Laser-assisted atom probe tomography (APT) was used to measure the indium mole fraction x of c-plane, MOCVD-grown, GaN/In(x)Ga(1-x)N/GaN test structures and the results were compared with Rutherford backscattering analysis (RBS). Four sample types were examined with (RBS determined) x = 0.030, 0.034, 0.056, and 0.112. The respective In(x)Ga(1-x)N layer thicknesses were 330 nm, 327 nm, 360 nm, and 55 nm. APT data were collected at (fixed) laser pulse energy (PE) selected within the range of (2-1000) fJ. Sample temperatures were = 54 K. PE within (2-50) fJ yielded x values that agreed with RBS (within uncertainty) and were comparatively insensitive to region-of-interest (ROI) geometry and orientation. By contrast, approximate stoichiometry was only found in the GaN portions of the samples provided PE was within (5-20) fJ and the analyses were confined to cylindrical ROIs (of diameters =20 nm) that were coaxial with the specimen tips. m-plane oriented tips were derived from c-axis grown, core-shell, GaN/In(x)Ga(1-x)N nanorod heterostructures. Compositional analysis along [0 0 0 1] (transverse to the long axis of the tip), of these m-plane samples revealed a spatial asymmetry in charge-state ratio (CSR) and a corresponding asymmetry in the resultant tip shape along this direction; no asymmetry in CSR or tip shape was observed for analysis along [-1 2-1 0]. Simulations revealed that the electric field strength at the tip apex was dominated by the presence of a p-type inversion layer, which developed under typical tip-electrode bias conditions for the n-type doping levels considered. Finally, both c-plane and m-plane sample types showed depth-dependent variations in absolute ion counts that depended upon ROI placement.
We report the influence of the In mole fraction on the material and electrical characteristics of p-i-n InxGa1-xN homojunctions (x = 0.10-0.40) synthesized by plasma-assisted molecular-beam epitaxy on GaN-on-sapphire substrates. Junctions terminated with p-InGaN present improved carrier extraction efficiency in comparison with devices capped with p-GaN, due to the deleterious effect of polarization discontinuities on the device performance. We demonstrate that the presence of Mg does not perturb the In incorporation in InGaN, and it leads to a significant reduction of the stacking fault densit…
We report the interplay between In incorporation and strain relaxation kinetics in high-In-content InxGa1-xN (x = 0.3) layers grown by plasma-assisted molecular-beam epitaxy. For In mole fractions x = 0.13-0.48, best structural and morphological quality is obtained under In excess conditions, at In accumulation limit, and at a growth temperature where InGaN decomposition is active. Under such conditions, in situ and ex situ analysis of the evolution of the crystalline structure with the growth thickness points to an onset of misfit relaxation after the growth of 40 nm, and a gradual relaxation…
InGaN/GaN tunnel junction contacts were grown on top of an InGaN/GaN blue (450 nm) light emitting diode wafer using plasma assisted molecular beam epitaxy. The tunnel junction contacts enable low spreading resistance n-GaN top contact layer thereby requiring less top metal contact coverage on the surface. A voltage drop of 5.3 V at 100 mA, forward resistance of 2 x 10-2 ohm cm2 and a higher light output power are measured in tunnel junction LED. A low resistance of 5 x 10-4 ohm cm2 was measured in a MBE grown tunnel junction on GaN PN junction device, indicating that the tunnel junction LED de…
We report a correlative microscopy study of a sample containing three stacks of InGaN/GaN quantum dots (QDs) grown at different substrate temperature, each stack consisting of 3 layers of QDs. Decreasing the substrate temperature along the growth axis leads to the proliferation of structural defects. However, the luminescence intensity increases towards the surface, in spite of the higher density of threading dislocations, revealing that the QD layers closer to the substrate behave as traps for non-radiative point defects. During atom probe tomography experiments combined with in-situ micro-ph…
Photoelectrocatalytic (PEC) reduction of N2 to ammonia (NH3) is emerging as the potential alternative to overcome the standard Haber-Bosch approach. In this communication, solar N2 reduction was demonstrated with molybdenum carbide (Mo2C) co-catalyst assisted indium gallium nitride (InGaN) nanowires. The effect of aiding Mo2C on InGaN NWs arrests the dark current and demonstrated the saturation current under illumination was briefly elucidated. Large NH3 production of 7.2 gh-1cm-2 with high Faradaic efficiency of 12.6 % was realized at -0.2 V vs. reversible hydrogen electrode for the Mo2C/GaN/…
