Cross-sectional Scanning Tunneling Microscopy Research Articles

Built-in Electric Field Induced Mechanical Property Change at the Lanthanum Nickelate/Nb-doped Strontium Titanate Interfaces.

The interactions between electric field and the mechanical properties of materials are important for the applications of microelectromechanical and nanoelectromechanical systems, but relatively unexplored for nanoscale materials. Here, we observe an apparent correlation between the change of the fractured topography of Nb-doped SrTiO3 (Nb:STO) within the presence of a built-in electric field resulting from the Schottky contact at the interface of a metallic LaNiO3 thin film utilizing cross-sectional scanning tunneling microscopy and spectroscopy. The change of the inter-atomic bond length mechanism is argued to be the most plausible origin. This picture is supported by the strong-electric-field-dependent permittivity in STO and the existence of the dielectric dead layer at the interfaces of STO with metallic films. These results provided direct evidence and a possible mechanism for the interplay between the electric field and the mechanical properties on the nanoscale for perovskite materials.

Mn doped InSb studied at the atomic scale by cross-sectional scanning tunneling microscopy

We present an atomically resolved study of metal-organic vapor epitaxy grown Mn doped InSb. Both topographic and spectroscopic measurements have been performed by cross-sectional scanning tunneling microscopy (STM). The measurements on the Mn doped InSb samples show a perfect crystal structure without any precipitates and reveal that Mn acts as a shallow acceptor. The Mn concentration of the order of ∼1020 cm−3 obtained from the cross-sectional STM data compare well with the intended doping concentration. While the pair correlation function of the Mn atoms showed that their local distribution is uncorrelated beyond the STM resolution for observing individual dopants, disorder in the Mn ion location giving rise to percolation pathways is clearly noted. The amount of clustering that we see is thus as expected for a fully randomly disordered distribution of the Mn atoms and no enhanced clustering or second phase material was observed.

One-Dimensional Nature of InAs/InP Quantum Dashes Revealed by Scanning Tunneling Spectroscopy.

We report on low-temperature cross-sectional scanning tunneling microscopy and spectroscopy on InAs(P)/InGaAsP/InP(001) quantum dashes, embedded in a diode-laser structure. The laser active region consists of nine InAs(P) quantum dash layers separated by the InGaAsP quaternary alloy barriers. The effect of the p-i-n junction built-in potential on the band structure has been evidenced and quantified on large-scale tunneling spectroscopic measurements across the whole active region. By comparing the tunneling current onset channels, a consistent energy shift has been measured in successive quantum dash or barrier layers, either for the ground state energy of similar-sized quantum dashes or for the conduction band edge of the barriers, corresponding to the band-bending slope. The extracted values are in good quantitative agreement with the theoretical band structure calculations, demonstrating the high sensitivity of this spectroscopic measurement to probe the electronic structure of individual nanostructures, relative to local potential variations. Furthermore, by taking advantage of the potential gradient, we compared the local density of states over successive quantum dash layers. We observed that it does not vanish while increasing energy, for any of the investigated quantum dashes, in contrast to what would be expected for discrete level zero-dimensional (0D) structures. In order to acquire further proof and fully address the open question concerning the quantum dash dimensionality nature, we focused on individual quantum dashes obtaining high-energy-resolution measurements. The study of the local density of states clearly indicates a 1D quantum-wirelike nature for these nanostructures whose electronic squared wave functions were subsequently imaged by differential conductivity mapping.

Strong charge-carrier localization in InAs/GaAs submonolayer stacks prepared by Sb-assisted metalorganic vapor-phase epitaxy

Stacks of InAs/GaAs submonolayer depositions forming small In-rich islands are interesting for efficient optoelectronic applications due to the high areal density of localization centers and their fast carrier relaxation. The electronic confinement of charge carriers in InAs/GaAs submonolayers can be influenced by adding Sb during growth. Eight-band $k\ifmmode\cdot\else\textperiodcentered\fi{}p$ simulations show that electrons and holes experience a different localization depending on where the Sb is incorporated into the submonolayer stacks. Samples grown with metalorganic vapor-phase epitaxy show sharp interfaces between InAs(Sb)/GaAs submonolayers and the surrounding matrix material in transmission electron microscopy and x-ray diffraction measurements. Cross-sectional scanning tunneling microscopy shows the formation of In-rich agglomerations as well as a slight clustering of Sb atoms. Temperature-dependent photoluminescence and spatially resolved cathodoluminescence show evidence for strong electronic confinement whose depth is controlled by the Sb amount.

