Single SiGe quantum dot emission deterministically enhanced in a high-Q photonic crystal resonator.

We report the resonantly enhanced radiative emission from a single SiGe quantum dot (QD), which is deterministically embedded into a bichromatic photonic crystal resonator (PhCR) at the position of its largest modal electric field by a scalable method. By optimizing our molecular beam epitaxy (MBE) growth technique, we were able to reduce the amount of Ge within the whole resonator to obtain an absolute minimum of exactly one QD, accurately positioned by lithographic methods relative to the PhCR, and an otherwise flat, a few monolayer thin, Ge wetting layer (WL). With this method, record quality (Q) factors for QD-loaded PhCRs up to Q ∼ 105 are achieved. A comparison with control PhCRs on samples containing a WL but no QDs is presented, as well as a detailed analysis of the dependence of the resonator-coupled emission on temperature, excitation intensity, and emission decay after pulsed excitation. Our findings undoubtedly confirm a single QD in the center of the resonator as a potentially novel photon source in the telecom spectral range.

Photoluminescence enhancement by deterministically site-controlled, vertically stacked SiGe quantum dots.

The Si/SiGe heterosystem would be ideally suited for the realization of complementary metal-oxide-semiconductor (CMOS)-compatible integrated light sources, but the indirect band gap, exacerbated by a type-II band offset, makes it challenging to achieve efficient light emission. We address this problem by strain engineering in ordered arrays of vertically close-stacked SiGe quantum dot (QD) pairs. The strain induced by the respective lower QD creates a preferential nucleation site for the upper one and strains the upper QD as well as the Si cap above it. Electrons are confined in the strain pockets in the Si cap, which leads to an enhanced wave function overlap with the heavy holes near the upper QD's apex. With a thickness of the Si spacer between the stacked QDs below 5 nm, we separated the functions of the two QDs: The role of the lower one is that of a pure stressor, whereas only the upper QD facilitates radiative recombination of QD-bound excitons. We report on the design and strain engineering of the QD pairs via strain-dependent Schrödinger-Poisson simulations, their implementation by molecular beam epitaxy, and a comprehensive study of their structural and optical properties in comparison with those of single-layer SiGe QD arrays. We find that the double QD arrangement shifts the thermal quenching of the photoluminescence signal at higher temperatures. Moreover, detrimental light emission from the QD-related wetting layers is suppressed in the double-QD configuration.

Single-Shot Readout of Hole Spins in Ge.

The strong atomistic spin-orbit coupling of holes makes single-shot spin readout measurements difficult because it reduces the spin lifetimes. By integrating the charge sensor into a high bandwidth radio frequency reflectometry setup, we were able to demonstrate single-shot readout of a germanium quantum dot hole spin and measure the spin lifetime. Hole spin relaxation times of about 90 µs at 500 mT are reported, with a total readout visibility of about 70%. By analyzing separately the spin-to-charge conversion and charge readout fidelities, we have obtained insight into the processes limiting the visibilities of hole spins. The analyses suggest that high hole visibilities are feasible at realistic experimental conditions, underlying the potential of hole spins for the realization of viable qubit devices.

A germanium hole spin qubit.

Holes confined in quantum dots have gained considerable interest in the past few years due to their potential as spin qubits. Here we demonstrate two-axis control of a spin 3/2 qubit in natural Ge. The qubit is formed in a hut wire double quantum dot device. The Pauli spin blockade principle allowed us to demonstrate electric dipole spin resonance by applying a radio frequency electric field to one of the electrodes defining the double quantum dot. Coherent hole spin oscillations with Rabi frequencies reaching 140 MHz are demonstrated and dephasing times of 130 ns are measured. The reported results emphasize the potential of Ge as a platform for fast and electrically tunable hole spin qubit devices.

Free-running Sn precipitates: an efficient phase separation mechanism for metastable Ge1-xSnx epilayers.

