arXiv subjects

Ryan B. Lewis

Publications and source records attributed to Ryan B. Lewis.

At least 19 recordsLinked to original sources

arXiv2026

Spontaneous Nanopatterning and Strain Relaxation in SiGe Layers Grown by Oxidative Solid Phase Epitaxy

The wafer-scale monolithic integration of III-V materials on Si would lead to revolutionary optoelectronic hardware for data, computing and other applications. However, heteroepitaxy of III-Vs on Si requires overcoming the large lattice and thermal mismatches between the materials and reducing threading dislocations densities. In this work, we explore the oxidative solid phase epitaxy (SPE) of Ge+ implanted Si(111) to form ultra-thin strain-relieving SiGe metamorphic buffer layers for heteroepitaxy on Si. The SPE process is shown to result in a nanopatterning of the Ge concentration variation across the sample surface, visible by scanning and transmission electron microscopy (SEM and TEM). The concentration patterning is the result of a hexagonal network of Shockley partial dislocations at the SiGe/Si interface. Analyzing the pattern spacing observed by SEM is demonstrated as an easy, non-destructive method for obtaining the local strain state of SiGe layers. This work is important for engineering ultra-thin SiGe metamorphic buffer layers for III-V optoelectronics heteroepitaxy on the silicon platform.

cond-mat.mtrl-sci↗

arXiv2025

Electron Microscopy Study of Core-Shell Nanowire Bending and Twisting

The spontaneous bending of core-shell nanowires through asymmetric shell deposition has implications for sensors, enabling both parallel fabrication and creating advantageous out-of-plane nanowire sensor geometries. This study investigates the impact of shell deposition geometry on the shell distribution and bending of GaAs-InP core-shell nanowires. Scanning and transmission electron microscopy methods are employed to quantify nanowire twisting and bending. A practical analytical electron tomography reconstruction technique is developed for characterizing the nanowire shell distribution, which utilizes the hexagonal nanowire shape to reconstruct two-dimensional cross-sections along the nanowire length. The study reveals that the orientation of the phosphorus beam with respect to the nanowire side facets induces significant variations in nanowire bending and twisting. The findings demonstrate the important role of crystallographic orientation during core-shell nanowire synthesis for engineering the shape of bent nanowire sensors.

physics.app-ph↗

arXiv2024

Atom probe composition and in situ electronic structure of epitaxial quantum dot ensembles

Dense arrays of semiconductor quantum dots are currently employed in highly efficient quantum dot lasers for data communications and other applications. Traditionally, the electronic properties of such quantum nanostructures have been treated as isolated objects, with the degree of hybridization between neighboring quantum dots and the wetting layer left unexplored. Here, we use atom probe tomography and transmission electron microscopy to uncover the three-dimensional composition profile of a high-density ensemble of epitaxial InAs/GaAs quantum dots. The sub-nanometer compositional data is used to construct the 3D local band structure and simulate the electronic eigenstates within the dense quantum dot ensemble using finite element method. This in situ electronic simulation reveals a high degree of hybridization between neighboring quantum dots and the wetting layer, in stark contrast to the usual picture of isolated quantum nanostructures. The simulated transition energies are compared with low temperature photoluminescence. This work has important applications for quantum dot laser design and paves the way to engineering ensemble effects in quantum dot lasers and other quantum nanostructures.

cond-mat.mes-hall↗

arXiv2024

Ultra-thin strain-relieving Si$_{1-x}$Ge$_x$ layers enabling III-V epitaxy on Si

The explosion of artificial intelligence, possible end of Moore's law, dawn of quantum computing and continued exponential growth of data communications traffic have brought new urgency to the need for laser integration on the diversified Si platform. While diode lasers on III-V platforms have long powered internet data communications and other optoelectronic technologies, direct integration with Si remains problematic. A paradigm-shifting solution requires exploring new and unconventional materials and integration approaches. In this work, we show that a sub-10-nm ultra-thin Si$_{1-x}$Ge$_x$ buffer layer fabricated by an oxidative solid-phase epitaxy process can facilitate extraordinarily efficient strain relaxation. The Si$_{1-x}$Ge$_x$ layer is formed by ion implanting Ge into Si(111) and selectively oxidizing Si atoms in the resulting ion-damaged layer, precipitating a fully strain-relaxed Ge-rich layer between the Si substrate and surface oxide. The efficient strain relaxation results from the high oxidation temperature, producing a periodic network of dislocations at the substrate interface, coinciding with modulations of the Ge content in the Si$_{1-x}$Ge$_x$ layer and indicating the presence of defect-mediated diffusion of Si through the layer. The epitaxial growth of high-quality GaAs is demonstrated on this ultra-thin Si$_{1-x}$Ge$_x$ layer, demonstrating a promising new pathway for integrating III-V lasers directly on the Si platform.

