Density fluctuations as door-opener for diffusion on crowded surfaces

Science ◽  
2019 ◽  
Vol 363 (6428) ◽  
pp. 715-718 ◽  
Author(s):  
Ann-Kathrin Henß ◽  
Sung Sakong ◽  
Philipp K. Messer ◽  
Joachim Wiechers ◽  
Rolf Schuster ◽  
...  
Keyword(s):  
High Speed ◽  
Density Functional ◽  
Local Density ◽  
Variable Temperature ◽  
Industrial Process ◽  
Density Fluctuations ◽  
Scanning Tunneling ◽  
Fast Diffusion ◽  
Tunneling Microscopy ◽  
Adsorption Sites

How particles can move on a catalyst surface that, under the conditions of an industrial process, is highly covered by adsorbates and where most adsorption sites are occupied has remained an open question. We have studied the diffusion of O atoms on a fully CO-covered Ru(0001) surface by means of high-speed/variable-temperature scanning tunneling microscopy combined with density functional theory calculations. Atomically resolved trajectories show a surprisingly fast diffusion of the O atoms, almost as fast as on the clean surface. This finding can be explained by a “door-opening” mechanism in which local density fluctuations in the CO layer intermittently create diffusion pathways on which the O atoms can move with low activation energy.

STM Image Simulation: Effect of the Number of Tunneling States and the Isosurface Value

2004 ◽  
Vol 838 ◽  
Author(s):  
Juan Radilla ◽  
Marcelo Galván ◽  
Yolanda Trinidad-Reyes ◽  
Nikola Batina
Keyword(s):  
Density Functional ◽  
Local Density ◽  
Scanning Tunneling ◽  
Good Resolution ◽  
Image Simulation ◽  
Tunneling Microscopy ◽  
Functional Theory ◽  
Image Appearance ◽  
Stm Image ◽  
Simulated Images

ABSTRACTIn this work, Scanning Tunneling Microscopy (STM) images were simulated for the organic molecule 3,4,9,10 perylenetetracarboxylic dianhydride (PTCDA) to study the effect of the number of tunneling states and the integrated Local Density of States (LDOS) isosurface value. Local Density Approximation of Density Functional Theory (DFT-LDA) calculations were performed to achieve the simulated images under the Tersoff and Hamann approximation. The number of tunneling states has a strong effect on the image appearance of the patterns. Intermediate isosurface values for the integrated LDOS produce good resolution and matching in relation to the experimental STM image. Both parameters seem to be of significant importance for STM image simulation.

Modeling of Metal(100) Homoepitaxial Film Growth at Very Low Temperatures

2000 ◽  
Vol 619 ◽  
Author(s):  
K.J. Caspersen ◽  
C.R. Stoldt ◽  
P.A. Thiel ◽  
J.W. Evans
Keyword(s):  
Low Temperatures ◽  
Film Growth ◽  
Diffusion Processes ◽  
Variable Temperature ◽  
Scanning Tunneling ◽  
Film Morphology ◽  
Tunneling Microscopy ◽  
Adsorption Sites ◽  
Temperature Scanning ◽  
Homoepitaxial Film

ABSTRACTWe model the growth of Ag films deposited on Ag(100) below 140K. Our recent Variable-Temperature Scanning Tunneling Microscopy (VTSTM) studies reveal “smooth growth” from 120-140K, consistent with earlier diffraction studies. However, we also find rougher growth for lower temperatures. This unexpected behavior is modeled by describing the deposition dynamics using a “restricted downward funneling” model, wherein deposited atoms get caught on the sides of steep nanoprotrusions (which are prevalent below 120K), rather than always funneling down to lower four-fold hollow adsorption sites. At OK, where no thermal diffusion processes are operative, this leads to the formation of overhangs and internal defects (or voids). Above 40K, low barrier interlayer diffusion processes become operative, producing the observed smooth growth by 120K. We also discuss how the apparent film morphology mapped out by the STM tip “smears” features of the actual film morphology (which are small at low temperature), and also can lead to underestimation of the roughness.

