Measurement of phosphorus segregation in silicon at the atomic-scale using STM

In order to fabricate precise atomic-scale devices in silicon using a combination of scanning tunnelling microscopy (STM) and molecular beam epitaxy it is necessary to minimize the segregation/diffusion of dopant atoms during silicon encapsulation. We characterize the surface segregation/diffusion of phosphorus atoms from a $\delta$-doped layer in silicon after encapsulation at 250$^{\circ}$C and room temperature using secondary ion mass spectrometry (SIMS), Auger electron spectroscopy (AES), and STM. We show that the surface phosphorus density can be reduced to a few percent of the initial $\delta$-doped density if the phosphorus atoms are encapsulated with 5 or 10 monolayers of epitaxial silicon at room temperature. We highlight the limitations of SIMS and AES to determine phosphorus segregation at the atomic-scale and the advantage of using STM directly

Encapsulation of phosphorus dopants in silicon for the fabrication of a quantum computer

The incorporation of phosphorus in silicon is studied by analyzing phosphorus delta-doped layers using a combination of scanning tunneling microscopy, secondary ion mass spectrometry and Hall effect measurements. The samples are prepared by phosphine saturation dosing of a Si(100) surface at room temperature, a critical annealing step to incorporate phosphorus atoms, and subsequent epitaxial silicon overgrowth. We observe minimal dopant segregation (5 nm), complete electrical activation at a silicon growth temperature of 250 degrees C and a high two-dimensional electron mobility of 100 cm2/Vs at a temperature of 4.2 K. These results, along with preliminary studies aimed at further minimizing dopant diffusion, bode well for the fabrication of atomically precise dopant arrays in silicon such as those found in recent solid-state quantum computer architectures.Comment: 3 pages, 4 figure

The formation of a Sn monolayer on Ge(1 0 0) studied at the atomic scale

The growth of multi-layer germanium-tin (GeSn) quantum wells offers an intriguing pathway towards the integration of lasers in a CMOS platform. An important step in growing high quality quantum well interfaces is the formation of an initial wetting layer. However, key atomic-scale details of this process have not previously been discussed. We use scanning tunneling microscopy combined with density functional theory to study the deposition of Sn on Ge(1 0 0) at room temperature over a coverage range of 0.01 to 1.24 monolayers. We demonstrate the formation of a sub-2% Ge content GeSn wetting layer from three atomic-scale characteristic ad-dimer structural components, and show that small quantities of Sn incorporate into the Ge surface forming two atomic configurations. The ratio of the ad-dimer structures changes with increasing Sn coverage, indicating a change in growth kinetics. At sub-monolayer coverage, the least densely packing ad-dimer structure is most abundant. As the layer closes, forming a two-dimensional wetting layer, the more densely packing ad-dimer structure become dominant. These results demonstrate the capability to form an atomically smooth wetting layer at room temperature, and provide critical atomic-scale insights for the optimization of growth processes of GeSn multi-quantum-wells to meet the quality requirements of optical GeSn-based devices

Quantum engineering at the silicon surface using dangling bonds.

Individual atoms and ions are now routinely manipulated using scanning tunnelling microscopes or electromagnetic traps for the creation and control of artificial quantum states. For applications such as quantum information processing, the ability to introduce multiple atomic-scale defects deterministically in a semiconductor is highly desirable. Here we use a scanning tunnelling microscope to fabricate interacting chains of dangling bond defects on the hydrogen-passivated silicon (001) surface. We image both the ground-state and the excited-state probability distributions of the resulting artificial molecular orbitals, using the scanning tunnelling microscope tip bias and tip-sample separation as gates to control which states contribute to the image. Our results demonstrate that atomically precise quantum states can be fabricated on silicon, and suggest a general model of quantum-state fabrication using other chemically passivated semiconductor surfaces where single-atom depassivation can be achieved using scanning tunnelling microscopy

STM characterization of the Si-P heterodimer

We use scanning tunneling microscopy (STM) and Auger electron spectroscopy to study the behavior of adsorbed phosphine (PH$_{3}$) on Si(001), as a function of annealing temperature, paying particular attention to the formation of the Si-P heterodimer. Dosing the Si(001) surface with ${\sim}$0.002 Langmuirs of PH$_{3}$ results in the adsorption of PH$_{x}$ (x=2,3) onto the surface and some etching of Si to form individual Si ad-dimers. Annealing to 350$^{\circ}$C results in the incorporation of P into the surface layer to form Si-P heterodimers and the formation of short 1-dimensional Si dimer chains and monohydrides. In filled state STM images, isolated Si-P heterodimers appear as zig-zag features on the surface due to the static dimer buckling induced by the heterodimer. In the presence of a moderate coverage of monohydrides this static buckling is lifted, rending the Si-P heterodimers invisible in filled state images. However, we find that we can image the heterodimer at all H coverages using empty state imaging. The ability to identify single P atoms incorporated into Si(001) will be invaluable in the development of nanoscale electronic devices based on controlled atomic-scale doping of Si.Comment: 6 pages, 4 figures (only 72dpi

DSYB catalyses the key step of dimethylsulfoniopropionate biosynthesis in many phytoplankton