cond-mat.mtrl-sci↗

arXiv2023

Phosphorus-Controlled Nanoepitaxy in the Asymmetric Growth of GaAs-InP Core-Shell Bent Nanowires

Breakthroughs extending nanostructure engineering beyond what is possible with current fabrication techniques will be crucial for enabling next-generation nanotechnologies. Nanoepitaxy of strain-engineered bent nanowire heterostructures presents a promising platform for realizing bottom-up and scalable fabrication of nanowire devices. The synthesis of these structures requires the selective asymmetric deposition of lattice-mismatched shells-a complex growth process which is not well understood. We present the nanoepitaxial growth of GaAs-InP core-shell bent nanowires and connecting nanowire pairs to form nano-arches. Compositional analysis of nanowire cross-sections reveals the critical role of adatom diffusion in the nanoepitaxial growth process, which leads to two distinct growth regimes: indium-diffusion limited growth and phosphorous-limited growth. The highly controllable phosphorous-limited growth mode is employed to synthesize connected nanowire pairs and quantify the role of flux shadowing on the shell growth process. These results provide important insight into three-dimensional nanoepitaxy and enable new possibilities for nanowire device fabrication.

physics.app-ph↗

arXiv2023

Bismuth surfactant-enhanced III-As epitaxy on GaAs(111)A

Quantum dot (QD) growth on high ($c_{3v}$) symmetry GaAs{111} surfaces holds promise for efficient entangled photon sources. Unfortunately, homoepitaxy on GaAs{111} surfaces suffers from surface roughness/defects and InAs deposition does not natively support Stranski-Krastanov (SK) QD growth. Surfactants have been identified as effective tools to alter the epitaxial growth process of III-V materials, however, their use remains unexplored on GaAs{111}. Here, we investigate Bi as a surfactant in III-As molecular beam epitaxy (MBE) on GaAs(111)A substrates, demonstrating that Bi can eliminate surface defects/hillocks in GaAs and (Al,Ga)As layers, yielding atomically-smooth hillock-free surfaces with RMS roughness values as low as 0.13 nm. Increasing Bi fluxes are found to result in smoother surfaces and Bi is observed to increase adatom diffusion. The Bi surfactant is also shown to trigger a morphological transition in InAs/GaAs(111)A films, directing the 2D InAs layer to rearrange into 3D nanostructures, which are promising candidates for high-symmetry quantum dots. The desorption activation energy ($U_{Des}$) of Bi on GaAs(111)A was measured by reflection high energy electron diffraction (RHEED), yielding $U_{Des}$ = 1.7 $\pm$ 0.4 eV. These results illustrate the potential of Bi surfactants on GaAs(111)A and will help pave the way for GaAs(111)A as a platform for technological applications including quantum photonics.

cond-mat.mtrl-sci↗

arXiv2022

Carrier Recombination in Highly Uniform and Phase-Pure GaAs/(Al,Ga)As Core/Shell Nanowire Arrays on Si(111): Mott Transition and Internal Quantum Efficiency

GaAs-based nanowires are among the most promising candidates for realizing a monolithical integration of III-V optoelectronics on the Si platform. To realize their full potential for applications as light absorbers and emitters, it is crucial to understand their interaction with light governing the absorption and extraction efficiency, as well as the carrier recombination dynamics determining the radiative efficiency. Here, we study the spontaneous emission of zincblende GaAs/(Al,Ga)As core/shell nanowire arrays by $μ$-photoluminescence spectroscopy. These ordered arrays are synthesized on patterned Si(111) substrates using molecular beam epitaxy, and exhibit an exceptionally low degree of polytypism for interwire separations exceeding a critical value. We record emission spectra over more than five orders of excitation density for both steady-state and pulsed excitation to identify the nature of the recombination channels. An abrupt Mott transition from excitonic to electron-hole-plasma recombination is observed, and the corresponding Mott density is derived. Combining these experiments with simulations and additional direct measurements of the external quantum efficiency using a perfect diffuse reflector as reference, we are able to extract the internal quantum efficiency as a function of carrier density and temperature as well as the extraction efficiency of the nanowire array. The results vividly document the high potential of GaAs/(Al,Ga)As core/shell nanowires for efficient light emitters integrated on the Si platform. Furthermore, the methodology established in this work can be applied to nanowires of any other materials system of interest for optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2021