Local density of states at metal-semiconductor interfaces: an atomic scale study.

We investigate low temperature grown, abrupt, epitaxial, nonintermixed, defect-free n-type and p-type Fe/GaAs(110) interfaces by cross-sectional scanning tunneling microscopy and spectroscopy with atomic resolution. The probed local density of states shows that a model of the ideal metal-semiconductor interface requires a combination of metal-induced gap states and bond polarization at the interface which is nicely corroborated by density functional calculations. A three-dimensional finite element model of the space charge region yields a precise value for the Schottky barrier height.

Monolayer-by-monolayer compositional analysis of InAs/InAsSb superlattices with cross-sectional STM

We use cross-sectional scanning tunneling microscopy (STM) to reconstruct the monolayer-by-monolayer composition profile across a representative subset of MBE-grown InAs/InAsSb superlattice layers and find that antimony segregation frustrates the intended compositional discontinuities across both antimonide-on-arsenide and arsenide-on-antimonide heterojunctions. Graded, rather than abrupt, interfaces are formed in either case. We likewise find that the incorporated antimony per superlattice period varies measurably from beginning to end of the multilayer stack. Although the intended antimony discontinuities predict significant discrepancies with respect to the experimentally observed high-resolution x-ray diffraction spectrum, dynamical simulations based on the STM-derived profiles provide an excellent quantitative match to all important aspects of the x-ray data.

Structural, electronic, and magnetic properties of single MnAs nanoclusters in GaAs

MnAs nanoclusters in GaAs were investigated with cross-sectional scanning tunneling microscopy. The topographic images reveal that the small clusters have the same zinc-blende crystal structure as the host material, while the larger clusters grow in a hexagonal crystal phase. The initial Mn concentration during molecular beam epitaxy growth has a strong influence on the size of the clusters that form during the annealing step. The local band structure of a single MnAs cluster is probed with scanning tunneling spectroscopy, revealing a Coulomb blockade effect that correlates with the size of the cluster. With a spin-sensitive tip, for the smaller clusters, superparamagnetic switching between two distinct states is observed at T = 77 K. The larger clusters do not change their magnetic state at this temperature, i.e., they are superferromagnetic, confirming that they are responsible for the ferromagnetic behavior of this material at room-temperature.

Composition profiling of GaAs/AlGaAs quantum dots grown by droplet epitaxy

Droplet epitaxy (DE) is a growth method which can create III-V quantum dots (QDs) whose optoelectronic properties can be accurately controlled through the crystallisation conditions. In this work, GaAs/AlGaAs DE-QDs have been analyzed with the complimentary techniques of cross-sectional scanning tunneling microscopy and atom probe tomography. Structural details and a quantitative chemical analysis of QDs of different sizes are obtained. Most QDs were found to be pure GaAs, while a small proportion exhibited high intermixing caused by a local etching process. Large QDs with a high aspect ratio were observed to have an Al-rich crown above the GaAs QD. This structure is attributed to differences in mobility of the cations during the capping phase of the DE growth.

Influence of Sb incorporation on InGaAs(Sb)N/GaAs band alignment

We have investigated the influence of Sb incorporation on the effective band gaps and band offsets at InGaAs(Sb)N/GaAs interfaces grown by metalorganic vapor phase epitaxy. Cross-sectional scanning tunneling microscopy and spectroscopy reveal 1.2 eV (1.1 eV) effective band gaps of InGaAs(Sb)N alloys. At the InGaAsN/GaAs (InGaAsSbN/GaAs) interfaces, type II (type I) band offsets are observed. We discuss the relative influences of strain-induced splitting of the valence band and the incorporation of Sb on the band gaps and band offsets at InGaAsN/GaAs and InGaAsSbN/GaAs interfaces.

Atomic intermixing and interface roughness in short-period InAs/GaSb superlattices for infrared photodetectors

A set of advanced characterization methods, including high-resolution X-ray diffraction (measurements and simulations), cross-sectional scanning tunneling microscopy, and high-angle annular dark-field scanning transmission electron microscopy is applied to quantify the interface roughness and atomic intermixing (in both cation and anion sub-lattices) in short period (6–7 nm) InAs/GaSb superlattices intended for mid-wavelength (M) and long-wavelength (L) infrared detectors. The undesired atomic intermixing and interface roughness in the L-samples were found to be considerably lower than in the M-samples. In all specimens, anion intermixing is much higher than that in the cation sub-lattice. Possible origins of these findings are discussed.

