A5010837391- Spectroscopy and Laser Applications
- Advanced Chemical Physics Studies
- nanoparticles nucleation surface interactions
- Atmospheric chemistry and aerosols
- Combustion and flame dynamics
- Spectroscopy and Quantum Chemical Studies
- Laser Design and Applications
- Catalytic Processes in Materials Science
- Coagulation and Flocculation Studies
- Atomic and Molecular Physics
- Mass Spectrometry Techniques and Applications
- Atmospheric Ozone and Climate
- Laser-induced spectroscopy and plasma
- Ion-surface interactions and analysis
- X-ray Diffraction in Crystallography
- Advanced Combustion Engine Technologies
- Molecular Junctions and Nanostructures
- Crystallization and Solubility Studies
- Atmospheric and Environmental Gas Dynamics
- Gas Sensing Nanomaterials and Sensors
- Laser-Matter Interactions and Applications
- Ammonia Synthesis and Nitrogen Reduction
- Surface Chemistry and Catalysis
- Iron oxide chemistry and applications
- Advanced Photocatalysis Techniques
Open University of Israel
2015-2025
Weizmann Institute of Science
2012
University of California, Santa Barbara
2008-2010
Tel Aviv University
2000-2007
Nature of the molecule-surface encounter Adsorption is an important initial step in all heterogeneous chemical processes. However, detailed adsorption dynamics are complex and challenging to follow experimentally. Using fact that vibrationally excited carbon monoxide molecules can be trapped on Au(111) surface with degrees freedom being equilibrated except vibrational ones, Borodin et al. show relaxation time serve as internal clock microscopic pathways equilibration surface. On basis...
We report a rotationally resolved spectroscopic detection scheme for vibrationally excited molecular oxygen with high sensitivity. Two-color (2 + 1′) resonance-enhanced multiphoton ionization (REMPI) spectra of O2 hot bands were recorded the first time via 3dπ(v′=0)←X3Σg− (v″ = 1) Rydberg transitions. Spectroscopic constants and relative Franck–Condon factors extracted compared to simulations. This new access quantum-state-resolved diagnostics promises shed light on physical chemical...
The mechanism and consequently the magnitude of vibrational relaxation molecules on surfaces differ significantly between insulators metals, making energy transfer at NO/metal versus NO/insulator interface a canonical example in field. We report influence surface temperature, initial state, incident translational probability vibrationally excited NO(vI = 3 vI 11) undergoing direct scattering from thin films vanadium dioxide (VO2) across Mott transition 68 °C. At that thin-film VO2 transforms...
The Born–Oppenheimer Approximation (BOA) forms the basis for calculating electronically adiabatic potential energy surfaces, thus providing framework developing a molecular level understanding of variety important chemical problems. For surface chemistry at metal it is now clear that some processes nonadiabatic effects can be important, even dominant; however, magnitude BOA breakdown may vary widely from one system to another. In this paper we show molecular-beam scattering experiments used...
Surface phenomena: measurements of absolute probabilities are reported for the vibrational excitation NO(v=0→1,2) molecules scattered from a Au(111) surface. These were quantitatively compared to calculations based on ab initio theoretical approaches electronically nonadiabatic molecule-surface interactions. Good agreement was found between theory and experiment (see picture; T(s) =surface temperature, P=excitation probability, E=incidence energy translation).
Translational motion is believed to be a spectator degree of freedom in electronically nonadiabatic vibrational energy transfer between molecules and metal surfaces, but the experimental evidence available support this view limited. In work, we have experimentally determined translational inelasticity collisions NO with single-crystal Au(111) surface—a system strong electronic nonadiabaticity. State-to-state molecular beam surface scattering was combined an IR-UV double resonance scheme...
Views Icon Article contents Figures & tables Video Audio Supplementary Data Peer Review Share Twitter Facebook Reddit LinkedIn Tools Reprints and Permissions Cite Search Site Citation Kai Golibrzuch, Pranav R. Shirhatti, Igor Rahinov, Alexander Kandratsenka, Daniel J. Auerbach, Alec M. Wodtke, Christof Bartels; The importance of accurate adiabatic interaction potentials for the correct description electronically nonadiabatic vibrational energy transfer: A combined experimental theoretical...