The revival of interest in Ge1-xSnx alloys with x ≥ 10% is mainly owed to the recent demonstration of optical gain in this group-IV heterosystem. Yet, Ge and Sn are immiscible over about 98% of the composition range, which renders epilayers based on this material system inherently metastable. Here, we address the temperature stability of pseudomorphic Ge1-xSnx films grown by molecular beam epitaxy. Both the growth temperature dependence and the influence of post-growth annealing steps were investigated. In either case we observe that the decomposition of epilayers with Sn concentrations of around 10% sets in above ≈230 °C, the eutectic temperature of the Ge/Sn system. Time-resolved in-situ annealing experiments in a scanning electron microscope reveal the crucial role of liquid Sn precipitates in this phase separation process. Driven by a gradient of the chemical potential, the Sn droplets move on the surface along preferential crystallographic directions, thereby taking up Sn and Ge from the strained Ge1-xSnx layer. While Sn-uptake increases the volume of the melt, single-crystalline Ge becomes re-deposited by a liquid-phase epitaxial process at the trailing edge of the droplet. This process makes phase separation of metastable GeSn layers particularly efficient at rather low temperatures.

Enhanced Telecom Emission from Single Group-IV Quantum Dots by Precise CMOS-Compatible Positioning in Photonic Crystal Cavities.

Efficient coupling to integrated high-quality-factor cavities is crucial for the employment of germanium quantum dot (QD) emitters in future monolithic silicon-based optoelectronic platforms. We report on strongly enhanced emission from single Ge QDs into L3 photonic crystal resonator (PCR) modes based on precise positioning of these dots at the maximum of the respective mode field energy density. Perfect site control of Ge QDs grown on prepatterned silicon-on-insulator substrates was exploited to fabricate in one processing run almost 300 PCRs containing single QDs in systematically varying positions within the cavities. Extensive photoluminescence studies on this cavity chip enable a direct evaluation of the position-dependent coupling efficiency between single dots and selected cavity modes. The experimental results demonstrate the great potential of the approach allowing CMOS-compatible parallel fabrication of arrays of spatially matched dot/cavity systems for group-IV-based data transfer or quantum optical systems in the telecom regime.

Arrays of Individual DNA Molecules on Nanopatterned Substrates.

Arrays of individual molecules can combine the advantages of microarrays and single-molecule studies. They miniaturize assays to reduce sample and reagent consumption and increase throughput, and additionally uncover static and dynamic heterogeneity usually masked in molecular ensembles. However, realizing single-DNA arrays must tackle the challenge of capturing structurally highly dynamic strands onto defined substrate positions. Here, we create single-molecule arrays by electrostatically adhering single-stranded DNA of gene-like length onto positively charged carbon nanoislands. The nanosites are so small that only one molecule can bind per island. Undesired adsorption of DNA to the surrounding non-target areas is prevented via a surface-passivating film. Of further relevance, the DNA arrays are of tunable dimensions, and fabricated on optically transparent substrates that enable singe-molecule detection with fluorescence microscopy. The arrays are hence compatible with a wide range of bioanalytical, biophysical, and cell biological studies where individual DNA strands are either examined in isolation, or interact with other molecules or cells.

Laser Level Scheme of Self-Interstitials in Epitaxial Ge Dots Encapsulated in Si.

Recently, it was shown that lasing from epitaxial Ge quantum dots (QDs) on Si substrates can be obtained if they are partially amorphized by Ge ion bombardment (GIB). Here, we present a model for the microscopic origin of the radiative transitions leading to enhanced photoluminescence (PL) from such GIB-QDs. We provide an energy level scheme for GIB-QDs in a crystalline Si matrix that is based on atomistic modeling with Monte Carlo (MC) analysis and density functional theory (DFT). The level scheme is consistent with a broad variety of PL experiments performed on as-grown and annealed GIB-QDs. Our results show that an extended point defect consisting of a split-[110] self-interstitial surrounded by a distorted crystal lattice of about 45 atoms leads to electronic states at the Γ-point of the Brillouin zone well below the conduction band minimum of crystalline Ge. Such defects in Ge QDs allow direct transitions of electrons localized at the split-interstitial with holes confined in the Ge QD. We identify the relevant growth and annealing parameters that will let GIB-QDs be employed as an efficient laser active medium.