Bending of core-shell nanowires by asymmetric shell deposition

Freestanding semiconductor nanowires have opened up new possibilities for semiconductor devices, enabling geometries, material combinations and strain states which were not previously possible. Along these lines, spontaneous bending in asymmetric core-shell nanowire heterostructures has recently been proposed as a means to realize previously unimagined device geometries, novel strain-gradient engineering and bottom-up device fabrication. The synthesis of these nanostructures exploits the nanowire geometry and the directionality of the shell deposition process. Here, we explore the underlying mechanisms of this bending process by modeling the evolution of nanowires during asymmetric shell deposition. We show how bending can lead to dramatic local shell thickness, curvature and strain variations along the length of the nanowire, and we elucidate the dependence of shell growth and bending on parameters such as the core and shell dimensions and materials, and angle of incidence of the deposition source. In addition, deposition shadowing by neighboring nanowires is explored. We show that shadowing can easily be employed to connect nanowire pairs, which could be used to fabricate novel nanowire sensors. Model results are compared with GaAs-InP and GaAs-(Al,In)As core-shell nanowire growth experiments. These results can be used to guide future experiments and to help pave the way to bent nanowire devices.

physics.ins-det↗

arXiv2021

Drastic effect of sequential deposition resulting from flux directionality on the luminescence efficiency of nanowire shells

Core-shell nanowire heterostructures form the basis for many innovative devices. When compound nanowire shells are grown by directional deposition techniques, the azimuthal position of the sources for the different constituents in the growth reactor, substrate rotation, and nanowire self-shadowing inevitably lead to sequential deposition. Here, we uncover for In$_{0.15}$Ga$_{0.85}$As/GaAs shell quantum wells grown by molecular beam epitaxy a drastic impact of this sequentiality on the luminescence efficiency. The photoluminescence intensity of shell quantum wells grown with a flux sequence corresponding to migration enhanced epitaxy, i. e. when As and the group-III metals essentially do not impinge at the same time, is more than two orders of magnitude higher than for shell quantum wells prepared with substantially overlapping fluxes. Transmission electron microscopy does not reveal any extended defects explaining this difference. Our analysis of photoluminescence transients shows that co-deposition has two detrimental microscopic effects. First, a higher density of electrically active point defects leads to internal electric fields reducing the electron-hole wave function overlap. Second, more point defects form that act as nonradiative recombination centers. Our study demonstrates that the source arrangement of the growth reactor, which is of mere technical relevance for planar structures, can have drastic consequences for the materials properties of nanowire shells. We expect that this finding holds also for other alloy nanowire shells.

cond-mat.mtrl-sci↗

arXiv2020

Spatially-resolved luminescence and crystal structure of single core-shell nanowires measured in the as-grown geometry

We report on the direct correlation between the structural and optical properties of single, as-grown core-multi-shell GaAs/In$_{0.15}$Ga$_{0.85}$As/GaAs/AlAs/GaAs nanowires. Fabricated by molecular beam epitaxy on a pre-patterned Si(111) substrate, on a row of well separated nucleation sites, it was possible to access individual nanowires in the as-grown geometry. The polytype distribution along the growth axis of the nanowires was revealed by synchrotron-based nanoprobe X-ray diffraction techniques monitoring the axial 111 Bragg reflection. For the same nanowires, the spatially-resolved emission properties were obtained by cathodoluminescence hyperspectral linescans in a scanning electron microscope. Correlating both measurements, we reveal a blueshift of the shell quantum well emission energy combined with an increased emission intensity for segments exhibiting a mixed structure of alternating wurtzite and zincblende stacking compared with the pure crystal polytypes. The presence of this mixed structure was independently confirmed by cross-sectional transmission electron microscopy.

cond-mat.mes-hall↗

arXiv2019

Coaxial GaAs/(In,Ga)As dot-in-a-well nanowire heterostructures for electrically driven infrared light generation on Si in the telecommunication O band

