance with polycrystalline semiconductors.