Height stabilization of GaSb/GaAs quantum dots by Al-rich capping

GaSb quantum dots (QDs) in a GaAs matrix are investigated with cross-sectional scanning tunneling microscopy (X-STM) and photoluminescence (PL). We observe that Al-rich capping materials prevent destabilization of the nanostructures during the capping stage of the molecular beam epitaxy (MBE) growth process and thus preserves the QD height. However, the strain induced by the absence of destabilization causes many structural defects to appear around the preserved QDs. These defects originate from misfit dislocations near the GaSb/GaAs interface and extend into the capping layer as stacking faults. The lack of a red shift in the QD PL suggests that the preserved dots do not contribute to the emission spectra. We suggest that a better control over the emission wavelength and an increase of the PL intensity is attainable by growing smaller QDs with an Al-rich overgrowth.

Meandering of overgrown v-shaped defects in epitaxial GaN layers

The meandering of v-shaped defects in GaN(0001) epitaxial layers is investigated by cross-sectional scanning tunneling microscopy. The spatial position of v-shaped defects is mapped on (101¯0) cleavage planes using a dopant modulation, which traces the overgrown growth front. Strong lateral displacements of the apex of the v-shaped defects are observed. The lateral displacements are suggested to be induced by the meandering of threading dislocations present in the v-shaped defects. The meandering of the dislocation is attributed to interactions with inhomogeneous strain fields.

InAs quantum dot morphology after capping with In, N, Sb alloyed thin films

Using a thin capping layer to engineer the structural and optical properties of InAs/GaAs quantum dots (QDs) has become common practice in the last decade. Traditionally, the main parameter considered has been the strain in the QD/capping layer system. With the advent of more exotic alloys, it has become clear that other mechanisms significantly alter the QD size and shape as well. Larger bond strengths, surfactants, and phase separation are known to act on QD properties but are far from being fully understood. In this study, we investigate at the atomic scale the influence of these effects on the morphology of capped QDs with cross-sectional scanning tunneling microscopy. A broad range of capping materials (InGaAs, GaAsSb, GaAsN, InGaAsN, and GaAsSbN) are compared. The QD morphology is related to photoluminescence characteristics.

Magnetic anisotropy of single Mn acceptors in GaAs in an external magnetic field

We investigate the effect of an external magnetic field on the physical properties of the acceptor hole states associated with single Mn acceptors placed near the (110) surface of GaAs. Cross-sectional scanning tunneling microscopy images of the acceptor local density of states (LDOS) show that the strongly anisotropic hole wave function is not significantly affected by a magnetic field up to 6 T. These experimental results are supported by theoretical calculations based on a tight-binding model of Mn acceptors in GaAs. For Mn acceptors on the (110) surface and the subsurfaces immediately underneath, we find that an applied magnetic field modifies significantly the magnetic anisotropy landscape. However, the acceptor hole wave function is strongly localized around the Mn and the LDOS is quite independent of the direction of the Mn magnetic moment. On the other hand, for Mn acceptors placed on deeper layers below the surface, the acceptor hole wave function is more delocalized and the corresponding LDOS is much more sensitive on the direction of the Mn magnetic moment. However, the magnetic anisotropy energy for these magnetic impurities is large (up to 15 meV), and a magnetic field of 10 T can hardly change the landscape and rotate the direction of the Mn magnetic moment away from its easy axis. We predict that substantially larger magnetic fields are required to observe a significant field dependence of the tunneling current for impurities located several layers below the GaAs surface.

Influence of GaAs surface termination on GaSb/GaAs quantum dot structure and band offsets

We have investigated the influence of GaAs surface termination on the nanoscale structure and band offsets of GaSb/GaAs quantum dots (QDs) grown by molecular-beam epitaxy. Transmission electron microscopy reveals both coherent and semi-coherent clusters, as well as misfit dislocations, independent of surface termination. Cross-sectional scanning tunneling microscopy and spectroscopy reveal clustered GaSb QDs with type I band offsets at the GaSb/GaAs interfaces. We discuss the relative influences of strain and QD clustering on the band offsets at GaSb/GaAs interfaces.

