J. Houard

Correlation of microphotoluminescence spectroscopy, scanning transmission electron microscopy, and atom probe tomography on a single nano-object containing an InGaN/GaN multiquantum well system.

A single nanoscale object containing a set of InGaN/GaN nonpolar multiple-quantum wells has been analyzed by microphotoluminescence spectroscopy (μPL), high-resolution scanning transmission electron microscopy (HR-STEM) and atom probe tomography (APT). The correlated measurements constitute a rich and coherent set of data supporting the interpretation that the observed μPL narrow emission lines, polarized perpendicularly to the crystal c-axis and with energies in the interval 2.9-3.3 eV, are related to exciton states localized in potential minima induced by the irregular 3D In distribution within the quantum well (QW) planes. This novel method opens up interesting perspectives, as it will be possible to apply it on a wide class of quantum confining emitters and nano-objects.

Quantitative analysis of doped/undoped ZnO nanomaterials using laser assisted atom probe tomography: Influence of the analysis parameters

In the last decade, atom probe tomography has become a powerful tool to investigate semiconductor and insulator nanomaterials in microelectronics, spintronics, and optoelectronics. In this paper, we report an investigation of zinc oxide nanostructures using atom probe tomography. We observed that the chemical composition of zinc oxide is strongly dependent on the analysis parameters used for atom probe experiments. It was observed that at high laser pulse energies, the electric field at the specimen surface is strongly dependent on the crystallographic directions. This dependence leads to an inhomogeneous field evaporation of the surface atoms, resulting in unreliable measurements. We show that the laser pulse energy has to be well tuned to obtain reliable quantitative chemical composition measurements of undoped and doped ZnO nanomaterials.

Conditions to cancel the laser polarization dependence of a subwavelength tip

Using laser assisted atom probe tomography, we investigate the polarization dependence of the absorption coefficient of a subwavelength Al tip illuminated by an ultrashort laser pulse. In practice, we find an equilibrium condition as a function of the incident wavelength for which the atom evaporation rate becomes independent of the wave polarization. It is experimentally shown that this condition only depends on the ratio between the tip radius and the laser wavelength. Furthermore, our calculations demonstrate that a transverse local plasmon polariton mode can be resonantly excited at the tip apex.

Statistical nanoscale study of localised radiative transitions in GaN/AlGaN quantum wells and AlGaN epitaxial layers

Compositional disorder has important consequences on the optical properties of III-nitride ternary alloys. In AlGaN epilayers and AlGaN-based quantum heterostructures, the potential fluctuations induced by such disorder lead to the localisation of carriers at low temperature, which affects their transition energies. Using the correlations between micro-photoluminescence, scanning transmission electron microscopy and atom probe tomography we have analysed the optical behaviour of Al0.25Ga0.75N epilayers and that of GaN/AlGaN quantum wells, and reconstructed in three dimensions the distribution of chemical species with sub-nanometre spatial resolution. These composition maps served as the basis for the effective mass calculation of electrons and holes involved in radiative transitions. Good statistical predictions were subsequently obtained for the above-mentioned transition and localisation energies by establishing a link with their microstructural properties.

Three-dimensional atomic-scale investigation of ZnO-MgxZn1−xO m-plane heterostructures

The structural, compositional, and optical properties of ZnO/MgxZn1−xO m-plane heterostructures are investigated using scanning transmission electron microscopy, laser-assisted atom probe tomography, and micro-photoluminescence. Coupled with electron tomography, atom probe tomography is currently the only technique providing a 3D reconstruction of the position of the atoms of a nanoscale specimen with their chemical nature. The multi-quantum well system investigated exhibits a V-groove grating profile along the a-axis accompanied by the formation of Zn- and Mg-enriched regions corresponding to the edges pointing towards the substrate and towards the upper surface, respectively. The optical signature of these heterostructures has been investigated by performing micro-photoluminescence on atom probe tip specimens. Effective mass calculations based on the 3D microscopy data indicate that the quantum well geometry and barrier composition yield a localization of hole states at the bottom of the V-groove.