Core-shell GaAs-based nanowires monolithically integrated on Si constitute a promising class of nanostructures that could enable light emitters for fast inter- and intrachip optical connections. We introduce and fabricate a novel coaxial GaAs/(In,Ga)As dot-in-a-well nanowire heterostructure to reach spontaneous emission in the Si transparent region, which is crucial for applications in Si photonics. Specifically, we achieve room temperature emission at 1.27 $μ$m in the telecommunication O band. The presence of quantum dots in the heterostructure is evidenced by a structural analysis based on scanning transmission electron microscopy. The spontaneous emission of these nanowire structures is investigated by cathodoluminescence and photoluminescence spectroscopy. Thermal redistribution of charge carriers to larger quantum dots explains the long wavelength emission achieved at room temperature. Finally, in order to demonstrate the feasibility of the presented nanowire heterostructures as electrically driven light emitters monolithically integrated on Si, a light emitting diode is fabricated exhibiting room-temperature electroluminescence at 1.26 $μ$m.

cond-mat.mtrl-sci↗

arXiv2019

Bismuth-surfactant-induced growth and structure of InAs/GaAs(110) quantum dots

We explore the Bi-surfactant-directed self-assembly and structure of InAs quantum dots grown on GaAs(110) by molecular beam epitaxy. The addition of a Bi flux during InAs deposition changes the InAs growth mode from two-dimensional (2D) Frank-van der Merwe to Stranski-Krastanov, resulting in the formation of three-dimensional (3D) InAs islands on the surface. Furthermore, exposing static InAs 2D layers to Bi induces a rearrangement of the strained layer into 3D islands. We explore the effect of varying the InAs thickness and Bi flux for these two growth approaches, observing a critical thickness for 3D island formation in both cases. Characterization of (110) InAs quantum dots with high-resolution transmission electron microscopy reveals that larger islands grown by the Stranski-Krastanov mode are plastically relaxed, while small islands grown by the on-demand approach are coherent. Strain relaxation along the [1-10] direction is achieved by 90 degree pure-edge dislocations with dislocation lines running along [001]. In contrast, strain relief along [001] is by 60 degree misfit dislocations. This behaviour is consistent with observations of planar (In,Ga)As/GaAs(110) layers. These results illustrate how surfactant Bi can provoke and control quantum dot formation where it normally does not occur.

cond-mat.mtrl-sci↗

arXiv2019

Axial GaAs/Ga(As,Bi) Nanowire Heterostructures

Bi-containing III-V semiconductors constitute an exciting class of metastable compounds with wide-ranging potential optoelectronic and electronic applications. However, the growth of III-V-Bi alloys requires group-III-rich growth conditions, which pose severe challenges for planar growth. In this work, we exploit the naturally-Ga-rich environment present inside the metallic droplet of a self-catalyzed GaAs nanowire to synthesize metastable GaAs/GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ axial nanowire heterostructures with high Bi contents. The axial GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ segments are realized with molecular beam epitaxy by first enriching only the vapor-liquid-solid (VLS) Ga droplets with Bi, followed by exposing the resulting Ga-Bi droplets to As$_2$ at temperatures ranging from 270 to 380$\,^{\circ}$C to precipitate GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ only under the nanowire droplets. Microstructural and elemental characterization reveals the presence of single crystal zincblende GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ axial nanowire segments with Bi contents up to (10$\pm$2)$\%$. This work illustrates how the unique local growth environment present during the VLS nanowire growth can be exploited to synthesize heterostructures with metastable compounds.

cond-mat.mtrl-sci↗

arXiv2018

Optimization of ohmic contacts to n-type GaAs nanowires

III-V nanowires are comprehensively studied because of their suitability for optoelectronic quantum technology applications. However, their small dimensions and the spatial separation of carriers from the wire surface render electrical contacting difficult. Systematically studying ohmic contact formation by diffusion to $n$-doped GaAs nanowires, we provide a set of optimal annealing parameters for Pd/Ge/Au ohmic contacts. We reproducibly achieve low specific contact resistances of $\sim2\times10^{-7}\,Ω\text{cm}^2$ at room temperature becoming an order of magnitude higher at $T\simeq4.2\,$K. We provide a phenomenological model to describe contact resistances as a function of diffusion parameters. Implementing a transfer-matrix method, we numerically study the influence of the Schottky barrier on the contact resistance. Our results indicate that contact resistances can be predicted using various barrier shapes but further insights into structural properties would require a full microscopic understanding of the complex diffusion processes.

