From Crystalline to Amorphous Germania Bilayer Films at the Atomic Scale: Preparation and Characterization

A new two-dimensional (2D) germanium dioxide film has been prepared. The film consists of interconnected germania tetrahedral units forming a bilayer structure, weakly coupled to the supporting Pt(111) metal-substrate. Density functional theory calculations predict a stable structure of 558-membered rings for germania films, while for silica films 6-membered rings are preferred. By varying the preparation conditions the degree of order in the germania films is tuned. Crystalline, intermediate ordered and purely amorphous film structures are resolved by analysing scanning tunnelling microscopy images

From Crystalline to Amorphous Germania Bilayer Films at the Atomic Scale: Preparation and Characterization

A new two-dimensional (2D) germanium dioxide film has been prepared. The film consists of interconnected germania tetrahedral units forming a bilayer structure, weakly coupled to the supporting Pt(111) metal-substrate. Density functional theory calculations predict a stable structure of 558-membered rings for germania films, while for silica films 6-membered rings are preferred. By varying the preparation conditions the degree of order in the germania films is tuned. Crystalline, intermediate ordered and purely amorphous film structures are resolved by analysing scanning tunnelling microscopy images

Spiral high-speed scanning tunneling microscopy: Tracking atomic diffusion on the millisecond timescale

Scanning tunneling microscopy (STM) is one of the most prominent techniques to resolve atomic structures of flat surfaces and thin films. With the scope to answer fundamental questions in physics and chemistry, it was used to elucidate numerous sample systems at the atomic scale. However, dynamic sample systems are difficult to resolve with STM due to the long acquisition times of typically more than 100 s per image. Slow electronic feedback loops, slow data acquisition, and the conventional raster scan limit the scan speed. Raster scans introduce mechanical noise to the image and acquire data discontinuously. Due to the backward and upward scan or the flyback movement of the tip, image acquisition times are doubled or even quadrupled. By applying the quasi-constant height mode and by using a combination of high-speed electronics for data acquisition and innovative spiral scan patterns, we could increase the frame rate in STM significantly. In the present study, we illustrate the implementation of spiral scan geometries and focus on the scanner input signal and the image visualization. Constant linear and constant angular velocity spirals were tested on the Ru(0001) surface to resolve chemisorbed atomic oxygen. The spatial resolution of the spiral scans is comparable to slow raster scans, while the imaging time was reduced from ~100 s to ~8 ms. Within 8 ms, oxygen diffusion processes were atomically resolved

Continuous network structure of two-dimensional silica across a supporting metal step edge: An atomic scale study

The network structure of a silica bilayer film at a monolayer-bilayer transition and across a supporting metal step edge was studied at the atomic scale by scanning tunneling microscopy. The ring size distribution, ring-ring distances, and height profiles are analyzed across the step edge region. Density functional theory proposes two models to explain the observed network structure: a pinning of the lower layer to the substrate and a carpetlike mode. The results indicate a continuous coverage of the silica bilayer film across the step edge

A high-speed variable-temperature ultrahigh vacuum scanning tunneling microscope with spiral scan capabilities

We present the design and development of a variable-temperature high-speed scanning tunneling microscope (STM). The setup consists of a two-chamber ultra-high vacuum system, including a preparation and a main chamber. The preparation chamber is equipped with standard preparation tools for sample cleaning and film growth. The main chamber hosts the STM that is located within a continuous flow cryostat for counter-cooling during high-temperature measurements. The microscope body is compact, rigid, and highly symmetric to ensure vibrational stability and low thermal drift. We designed a hybrid scanner made of two independent tube piezos for slow and fast scanning, respectively. A commercial STM controller is used for slow scanning, while a high-speed Versa Module Eurocard bus system controls fast scanning. Here, we implement non-conventional spiral geometries for high-speed scanning, which consist of smooth sine and cosine signals created by an arbitrary waveform generator. The tip scans in a quasi-constant height mode, where the logarithm of the tunneling current signal can be regarded as roughly proportional to the surface topography. Scan control and data acquisition have been programmed in the experimental physics and industrial control system framework. With the spiral scans, we atomically resolved diffusion processes of oxygen atoms on the Ru(0001) surface and achieved a time resolution of 8.3 ms per frame at different temperatures. Variable-temperature measurements reveal an influence of the temperature on the oxygen diffusion rate

Motion and structure of atmospheric mesoscale baroclinic vortices: dry air and weak environmental shear