Premixed, laminar H2/O2/Ar and CH4/O2/N2 low-pressure flat flames doped with iron pentacarbonyl (Fe(CO)5) were used to investigate the initial steps towards formation of iron-oxide nanoparticles. The particles extracted from flame using a molecular beam sampling probe mass flow rate condensed material was measured by quartz crystal microbalance (QCM). It observed that are already formed on cold side flame, vanish quickly once they pass through front. To understand process assess...
We report zero-coverage reaction probabilities (S0) for HCl dissociative adsorption on Au(111) obtained by the seeded molecular beam hot-nozzle method. For measurements at normal incidence with mean translational energies ranging from 0.94 to 2.56 eV (nozzle temperatures 296 1060 K), S0 increased 6 × 10(-6) 2 10(-2). also increasing nozzle temperature fixed energy associated motion surface. Accounting influence of vibrational state population and distributions in incident beam, we are able...
We report accurate time-resolved measurements of NH3 desorption from Pt(111) and Pt(332) use these results to determine elementary rate constants for steps, (111) terrace sites diffusion on terraces. Modeling the extracted with transition state theory, we find that conventional models partition functions, which rely uncoupled degrees freedom (DOFs), are not able reproduce experimental observations. The can be reproduced using a more sophisticated function, couples DOFs most sensitive...
We report high resolution state-to-state time-of-flight (TOF) measurements for scattering of HCl(v=2, J=1) from a Au(111) single crystal surface both vibrationally elastic (v=2→2) as well inelastic (v=2→1) channels at seven incidence energies between 0.28 and 1.27 eV. The dependences the TOF results on final HCl rotational state temperature are also reported. translational energy transferred to depends linearly is close surface-atom impulse (Baule) limit over entire range studied....
In this work we seek to examine the nature of collisional energy transfer between HCl and Au(111) for nonreactive scattering events that sample geometries near transition state dissociative adsorption by varying both vibrational translational incident molecules in range dissociation barrier. Specifically, report absolute excitation probabilities HCl(v = 0 → 1) 1 2) from clean as a function surface temperature incidence energy. The 2 3) channel could not be observed-presumably due onset...
To fully master a scaled-up combustion synthesis of nanoparticles toward wide library materials with tailored functionalities, detailed understanding the underlying kinetic mechanism is required. In this respect, flame iron oxide model case, being one better understood systems and guiding way how other material could be advanced. mini-review, we highlight, on example an system, approach combining laser spectroscopy mass spectrometry simulations. The experiments deliver information...
Studying dynamics of the dissociative adsorption and recombinative desorption hydrogen on copper surfaces has shaped our atomic-scale understanding surface chemistry, yet experimentally determining thermal rates for these processes, which dictate outcome catalytic reactions, been impossible so far. In this work, we determine rate constants Cu(111) between 200 1000 K using data from reaction experiments. Contrary to current understanding, findings demonstrate predominant role quantum...
We measured absolute probabilities for vibrational excitation of NO(v = 0) molecules in collisions with a Au(111) surface at an incidence energy translation 0.4 eV and temperatures between 300 1100 K. In addition to previously reported v 1 2, we observed 3. The exhibit Arrhenius dependence on temperature, indicating that the dominant mechanism is nonadiabatic coupling electron-hole pairs. experimental data are analyzed terms recently introduced kinetic model, which was extended include four...
We report measurements of translational energy distributions when scattering NO(vi = 3, Ji 1.5) from a Au(111) surface into vibrational states vf 1, 2, 3 and rotational up to Jf 32.5 for various incidence energies ranging 0.11 eV 0.98 eV. observed that the vibration-to-translation as well translation-to-rotation coupling depend on energy, EI. The coupling, i.e. additional recoil vibrationally inelastic (v → 1) scattering, is seen increase with increasing final decreases approximately...