scholarly journals Kinetic Roughening of Multilayer Ag/Ag(100) Films: Complex Temperature-Dependence in a Simple System

2000 ◽  
Vol 619 ◽  
Author(s):  
C.R. Stoldt ◽  
K.J. Caspersen ◽  
M.C. Bartelt ◽  
C.J. Jenks ◽  
J.W. Evans ◽  
...  
Keyword(s):  
Lattice Gas ◽  
Film Growth ◽  
Kinetic Monte Carlo ◽  
Variable Temperature ◽  
Scanning Tunneling ◽  
Tunneling Microscopy ◽  
Adsorption Sites ◽  
Lattice Gas Models ◽  
Temperature Scanning ◽  
Complex Temperature

ABSTRACTMetal(100) homoepitaxial systems constitute perhaps the simplest class of systems in which to study thin film growth. Yet, our Variable-Temperature Scanning Tunneling Microscopy (VTSTM) analysis of Ag/Ag(100) homoepitaxy reveals that the variation of roughness with temperature is extraordinarily complex. As the deposition temperature is reduced from 300K to 50K, the roughness of 25 monolayer films first increases, then decreases, and then increases again. Furthermore, a transition from mound formation to self-affine (semi-fractal) growth occurs at around 135K. We postulate that the following the atomistic mechanisms underly this behavior: the existence of a small step-edge barrier inhibiting diffusive downward transport; “downward funneling” of atoms deposited at step edges and microprotrusions towards lower four-fold hollow adsorption sites; and statistically significant deviations from “complete” downward funneling at lower temperatures, where deposited atoms instead become trapped on the sides of (the more prevalent) small steep microprotrusions. To support these postulates, we employ kinetic Monte Carlo simulations to show that atomistic (lattice-gas) models for epitaxial growth, which incorporate these mechanisms, reproduce the experimental data quantitatively.

scholarly journals Imaging and identification of point defects in PtTe2

2021 ◽  
Vol 5 (1) ◽  
Author(s):  
Kuanysh Zhussupbekov ◽  
Lida Ansari ◽  
John B. McManus ◽  
Ainur Zhussupbekova ◽  
Igor V. Shvets ◽  
...  
Keyword(s):  
Point Defects ◽  
Density Functional ◽  
Transition Metal Dichalcogenides ◽  
Density Functional Theory Calculations ◽  
Charge Carrier Mobility ◽  
Scanning Tunneling Spectroscopy ◽  
Scanning Tunneling ◽  
Tunneling Microscopy ◽  
Recombination Rates ◽  
And Performance

AbstractThe properties and performance of two-dimensional (2D) materials can be greatly affected by point defects. PtTe2, a 2D material that belongs to the group 10 transition metal dichalcogenides, is a type-II Dirac semimetal, which has gained a lot of attention recently due to its potential for applications in catalysis, photonics, and spintronics. Here, we provide an experimental and theoretical investigation of point defects on and near the surface of PtTe2. Using scanning tunneling microscopy and scanning tunneling spectroscopy (STS) measurements, in combination with first-principle calculations, we identify and characterize five common surface and subsurface point defects. The influence of these defects on the electronic structure of PtTe2 is explored in detail through grid STS measurements and complementary density functional theory calculations. We believe these findings will be of significance to future efforts to engineer point defects in PtTe2, which is an interesting and enticing approach to tune the charge-carrier mobility and electron–hole recombination rates, as well as the site reactivity for catalysis.

scholarly journals Dual role of CO in the stability of subnano Pt clusters at the Fe3O4(001) surface

2016 ◽  
Vol 113 (32) ◽  
pp. 8921-8926 ◽  
Author(s):  
Roland Bliem ◽  
Jessi E. S. van der Hoeven ◽  
Jan Hulva ◽  
Jiri Pavelec ◽  
Oscar Gamba ◽  
...  
Keyword(s):  
Density Functional ◽  
Elevated Temperatures ◽  
Time Lapse ◽  
Dual Role ◽  
Oxidation Catalyst ◽  
Scanning Tunneling ◽  
Tunneling Microscopy ◽  
Active Metal ◽  
Catalytically Active ◽  
The Stability