Co-Immobilization of Proteins and DNA Origami Nanoplates to Produce High-Contrast Biomolecular Nanoarrays.

The biofunctionalization of nanopatterned surfaces with DNA origami nanostructures is an important topic in nanobiotechnology. An unexplored challenge is, however, to co-immobilize proteins with DNA origami at pre-determined substrate sites in high contrast relative to the nontarget areas. The immobilization should, in addition, preferably be achieved on a transparent substrate to allow ultrasensitive optical detection. If successful, specific co-binding would be a step towards stoichiometrically defined arrays with few to individual protein molecules per site. Here, we successfully immobilize with high specificity positively charged avidin proteins and negatively charged DNA origami nanoplates on 100 nm-wide carbon nanoislands while suppressing undesired adsorption to surrounding nontarget areas. The arrays on glass slides achieve unprecedented selectivity factors of up to 4000 and allow ultrasensitive fluorescence read-out. The co-immobilization onto the nanoislands leads to layered biomolecular architectures, which are functional because bound DNA origami influences the number of capturing sites on the nanopatches for other proteins. The novel hybrid DNA origami-protein nanoarrays allow the fabrication of versatile research platforms for applications in biosensing, biophysics, and cell biology, and, in addition, represent an important step towards single-molecule protein arrays.

Lasing from Glassy Ge Quantum Dots in Crystalline Si.

Semiconductor light-emitters compatible with standard Si integration technology (SIT) are of particular interest for overcoming limitations in the operating speed of microelectronic devices. Light sources based on group IV elements would be SIT-compatible, but suffer from the poor optoelectronic properties of bulk Si and Ge. Here we demonstrate that epitaxially grown Ge quantum dots (QDs) in a defect-free Si matrix show extraordinary optical properties if partially amorphized by Ge-ion bombardment (GIB). In contrast to conventional SiGe nanostructures, these QDs exhibit dramatically shortened carrier lifetimes and negligible thermal quenching of the photoluminescence (PL) up to room temperature. Microdisk resonators with embedded GIB-QDs exhibit threshold behavior as well as a superlinear increase of the integrated PL intensity with concomitant line width narrowing as the pump power increases. These findings demonstrate light amplification by stimulated emission in a fully SIT-compatible group IV nanosystem.

Burgers Vector Analysis of Vertical Dislocations in Ge Crystals by Large-Angle Convergent Beam Electron Diffraction.

By transmission electron microscopy with extended Burgers vector analyses, we demonstrate the edge and screw character of vertical dislocations (VDs) in novel SiGe heterostructures. The investigated pillar-shaped Ge epilayers on prepatterned Si(001) substrates are an attempt to avoid the high defect densities of lattice mismatched heteroepitaxy. The Ge pillars are almost completely strain-relaxed and essentially defect-free, except for the rather unexpected VDs. We investigated both pillar-shaped and unstructured Ge epilayers grown either by molecular beam epitaxy or by chemical vapor deposition to derive a general picture of the underlying dislocation mechanisms. For the Burgers vector analysis we used a combination of dark field imaging and large-angle convergent beam electron diffraction (LACBED). With LACBED simulations we identify ideally suited zeroth and second order Laue zone Bragg lines for an unambiguous determination of the three-dimensional Burgers vectors. By analyzing dislocation reactions we confirm the origin of the observed types of VDs, which can be efficiently distinguished by LACBED. The screw type VDs are formed by a reaction of perfect 60° dislocations, whereas the edge types are sessile dislocations that can be formed by cross-slips and climbing processes. The understanding of these origins allows us to suggest strategies to avoid VDs.

Photoluminescence investigation of strictly ordered Ge dots grown on pit-patterned Si substrates.