Antenna effect in laser assisted atom probe tomography: How the field emitter aspect ratio can enhance atomic scale imaging

In this Letter, we show that, in contrast to what is generally admitted in laser assisted atom probe, it is possible to probe a tip under optimal analysis conditions using a single wavelength. We show that the field emitter geometry can be adjusted to the wavelength of the femtosecond laser pulses used to trigger the evaporation by taking into account the optical and thermal properties of the material. The resulting enhanced absorption at the tip apex generates an ultrafast ion emission leading to a surprisingly high mass resolving power and signal over noise ratio on materials having a bad thermal diffusivity. This antenna effect is discussed based on theoretical considerations and a modeling of the laser-tip interaction. It is then demonstrated though experimental results obtained on different specimen geometries.

Carrier Localization in GaN/AlN Quantum Dots As Revealed by Three-Dimensional Multimicroscopy

The localization of carrier states in GaN/AlN self-assembled quantum dots (QDs) is studied by correlative multimicroscopy relying on microphotoluminescence, electron tomography, and atom probe tomography (APT). Optically active field emission tip specimens were prepared by focused ion beam from an epitaxial film containing a stack of quantum dot layers and analyzed with different techniques applied subsequently on the same tip. The transition energies of single QDs were calculated in the framework of a 6-bands k.p model on the basis of APT and scanning transmission electron microscopy characterization showing that a good agreement between experimental and calculated energies can be obtained, overcoming the limitations of both techniques. The results indicate that holes effectively localize at interface fluctuations at the bottom of the QD, decreasing the extent of the wave function and the band-to-band transition energy. They also represent an important step toward the correlation of the three-dimensional atomic scale structural information with the optical properties of single light emitters based on quantum confinement.

Field-Dependent Measurement of GaAs Composition by Atom Probe Tomography

The composition of GaAs measured by laser-assisted atom probe tomography may be inaccurate depending on the experimental conditions. In this work, we assess the role of the DC field and the impinging laser energy on such compositional bias. The DC field is found to have a major influence, while the laser energy has a weaker one within the range of parameters explored. The atomic fraction of Ga may vary from 0.55 at low-field conditions to 0.35 at high field. These results have been interpreted in terms of preferential evaporation of Ga at high field. The deficit of As is most likely explained by the formation of neutral As complexes either by direct ejection from the tip surface or upon the dissociation of large clusters. The study of multiple detection events supports this interpretation.

Compositional accuracy of atom probe tomography measurements in GaN: Impact of experimental parameters and multiple evaporation events

A systematic study of the biases occurring in the measurement of the composition of GaN by Atom Probe Tomography was carried out, in which the role of surface electric field and laser pulse intensity has been investigated. Our data confirm that the electric field is the main factor influencing the measured composition, which exhibits a deficiency of N at low field and a deficiency of Ga at high field. The deficiency of Ga at high field is interpreted in terms of preferential evaporation of Ga. The detailed analysis of multiple evaporation events reveals that the measured composition is not affected by pile-up phenomena occurring in detection system. The analysis of correlation histograms yields the signature of the production of neutral N2 due to the dissociation of GaN32+ ions. However, the amount of N2 neutral molecules that can be detected cannot account for the N deficiency found at low field. Therefore, we propose that further mechanisms of neutral N evaporation could be represented by dissociation reactions such as GaN+→ Ga++ N and GaN2+→ Ga2++ N.

Optical Contactless Measurement of Electric Field-Induced Tensile Stress in Diamond Nanoscale Needles

The application of a high electrostatic field at the apex of monocrystalline diamond nanoscale needles induces an energy splitting of the photoluminescence lines of color centers. In particular, the splitting of the zero-phonon line of the neutral nitrogen-vacancy complex (NV0) has been studied within a laser-assisted tomographic atom probe equipped with an in situ microphotoluminescence bench. The measured quadratic dependence of the energy splitting on the applied voltage corresponds to the stress generated on the metal-like apex surface by the electrostatic field. Tensile stress up to 7 GPa has thus been measured in the proximity of the needle apex. Furthermore, the stress scales along the needle shank inversely proportionally to its axial cross section. We demonstrate thus a method for contactless piezo-spectroscopy of nanoscale systems by electrostatic field regulation for the study of their mechanical properties. These results also provide an experimental confirmation to the models of dielectrics surface metallization under high electrostatic field.