Isolated Elusive Fullerene and Lanthanoid Complex Species: Optical Spectroscopy in Cryogenic Matrixes and Low-Temperature STM

Elusive molecular species are studied with optical spectroscopy in cryogenic noble gas matrixes and with low-temperature STM. The existing apparatus for isolating elusive and reactive species in cryogenic matrixes is improved, enabling optical spectroscopy of previously inaccessible, mass-selected fullerene and azafullerene ions in unusual charge states, as well as electrosprayed complex ions. Vibronic excitations of single C60 and endohedral H2@C60 molecules on CuN surfaces are studied by STM

A Λ\Lambda-Fleming-Viot type model with intrinsically varying population size

We propose an extension of the classical $\Lambda$-Fleming-Viot model to intrinsically varying population sizes. During events, instead of replacing a proportion of the population, a random mass dies and a, possibly different, random mass of new individuals is added. The model can also incorporate a drift term, representing infinitesimally small, but frequent events. We investigate elementary properties of the model, analyse its relation to the $\Lambda$-Fleming-Viot model and describe a duality relationship. Through the lookdown framework, we provide a forward-in-time analysis of fixation and coming down from infinity. Furthermore, we present a new duality argument allowing one to deduce well-posedness of the measure-valued process without the necessity of proving uniqueness of the associated lookdown martingale problem

Molecular quantum spin network controlled by a single qubit

Scalable quantum technologies will require an unprecedented combination of precision and complexity for designing stable structures of well-controllable quantum systems. It is a challenging task to find a suitable elementary building block, of which a quantum network can be comprised in a scalable way. Here we present the working principle of such a basic unit, engineered using molecular chemistry, whose control and readout are executed using a nitrogen vacancy (NV) center in diamond. The basic unit we investigate is a synthetic polyproline with electron spins localized on attached molecular sidegroups separated by a few nanometers. We demonstrate the readout and coherent manipulation of very few ($\leq 6$) of these $S=1/2$ electronic spin systems and access their direct dipolar coupling tensor. Our results show, that it is feasible to use spin-labeled peptides as a resource for a molecular-qubit based network, while at the same time providing simple optical readout of single quantum states through NV-magnetometry. This work lays the foundation for building arbitrary quantum networks using well-established chemistry methods, which has many applications ranging from mapping distances in single molecules to quantum information processing.Comment: Author name typ

C58 on Au(111): a scanning tunneling microscopy study

C58 fullerenes were adsorbed onto room temperature Au(111) surface by low-energy (~6 eV) cluster ion beam deposition under ultrahigh vacuum conditions. The topographic and electronic properties of the deposits were monitored by means of scanning tunnelling microscopy (STM at 4.2 K). Topographic images reveal that at low coverages fullerene cages are pinned by point dislocation defects on the herringbone reconstructed gold terraces (as well as by step edges). At intermediate coverages, pinned monomers, act as nucleation centres for the formation of oligomeric C58 chains and 2D islands. At the largest coverages studied, the surface becomes covered by 3D interlinked C58 cages. STM topographic images of pinned single adsorbates are essentially featureless. The corresponding local densities of states are consistent with strong cage-substrate interactions. Topographic images of [C58]n oligomers show a stripe-like intensity pattern oriented perpendicular to the axis connecting the cage centers. This striped pattern becomes even more pronounced in maps of the local density of states. As supported by density functional theory, DFT calculations, and also by analogous STM images previously obtained for C60 polymers (M. Nakaya et al., J. Nanosci. Nanotechnol. 11, 2829 (2011)), we conclude that these striped orbital patterns are a fingerprint of covalent intercage bonds. For thick C58 films we have derived a band gap of 1.2 eV from scanning tunnelling spectroscopy data, STS, confirming that the outermost C58 layer behaves as a wide band semiconductor