Dimethylsulfoniopropionate (DMSP) is a globally important organosulfur molecule and the major precursor for dimethyl sulfide. These compounds are important info-chemicals, key nutrients for marine microorganisms, and are involved in global sulfur cycling, atmospheric chemistry and cloud formation1,2,3. DMSP production was thought to be confined to eukaryotes, but heterotrophic bacteria can also produce DMSP through the pathway used by most phytoplankton4, and the DsyB enzyme catalysing the key step of this pathway in bacteria was recently identified5. However, eukaryotic phytoplankton probably produce most of Earth’s DMSP, yet no DMSP biosynthesis genes have been identified in any such organisms. Here we identify functional dsyB homologues, termed DSYB, in many phytoplankton and corals. DSYB is a methylthiohydroxybutryate methyltransferase enzyme localized in the chloroplasts and mitochondria of the haptophyte Prymnesium parvum, and stable isotope tracking experiments support these organelles as sites of DMSP synthesis. DSYB transcription levels increased with DMSP concentrations in different phytoplankton and were indicative of intracellular DMSP. Identification of the eukaryotic DSYB sequences, along with bacterial dsyB, provides the first molecular tools to predict the relative contributions of eukaryotes and prokaryotes to global DMSP production. Furthermore, evolutionary analysis suggests that eukaryotic DSYB originated in bacteria and was passed to eukaryotes early in their evolution

The Ruegeria pomeroyi acuI Gene Has a Role in DMSP Catabolism and Resembles yhdH of E. coli and Other Bacteria in Conferring Resistance to Acrylate

The Escherichia coli YhdH polypeptide is in the MDR012 sub-group of medium chain reductase/dehydrogenases, but its biological function was unknown and no phenotypes of YhdH− mutants had been described. We found that an E. coli strain with an insertional mutation in yhdH was hyper-sensitive to inhibitory effects of acrylate, and, to a lesser extent, to those of 3-hydroxypropionate. Close homologues of YhdH occur in many Bacterial taxa and at least two animals. The acrylate sensitivity of YhdH− mutants was corrected by the corresponding, cloned homologues from several bacteria. One such homologue is acuI, which has a role in acrylate degradation in marine bacteria that catabolise dimethylsulfoniopropionate (DMSP) an abundant anti-stress compound made by marine phytoplankton. The acuI genes of such bacteria are often linked to ddd genes that encode enzymes that cleave DMSP into acrylate plus dimethyl sulfide (DMS), even though these are in different polypeptide families, in unrelated bacteria. Furthermore, most strains of Roseobacters, a clade of abundant marine bacteria, cleave DMSP into acrylate plus DMS, and can also demethylate it, using DMSP demethylase. In most Roseobacters, the corresponding gene, dmdA, lies immediately upstream of acuI and in the model Roseobacter strain Ruegeria pomeroyi DSS-3, dmdA-acuI were co-regulated in response to the co-inducer, acrylate. These observations, together with findings by others that AcuI has acryloyl-CoA reductase activity, lead us to suggest that YdhH/AcuI enzymes protect cells against damaging effects of intracellular acryloyl-CoA, formed endogenously, and/or via catabolising exogenous acrylate. To provide “added protection” for bacteria that form acrylate from DMSP, acuI was recruited into clusters of genes involved in this conversion and, in the case of acuI and dmdA in the Roseobacters, their co-expression may underpin an interaction between the two routes of DMSP catabolism, whereby the acrylate product of DMSP lyases is a co-inducer for the demethylation pathway

Split-off dimer defects on the Si(001)2x1 surface

Dimer vacancy (DV) defect complexes in the Si(001)2x1 surface were investigated using high-resolution scanning tunneling microscopy and first principles calculations. We find that under low bias filled-state tunneling conditions, isolated 'split-off' dimers in these defect complexes are imaged as pairs of protrusions while the surrounding Si surface dimers appear as the usual 'bean-shaped' protrusions. We attribute this to the formation of pi-bonds between the two atoms of the split-off dimer and second layer atoms, and present charge density plots to support this assignment. We observe a local brightness enhancement due to strain for different DV complexes and provide the first experimental confirmation of an earlier prediction that the 1+2-DV induces less surface strain than other DV complexes. Finally, we present a previously unreported triangular shaped split-off dimer defect complex that exists at SB-type step edges, and propose a structure for this defect involving a bound Si monomer.Comment: 8 pages, 7 figures, submitted to Phys. Rev.

Towards the fabrication of phosphorus qubits for a silicon quantum computer

The quest to build a quantum computer has been inspired by the recognition of the formidable computational power such a device could offer. In particular silicon-based proposals, using the nuclear or electron spin of dopants as qubits, are attractive due to the long spin relaxation times involved, their scalability, and the ease of integration with existing silicon technology. Fabrication of such devices however requires atomic scale manipulation - an immense technological challenge. We demonstrate that it is possible to fabricate an atomically-precise linear array of single phosphorus bearing molecules on a silicon surface with the required dimensions for the fabrication of a silicon-based quantum computer. We also discuss strategies for the encapsulation of these phosphorus atoms by subsequent silicon crystal growth.Comment: To Appear in Phys. Rev. B Rapid Comm. 5 pages, 5 color figure

Reaction paths of phosphine dissociation on silicon (001)

Using density functional theory and guided by extensive scanning tunneling microscopy (STM) image data, we formulate a detailed mechanism for the dissociation of phosphine (PH3) molecules on the Si(001) surface at room temperature. We distinguish between a main sequence of dissociation that involves PH2+H, PH+2H, and P+3H as observable intermediates, and a secondary sequence that gives rise to PH+H, P+2H, and isolated phosphorus adatoms. The latter sequence arises because PH2 fragments are surprisingly mobile on Si(001) and can diffuse away from the third hydrogen atom that makes up the PH3 stoichiometry. Our calculated activation energies describe the competition between diffusion and dissociation pathways and hence provide a comprehensive model for the numerous adsorbate species observed in STM experiments