By matched asymptotic expansions we analyze the simplified three-dimensional atmospheric flow regime of a nearly axisymmetric vortex in dry air that is in gradient wind balance and embedded in a quasi-geostrophic background wind with weak vertical shear. A description of the vortex' overall motion, its vertical tilt, and of the evolution of its leading-order axisymmetric core structure are developed. The analysis includes the influence of diabatic source terms in the vortex core as a first step towards an asymptotic theory for the structure and motion of hurricanes. The theory is closed except for the solution of a regularized quasi-geostrophic outer flow problem, the formulation of which is outlined here but whose detailed description and numerical integration are deferred to future work

Subvisible cirrus clouds – a dynamical system approach

Ice clouds, so-called cirrus clouds, occur very frequently in the tropopause region. A special class are subvisible cirrus clouds with an optical depth lower than 0.03, associated with very low ice crystal number concentrations. The dominant pathway for the formation of these clouds is not known well. It is often assumed that heterogeneous nucleation on solid aerosol particles is the preferred mechanism although homogeneous freezing of aqueous solution droplets might be possible, since these clouds occur in the low-temperature regime T < 235 K. For investigating subvisible cirrus clouds as formed by homogeneous freezing we develop a reduced cloud model from first principles, which is close enough to complex models but is also simple enough for mathematical analysis. The model consists of a three-dimensional set of ordinary differential equations, and includes the relevant processes as ice nucleation, diffusional growth and sedimentation. We study the formation and evolution of subvisible cirrus clouds in the low-temperature regime as driven by slow vertical updraughts (0 < w ≤ 0. 05 m s−1). The model is integrated numerically and also investigated by means of theory of dynamical systems. We found two qualitatively different states for the long-term behaviour of subvisible cirrus clouds. The first state is a stable focus; i.e. the solution of the differential equations performs damped oscillations and asymptotically reaches a constant value as an equilibrium state. The second state is a limit cycle in phase space; i.e. the solution asymptotically approaches a one-dimensional attractor with purely oscillatory behaviour. The transition between the states is characterised by a Hopf bifurcation and is determined by two parameters – vertical updraught velocity and temperature. In both cases, the properties of the simulated clouds agree reasonably well with simulations from a more detailed model, with former analytical studies, and with observations of subvisible cirrus, respectively. The reduced model can also provide qualitative interpretations of simulations with a complex and more detailed model at states close to bifurcation qualitatively. The results indicate that homogeneous nucleation is a possible formation pathway for subvisible cirrus clouds. The results motivate a minimal model for subvisible cirrus clouds (SVCs), which might be used in future work for the development of parameterisations for coarse large-scale models, representing structures of clouds.ISSN:1023-5809ISSN:1607-794

Subvisible cirrus clouds - a dynamical system approach

Ice clouds, so-called cirrus clouds, occur very frequently in the tropopause region. A special class are subvisible cirrus clouds with an optical depth lower than 0.03, associated with very low ice crystal number concentrations. The dominant pathway for the formation of these clouds is not known well. It is often assumed that heterogeneous nucleation on solid aerosol particles is the preferred mechanism although homogeneous freezing of aqueous solution droplets might be possible, since these clouds occur in the low-temperature regime T < 235 K. For investigating subvisible cirrus clouds as formed by homogeneous freezing we develop a reduced cloud model from first principles, which is close enough to complex models but is also simple enough for mathematical analysis. The model consists of a three-dimensional set of ordinary differential equations, and includes the relevant processes as ice nucleation, diffusional growth and sedimentation. We study the formation and evolution of subvisible cirrus clouds in the low-temperature regime as driven by slow vertical updraughts (0 < w ≤ 0. 05 m s−1). The model is integrated numerically and also investigated by means of theory of dynamical systems. We found two qualitatively different states for the long-term behaviour of subvisible cirrus clouds. The first state is a stable focus; i.e. the solution of the differential equations performs damped oscillations and asymptotically reaches a constant value as an equilibrium state. The second state is a limit cycle in phase space; i.e. the solution asymptotically approaches a one-dimensional attractor with purely oscillatory behaviour. The transition between the states is characterised by a Hopf bifurcation and is determined by two parameters – vertical updraught velocity and temperature. In both cases, the properties of the simulated clouds agree reasonably well with simulations from a more detailed model, with former analytical studies, and with observations of subvisible cirrus, respectively. The reduced model can also provide qualitative interpretations of simulations with a complex and more detailed model at states close to bifurcation qualitatively. The results indicate that homogeneous nucleation is a possible formation pathway for subvisible cirrus clouds. The results motivate a minimal model for subvisible cirrus clouds (SVCs), which might be used in future work for the development of parameterisations for coarse large-scale models, representing structures of clouds.ISSN:1023-5809ISSN:1607-794