Spectroscopic Signature of Local Alloy Fluctuations in InGaN/GaN Multi-Quantum-Disk Light Emitting Diode Heterostructures and Its Impact on the Optical Performance
This report classifies emission inhomogeneities that manifest in InGaN quantum well blue light-emitting diodes grown by plasma-assisted molecular beam epitaxy on free-standing GaN substrates. By a combination of spatially resolved electroluminescence and cathodoluminescence measurements, atomic force microscopy, scanning electron microscopy and hot wet KOH etching, the identified inhomogeneities are found to fall in four categories. Labeled here as type I through IV, they are distinguishable by their size, density, energy, intensity, radiative and electronic characteristics and chemical etch p…
Functional properties of nanomaterials strongly depend on their surface atomic structure, but they often become largely different from their bulk structure, exhibiting surface reconstructions and relaxations. However, most of the surface characterization methods are either limited to 2-dimensional measurements or not reaching to true 3D atomic-scale resolution, and single-atom level determination of the 3D surface atomic structure for general 3D nanomaterials still remains elusive. Here we show the measurement of 3D atomic structure of a Pt nanoparticle at 15 pm precision, aided by a deep lear…
Ion generation by photoionization and photofield tunneling of electrons during atom probe tomography of thermally grown chromia with deep UV laser light
We determined a full 3D atomic structure of a dumbbell-shaped Pt nanoparticle formed by a coalescence of two nanoclusters using deep learning assisted atomic electron tomography. Formation of double twin boundary was clearly observed at the interface, while substantial anisotropy and disorder were also found throughout the nanodumbbell. This suggests that the diffusion of interfacial atoms mainly governed the coalescence process, but other dynamic processes such as surface restructuring and plastic deformation were also involved. A full 3D strain tensor was clearly mapped, which allows direct …
The precise knowledge of the atomic order in monocrystalline alloys is fundamental to understand and predict their physical properties. With this perspective, we utilized laser-assisted atom probe tomography to investigate the three-dimensional distribution of atoms in non-equilibrium epitaxial Sn-rich group IV SiGeSn ternary semiconductors. Different atom probe statistical analysis tools including frequency distribution analysis, partial radial distribution functions, and nearest neighbor analysis were employed in order to evaluate and compare the behavior of the three elements to their spati…
Nanoscale L12-type ordered structures are widely used in face-centred cubic (FCC) alloys to exploit their hardening capacity and thereby improve mechanical properties. These fine-scale particles are typically fully coherent with matrix with the same atomic configuration disregarding chemical species, which makes them challenging to be characterized. Spatial distribution maps (SDMs) are used to probe local order by interrogating the three-dimensional (3D) distribution of atoms within reconstructed atom probe tomography (APT) data. However, it is almost impossible to manually analyse the complet…
A 4D-STEM Tomographic Framework Assisted by Object Tracking for Nanoparticle Structure Determination
EMAT, Department of Physics, University of Antwerp（安特卫普大学物理系）；CRISMAT, Normandie Université, ENSICAEN, UNICAEN, CNRS UMR 6508（诺曼底大学、ENSICAEN、UNICAEN、法国国家科学研究中心UMR 6508）；Department of Chemistry, KU Leuven（荷语鲁汶大学化学系）
Many biological materials exhibit a multiscale porosity with small, mostly nanoscale pores as well as large, macroscopic capillaries to simultaneously achieve optimized mass transport capabilities and lightweight structures with large inner surfaces. Realizing such a hierarchical porosity in artificial materials necessitates often sophisticated and expensive top-down processing that limits scalability. Here we present an approach that combines self-organized porosity based on metal-assisted chemical etching (MACE) with photolithographically induced macroporosity for the synthesis of single-cry…
Compositional Metrology of Atom Probe Applied to non-Metallic Materials
Università degli Studi di Padova（帕多瓦大学）；Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Legnaro（意大利国家核物理研究所，莱尼亚罗国家实验室）；CNR-ISMN, Istituto per lo Studio dei Materiali Nanostrutturati（意大利国家研究委员会纳米结构材料研究所）；University of Rouen Normandie, INSA Rouen Normandie, CNRS, Groupe de Physique des Matériaux UMR 6634（鲁昂诺曼底大学，鲁昂诺曼底国立应用科学学院，法国国家科学研究中心，材料物理小组）