cond-mat.mes-hall↗

arXiv2017

Diameter evolution of selective area grown Ga-assisted GaAs nanowires

We present a novel two-step approach for the selective area growth (SAG) of GaAs nanowires (NWs) by molecular beam epitaxy which has enabled a detailed exploration of the NW diameter evolution. In the first step, the growth parameters are optimized for the nucleation of vertically-oriented NWs. In the second step, the growth parameters are chosen to optimize the NW shape, allowing NWs with a thin diameter (45 nm) and an untapered morphology to be realized. This result is in contrast to the commonly observed thick, inversely tapered shape of SAG NWs. We quantify the flux dependence of radial vapour-solid (VS) growth and build a model that takes into account diffusion on the NW sidewalls to explain the observed VS growth rates. Combining this model for the radial VS growth with an existing model for the droplet dynamics at the NW top, we achieve full understanding of the diameter of NWs over their entire length and the evolution of the diameter and tapering during growth. We conclude that only the combination of droplet dynamics and VS growth results in an untapered morphology. This result enables NW shape engineering and has important implications for doping of NWs.

cond-mat.mes-hall↗

arXiv2017

Surface preparation and patterning by nano imprint lithography for the selective area growth of GaAs nanowires on Si(111)

The selective area growth of Ga-assisted GaAs nanowires (NWs) with a high vertical yield on Si(111) substrates is still challenging. Here, we explore different surface preparations and their impact on NW growth by molecular beam epitaxy. We show that boiling the substrate in ultrapure water leads to a significant improvement in the vertical yield of NWs (realizing 80%) grown on substrates patterned by electron-beam lithography (EBL). Tentatively, we attribute this improvement to a reduction in atomic roughness of the substrate in the mask opening. On this basis, we transfer our growth results to substrates processed by a technique that enables the efficient patterning of large arrays, nano imprint lithography (NIL). In order to obtain hole sizes below 50 nm, we combine the conventional NIL process with an indirect pattern transfer (NIL-IPT) technique. Thereby, we achieve smaller hole sizes than previously reported for conventional NIL and growth results that are comparable to those achieved on EBL patterned substrates.

cond-mat.mtrl-sci↗

arXiv2017

Fine structure of excitons in InAs quantum dots on GaAs(110) planar layers and nanowire facets

We investigate the optical properties of InAs quantum dots grown by molecular beam epitaxy on GaAs(110) using Bi as a surfactant. The quantum dots are synthesized on planar GaAs(110) substrates as well as on the {110} sidewall facets of GaAs nanowires. At 10 K, neutral excitons confined in these quantum dots give rise to photoluminescence lines between 1.1 and 1.4 eV. Magneto-photoluminescence spectroscopy reveals that for small quantum dots emitting between 1.3 and 1.4 eV, the electron-hole coherence length in and perpendicular to the (110) plane is on the order of 5 and 2 nm, respectively. The quantum dot photoluminescence is linearly polarized, and both binding and antibinding biexcitons are observed, two findings that we associate with the strain in the (110) plane This strain leads to piezoelectric fields and to a strong mixing between heavy and light hole states, and offers the possibility to tune the degree of linear polarization of the exciton photoluminescence as well as the sign of the binding energy of biexcitons.

cond-mat.mes-hall↗

arXiv2017

Self-assembly of InAs nanostructures on the sidewalls of GaAs nanowires directed by a Bi surfactant

Surface energies play a dominant role in the self-assembly of three dimensional (3D) nanostructures. In this letter, we show that using surfactants to modify surface energies can provide a means to externally control nanostructure self-assembly, enabling the synthesis of novel hierarchical nanostructures. We explore Bi as a surfactant in the growth of InAs on the {1-10} sidewall facets of GaAs nanowires. The presence of surface Bi induces the formation of InAs 3D islands by a process resembling the Stranski-Krastanov mechanism, which does not occur in the absence of Bi on these surfaces. The InAs 3D islands nucleate at the corners of the {1-10} facets above a critical shell thickness and then elongate along <110> directions in the plane of the nanowire sidewalls. Exploiting this growth mechanism, we realize a series of novel hierarchical nanostructures, ranging from InAs quantum dots on single {1-10} nanowire facets to zig-zag shaped nanorings completely encircling nanowire cores. Photoluminescence spectroscopy and cathodoluminescence spectral line scans reveal that small surfactant-induced InAs 3D islands behave as optically active quantum dots. This work illustrates how surfactants can provide an unprecedented level of external control over nanostructure self-assembly.

cond-mat.mes-hall↗