Visualizing short-range charge transfer at the interfaces between ferromagnetic and superconducting oxides

The interplay between antagonistic superconductivity and ferromagnetism has been a interesting playground to explore the interaction between competing ground states. Although this effect in systems of conventional superconductors is better understood, the framework of the proximity effect at complex-oxide-based superconductor/ferromagnet interfaces is not so clear. The main difficulty originates from the lack of experimental tools capable of probing the interfaces directly with high spatial resolution. Here we harness cross-sectional scanning tunnelling microscopy and spectroscopy together with atomic-resolution electron microscopy to understand the buried interfaces between cuprate and manganite layers. The results show that the fundamental length scale of the electronic evolution between YBa2Cu3O(7-δ) (YBCO) and La2/3Ca1/3MnO3 (LCMO) is confined to the subnanometre range. Our findings provide a complete and direct microscopic picture of the electronic transition across the YBCO/LCMO interfaces, which is an important step towards understanding the competition between ferromagnetism and superconductivity in complex-oxide heterostructures.

Evidence of deep traps in overgrown v-shaped defects in epitaxial GaN layers

The geometric and electronic structure of overgrown v-shaped defects in GaN epitaxial layers are investigated by cross-sectional scanning tunneling microscopy and spectroscopy. The v-defects are found to be hexagonal pit structures delimited by six {112¯2} planes. The electronic properties are inhomogeneous. In some areas the center of the v-defects exhibits a strongly inhibited tunneling current, indicating the presence of deep traps.

The structural, electronic and optical properties of GaSb/GaAs nanostructures for charge-based memory

The potential for GaSb nanostructures embedded in GaAs to operate as charge-based memory elements at room temperature is introduced and explored. Cross-sectional scanning-tunnelling microscopy is employed to directly probe and optimize the growth of nanostructures by molecular beam epitaxy. The results of structural analysis are combined with electrical measurements made with deep-level transient spectroscopy, showing excellent agreement with theoretical calculations which model the electronic structure of the nanostructures using 8-band k·p theory. Hole-localization energies exceeding 600 meV in quantum dots and near-100% material contrast between GaSb-rich quantum rings (QRs) and the surrounding GaAs matrix are revealed (no intermixing). Optical measurements confirm the depth of the hole localization, and demonstrate substantially lower inhomogeneous broadening than has previously been reported. Multiple peaks are partially resolved in ensemble photoluminescence of GaSb/GaAs QRs, and are attributed to charge states from discrete numbers of confined holes.

Quantification of atomic intermixing in short-period InAs/GaSb superlattices for infrared photodetectors

Cross-sectional scanning tunneling microscopy (XSTM) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) are applied for characterizing the MBE-grown short-period InAs/GaSb superlattices for mid- and long-wavelength infrared detection. The focus of this study is on atomic intermixing in close proximity to the interfaces, which is a key issue for device performance. HAADF-STEM permits visualization of the anion-cation dumbbells in individual sub-layers and is even capable to resolve anions and cations separated by 0.15 nm within a dumbbell. On this basis, the interfacial width is extracted with high accuracy. XSTM technique allows us direct counting of certain kinds of atoms within atomic rows, which sheds light on compositional fluctuations and isovalent atomic intermixing. Both methods reveal rather abrupt interfaces with InAs-on-GaSb interfaces being slightly wider than GaSb-on-InAs interfaces. According to HAADF-STEM, in the set of investigated samples, the 90%-to-10% interface width is confined within 2.6–4.4 monolayers (0.8–1.3 nm). In all the samples studied, XSTM analysis showed some residual concentration (on the level of a few atomic percent) of Sb atoms in the middle of the InAs sub-layers, as a result of As/Sb substitutions during growth. The level of intermixing is diminishing with increasing the thickness of individual InAs layers.

Atomic-Scale Interfacial Band Mapping across Vertically Phased-Separated Polymer/Fullerene Hybrid Solar Cells

Using cross-sectional scanning tunneling microscope (XSTM) with samples cleaved in situ in an ultrahigh vacuum chamber, this study demonstrates the direct visualization of high-resolution interfacial band mapping images across the film thickness in an optimized bulk heterojunction polymer solar cell consisting of nanoscale phase segregated blends of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM). We were able to achieve the direct observation of the interfacial band alignments at the donor (P3HT)-acceptor (PCBM) interfaces and at the interfaces between the photoactive P3HT:PCBM blends and the poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) anode modification layer with an atomic-scale spatial resolution. The unique advantage of using XSTM to characterize polymer/fullerene bulk heterojunction solar cells allows us to explore simultaneously the quantitative link between the vertical morphologies and their corresponding local electronic properties. This provides an atomic insight of interfacial band alignments between the two opposite electrodes, which will be crucial for improving the efficiencies of the charge generation, transport, and collection and the corresponding device performance of polymer solar cells.