High selectivity of TiC-CDC for CO2/N2 separation

A series of carbide-derived carbons (CDC) have been prepared starting from TiC and using different chlorine treatment temperatures (500–1200 °C). Contrary to N2 adsorption measurements at −196 °C, CO2 adsorption measurements at room temperature and high pressure (up to 1 MPa) together with immersion calorimetry measurements into dichloromethane suggest that the synthesized CDC exhibit a similar porous structure, in terms of narrow pore volume, independently of the temperature of the reactive extraction treatment used (samples synthesized below 1000 °C). Apparently, these carbide-derived carbons exhibit narrow constrictions were CO2 adsorption under standard conditions (0 °C and atmospheric pressure) is kinetically restricted. The same accounts for a slightly larger molecule as N2 at a lower adsorption temperature (−196 °C), i.e. textural parameters obtained from N2 adsorption measurements on CDC must be underestimated. Furthermore, here we show experimentally that nitrogen exhibits an unusual behavior, poor affinity, on these carbide-derived carbons. CH4 with a slightly larger diameter (0.39 nm) is able to partially access the inner porous structure whereas N2, with a slightly smaller diameter (0.36 nm), does not. Consequently, these CDC can be envisaged as excellent sorbent for selective CO2 capture in flue-gas streams.This work was supported by the National Science Centre under the Grant No. DEC–2011/01/N/ST5/05595. Rafał Janus wishes to thank the Foundation for Polish Science MPD Programme co-financed by the EU European Regional Development Fund for the financial support. The research was carried out with the equipment purchased thanks to the financial support of the European Regional Development Fund in the framework of the Polish Innovation Economy Operational Program (contract No. POIG.02.01.00-12-023/08)

Enabling micro-entertainment in vehicles based on context information

People spend a significant amount of time in their cars (US: 86 minutes/day, Europe: 43 minutes/day) while commuting, shop-ping, or traveling. Hence, the variety of entertainment in the car increases, and many vehicles are already equipped with displays, allowing for watching news, videos, accessing the Internet, or playing games. At the same time, the urbanization caused a mas-sive increase of traffic volume, which led to people spending an ever-increasing amount of their time in front of red traffic lights. An observation of the prevailing forms of entertainment in the car reveals that content such as text, videos, or games are often a mere adaptation of content produced for television, public displays, PCs, or mobile phones and do not adapt to the situation in the car. In this paper we report on a web survey assessing which forms of entertainment and which types of content are considered to be useful for in-car entertainment by drivers. We then introduce an algorithm, which is capable of learning standing times in front of traffic lights based on GPS information only. This, on one hand, allows for providing content of appropriate length, on the other hand, for directing the attention of the driver back to-wards the street at the right time. Finally, we present a prototype implemen-tation and a qualitative evaluation

Emulating lateral gravity wave propagation in a global chemistry-climate model (EMAC v2.55.2) through horizontal flux redistribution

The columnar approach of gravity wave (GW) parameterisations in weather and climate models has been identified as a potential reason for dynamical biases in middle-atmospheric dynamics. For example, GW momentum flux (GWMF) discrepancies between models and observations at 60°S arising through the lack of horizontal orographic GW propagation are suspected to cause deficiencies in representing the Antarctic polar vortex. However, due to the decomposition of the model domains onto different computing tasks for parallelisation, communication between horizontal grid boxes is computationally extremely expensive, making horizontal propagation of GWs unfeasible for global chemistry-climate simulations. To overcome this issue, we present a simplified solution to approximate horizontal GW propagation through redistribution of the GWMF at one single altitude by means of tailor-made redistribution maps. To generate the global redistribution maps averaged for each grid box, we use a parameterisation describing orography as a set of mountain ridges with specified location, orientation and height combined with a ray-tracing model describing lateral propagation of so-generated mountain waves. In the global chemistry-climate model (CCM) EMAC (ECHAM MESSy Atmospheric Chemistry), these maps then allow us to redistribute the GW momentum flux horizontally at one level, obtaining an affordable overhead of computing resources. The results of our simulations show GWMF and drag patterns that are horizontally more spread out than with the purely columnar approach; GWs are now also present above the ocean and regions without mountains. In this paper, we provide a detailed description of how the redistribution maps are computed and how the GWMF redistribution is implemented in the CCM. Moreover, an analysis shows why 15 km is the ideal altitude for the redistribution. First results with the redistributed orographic GWMF provide clear evidence that the redistributed GW drag in the Southern Hemisphere has the potential to modify and improve Antarctic polar vortex dynamics, thereby paving the way for enhanced credibility of CCM simulations and projections of polar stratospheric ozone

The patterning toolbox FIB-o-mat: Exploiting the full potential of focused helium ions for nanofabrication

Focused beams of helium ions are a powerful tool for high-fidelity machining with spatial precision below 5 nm. Achieving such a high patterning precision over large areas and for different materials in a reproducible manner, however, is not trivial. Here, we introduce the Python toolbox FIB-o-mat for automated pattern creation and optimization, providing full flexibility to accomplish demanding patterning tasks. FIB-o-mat offers high-level pattern creation, enabling high-fidelity large-area patterning and systematic variations in geometry and raster settings. It also offers low-level beam path creation, providing full control over the beam movement and including sophisticated optimization tools. Three applications showcasing the potential of He ion beam nanofabrication for two-dimensional material systems and devices using FIB-o-mat are presented