Interactions between catalytically active metal particles and reactant gases depend strongly on the particle size, particularly in the subnanometer regime where the addition of just one atom can induce substantial changes in stability, morphology, and reactivity. Here, time-lapse scanning tunneling microscopy (STM) and density functional theory (DFT)-based calculations are used to study how CO exposure affects the stability of Pt adatoms and subnano clusters at the Fe3O4(001) surface, a model CO oxidation catalyst. The results reveal that CO plays a dual role: first, it induces mobility among otherwise stable Pt adatoms through the formation of Pt carbonyls (Pt1–CO), leading to agglomeration into subnano clusters. Second, the presence of the CO stabilizes the smallest clusters against decay at room temperature, significantly modifying the growth kinetics. At elevated temperatures, CO desorption results in a partial redispersion and recovery of the Pt adatom phase.

scholarly journals Self-assembly of N-heterocyclic carbenes on Au(111)

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Alex Inayeh ◽  
Ryan R. K. Groome ◽  
Ishwar Singh ◽  
Alex J. Veinot ◽  
Felipe Crasto de Lima ◽  
...  
Keyword(s):  
Self Assembly ◽  
Density Functional ◽  
Surface Coverage ◽  
High Mobility ◽  
Heterocyclic Carbenes ◽  
Scanning Tunneling ◽  
Tunneling Microscopy ◽  
Surface Geometry ◽  
Functional Theory ◽  
Interesting Alternative

AbstractAlthough the self-assembly of organic ligands on gold has been dominated by sulfur-based ligands for decades, a new ligand class, N-heterocyclic carbenes (NHCs), has appeared as an interesting alternative. However, fundamental questions surrounding self-assembly of this new ligand remain unanswered. Herein, we describe the effect of NHC structure, surface coverage, and substrate temperature on mobility, thermal stability, NHC surface geometry, and self-assembly. Analysis of NHC adsorption and self-assembly by scanning tunneling microscopy and density functional theory have revealed the importance of NHC-surface interactions and attractive NHC-NHC interactions on NHC monolayer structures. A remarkable way these interactions manifest is the need for a threshold NHC surface coverage to produce upright, adatom-mediated adsorption motifs with low surface diffusion. NHC wingtip structure is also critical, with primary substituents leading to the formation of flat-lying NHC2Au complexes, which have high mobility when isolated, but self-assemble into stable ordered lattices at higher surface concentrations. These and other studies of NHC surface chemistry will be crucial for the success of these next-generation monolayers.

In-Plane Asymmetries on the Ge(111)-c(2×8) Surface Mapped with the Scanning Tunneling Microscope

1992 ◽  
Vol 295 ◽  
Author(s):  
P. Molinàs-Mata ◽  
J. Zegenhagen ◽  
M. Böhringer ◽  
N. Takeuchi ◽  
A. Selloni
Keyword(s):  
Local Density ◽  
Experimental Studies ◽  
Surface States ◽  
Small Sample ◽  
Constant Current ◽  
Scanning Tunneling ◽  
Tunneling Microscopy ◽  
Low Energy Electron ◽  
Tunneling Currents ◽  
Insight Into

AbstractWe report on new experimental studies of the Ge(111)-c(2×8) reconstruction performed with low-energy electron diffraction. (LEED) and scanning tunneling microscopy (STM). Weak quarter-order reflections are present in the c(2 × 8) LEED pattern in agreement with previous observations and results of ab initio calculations. In order to gain insight into the predicted splitting of dangling bond states, we compare constant current topographs (CCT's) performed at high-tunneling currents (40.nA) with first-principles calculations of the local density of states (LDOS) 1Å above the surface adatoms and obtain good qualitative agreement. We finally discuss to what extent the STM CCT's at high tunneling currents (small sample-tip distances (STD)) are sensitive to surface states outside the Г point.

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