We investigate the optical properties of ordered Ge quantum dots (QDs) by means of micro-photoluminescence spectroscopy (PL). These were grown on pit-patterned Si(001) substrates with a wide range of pit-periods and thus inter QD-distances (425-3400 nm). By exploiting almost arbitrary inter-QD distances achievable in this way we are able to choose the number of QDs that contribute to the PL emission in a range between 70 and less than three QDs. This well-defined system allows us to clarify, by PL-investigation, several points which are important for the understanding of the formation and optical properties of ordered QDs. We directly trace and quantify the amount of Ge transferred from the surrounding wetting layer (WL) to the QDs in the pits. Moreover, by exploiting different pit-shapes, we reveal the role of strain-induced activation energy barriers that have to be overcome for charge carriers generated outside the dots. These need to diffuse between the energy minimum of the WL in and between the pits, and the one in the QDs. In addition, we demonstrate that the WL in the pits is already severely intermixed with Si before upright QDs nucleate, which further enhances intermixing of ordered QDs as compared to QDs grown on planar substrates. Furthermore, we quantitatively determine the amount of Ge transferred by surface diffusion through the border region between planar and patterned substrate. This is important for the growth of ordered islands on patterned fields of finite size. We highlight that the Ge WL-facets in the pits act as PL emission centres, similar to upright QDs.

Superlattice photonic crystal as broadband solar absorber for high temperature operation.

A high performance solar absorber using a 2D tantalum superlattice photonic crystal (PhC) is proposed and its design is optimized for high-temperature energy conversion. In contrast to the simple lattice PhC, which is limited by diffraction in the short wavelength range, the superlattice PhC achieves solar absorption over broadband spectral range due to the contribution from two superposed lattices with different cavity radii. The superlattice PhC geometry is tailored to achieve maximum thermal transfer efficiency for a low concentration system of 250 suns at 1500 K reaching 85.0% solar absorptivity. In the high concentration case of 1000 suns, the superlattice PhC absorber achieves a solar absorptivity of 96.2% and a thermal transfer efficiency of 82.9% at 1500 K, amounting to an improvement of 10% and 5%, respectively, versus the simple square lattice PhC absorber. In addition, the performance of the superlattice PhC absorber is studied in a solar thermophotovoltaic system which is optimized to minimize absorber re-emission by reducing the absorber-to-emitter area ratio and using a highly reflective silver aperture.

Unexpected dominance of vertical dislocations in high-misfit ge/si(001) films and their elimination by deep substrate patterning.

An innovative strategy in dislocation analysis, based on comparison between continuous and tessellated film, demonstrates that vertical dislocations, extending straight up to the surface, easily dominate in thick Ge layers on Si(001) substrates. The complete elimination of dislocations is achieved by growing self-aligned and self-limited Ge microcrystals with fully faceted growth fronts, as demonstrated by AFM extensive etch-pit counts.

Recipes for the fabrication of strictly ordered Ge islands on pit-patterned Si(001) substrates.

We identify the most important parameters for the growth of ordered SiGe islands on pit-patterned Si(001) substrates. From a multi-dimensional parameter space we link individual contributions to isolate their influence on ordered island growth. This includes the influences of: the pit size, pit depth and pit period on the Si buffer layer and subsequent Ge growth; the pit sidewall inclination on Ge island growth; the amount of Ge on island morphologies as well as the influences of the pit-size homogeneity, the pit period, the Ge growth temperature and rate on island formation. We highlight that the initial pit shape and pit size in combination with the growth conditions of the Si buffer layer should be adjusted to provide suitable preconditions for the growth of Ge islands with the desired size, composition and nucleation position. Furthermore, we demonstrate that the wetting layer between pits can play the role of a stabilizer that inhibits shape transformations of ordered islands. Thus, dislocation formation within islands can be delayed, uniform arrays of one island type can be fabricated and secondary island nucleation between pits can be impeded. These findings allow us to fabricate perfectly ordered and homogeneous Ge islands on one and the same sample, even if the pit period is varied from a few hundred nanometres to several micrometres.

Morphological evolution of Ge/Si(001) quantum dot rings formed at the rim of wet-etched pits.

We demonstrate the formation of Ge quantum dots in ring-like arrangements around predefined {111}-faceted pits in the Si(001) substrate. We report on the complex morphological evolution of the single quantum dots contributing to the rings by means of atomic force microscopy and demonstrate that by careful adjustment of the epitaxial growth parameters, such rings containing densely squeezed islands can be grown with large spatial distances of up to 5 µm without additional nucleation of randomly distributed quantum dots between the rings.

Painting with biomolecules at the nanoscale: biofunctionalization with tunable surface densities.

We present a generic and flexible method to nanopattern biomolecules on surfaces. Carbon-containing nanofeatures are written at variable diameter and spacing by a focused electron beam on a poly(ethylene glycol) (PEG)-coated glass substrate. Proteins physisorb to the nanofeatures with remarkably high contrast factors of more than 1000 compared to the surrounding PEG surfaces. The biological activity of model proteins can be retained as shown by decorating avidin spots with biotinylated DNA, thereby underscoring the universality of the nano-biofunctionalized platform for the binding of other biotinylated ligands. In addition, biomolecule densities can be tuned over several orders of magnitude within the same array, as demonstrated by painting a microscale image with nanoscale pixels. We expect that these unique advantages open up entirely new ways to design biophysical experiments, for instance, on cells that respond to the nanoscale densities of activating molecules.

Nanoscale DNA tetrahedra improve biomolecular recognition on patterned surfaces.

The bottom-up approach of DNA nano-biotechnology can create biomaterials with defined properties relevant for a wide range of applications. This report describes nanoscale DNA tetrahedra that are beneficial to the field of biosensing and the targeted immobilization of biochemical receptors on substrate surfaces. The DNA nanostructures act as immobilization agents that are able to present individual molecules at a defined nanoscale distance to the solvent thereby improving biomolecular recognition of analytes. The tetrahedral display devices are self-assembled from four oligonucleotides. Three of the four tetrahedron vertices are equipped with disulfide groups to enable oriented binding to gold surfaces. The fourth vertex at the top of the bound tetrahedron presents the biomolecular receptor to the solvent. In assays testing the molecular accessibility via DNA hybridization and protein capturing, tetrahedron-tethered receptors outperformed conventional immobilization approaches with regard to specificity and amount of captured polypeptide by a factor of up to seven. The bottom-up strategy of creating DNA tetrahedrons is also compatible with the top-down route of nanopatterning of inorganic substrates, as demonstrated by the specific coating of micro- to nanoscale gold squares amid surrounding blank or poly(ethylene glycol)-passivated glass surfaces. DNA tetrahedra can create biofunctionalized surfaces of rationally designed properties that are of relevance in analytical chemistry, cell biology, and single-molecule biophysics.

Microphotoluminescence and perfect ordering of SiGe islands on pit-patterned Si(001) substrates.

We show that both the morphology and the optoelectronic properties of SiGe islands growing in the pits of periodically pre-patterned Si(001) substrates are determined by the amount of Ge deposited per unit cell of the pattern. Pit-periods (p) ranging from 300 to 900 nm were investigated, and Ge growth was performed by molecular beam epitaxy (MBE) at temperatures of 690 and 760 °C. The ordered SiGe islands show photoluminescence (PL) emission, which becomes almost completely quenched, once a critical island volume is exceeded. By atomic force and transmission electron microscope images we identify the transition from pyramid-shaped to dome-shaped islands with increasing p. Eventually, the nucleation of dislocations in the islands leads to PL quenching. Below a critical Ge coverage a narrowing and a blue shift of the PL emission is observed, as compared to islands grown on a planar reference area of the same sample.

Si rib waveguide photodetector with an ordered array of Ge islands for 1.5 microm.

This work demonstrates a rib waveguide photodetector based on a vertical Si p-i-n junction with Ge islands operating in the spectral region around lambda=1.55 microm at room temperature. A vertical stack of four layers of Ge islands is grown by molecular beam epitaxy on a silicon-on-insulator. Each layer is organized in a two-dimensional square grid with a period of 460 nm. The spectral response of the detector extends well beyond 1.6 mum at 300 K. The absorption length of approximately 135 microm (at 1/e decrease of intensity) at lambda=1.55 microm along the waveguide allows for relatively small-size devices for all-on-one-platform integration.