Publications de Rainer Beck | EPFL Graph Search

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The probability for dissociation of molecules on metal surfaces, which often controls the rate of industrially important catalytic processes, can depend strongly on how energy is partitioned in the incident molecule. There are many example systems where th ...

The state-resolved reactivity of CH4 in its totally symmetric C-H stretch vibration (nu(1)) has been measured on a Ni(100) surface. Methane molecules were accelerated to kinetic energies of 49 and 63.5 kJ/mol in a molecular beam and vibrationally excited t ...

Quantum state-resolved sticking coefficients on Pt(111) and Ni(111) surfaces have been measured for CH4 excited to the first overtone of the antisymmetric C-H stretch (2ν3) at well defined kinetic energies in the range of 10-90 kJ/mol. The ground state rea ...

Linewidths, unimolecular dissociation rates and product state distributions (PSDs) have been measured for single rovibratational states of the nu(1)=5-7 levels of gas-phase trans-nitrous acid (HONO) by double-resonance overtone photofragment spectroscopy (DROPS). The linewidth measurements, together with the unimolecular dissociation rates in 5nu(1), suggest that the intramolecular dynamics are not statistical but rather depend sensitively upon specific intramolecular couplings and the vibrational character

Using the technique of double-resonance overtone photofragment spectroscopy (DROPS), we have measured rotationally resolved vibrational overtone transitions to the previously unobserved 5v(1), 6v(1), and 7v(1) levels of gas-phase trans-nitrous acid (HONO) in its electronic ground state. Observing the onset of dissociation from different rovibrational states of 5v(1) near threshold determines the HO-NO bond energy to be D-0=16 772 +/- 14 cm(-1). Observed spectral splittings and broadening of individual rovib

Platinum (Pt) is a key material in automotive catalytic converters used to clean up the exhaust of the combustion engine. Pt particles in a ceramic matrix serve as an oxidation catalyst to eliminate toxic carbon monoxide (CO) and unburned hydrocarbons (CxH ...

Highly efficient preparation of molecules in a specific rovibrationally excited state for gas/surface reactivity measurements is achieved in a molecular beam using tunable infrared (IR) radiation from a single mode continuous wave optical parametric oscill ...

We present a tutorial review of our quantum state resolved experiments designed to study gas–surface reaction dynamics. The combination of a molecular beam, state specific reactant preparation by infrared laser pumping, and ultrahigh vacuum surface analysi ...

This book gives a representative survey of the state of the art of research on gas-surface interactions. It provides an overview of the current understanding of gas surface dynamics and, in particular, of the reactive and non-reactive processes of atoms and small molecules at surfaces. Leading scientists in the field, both from the theoretical and the experimental sides, write in this book about their most recent advances. Surface science grew as an interdisciplinary research area over the last decades, mos

We present a stereodynamics study of the dissociative chemisorption of vibrationally excited methane on the (100), (110), and (111) planes of a nickel single crystal surface. Using linearly polarized infrared excitation of the antisymmetric C–H stretch nor ...

The state-resolved reaction probability of CH4 on Pt(110)-(1×2) was measured as a function of CH4 translational energy for four vibrational eigenstates comprising different amounts of C-H stretch and bend excitation. State-specific reactivity is observed b ...

Methane dissociation on the step and terrace sites of a Pt(211) single crystal was studied by reflection absorption infrared spectroscopy (RAIRS) at a surface temperature of 120 K. The C−H stretch RAIRS signal of the chemisorbed methyl product species was ...

The dissociative chemisorption of singly deuterated methane (CH3D) has been studied on the steps and terraces of a Pt(211) surface by quantum state resolved molecular beam methods. At incident translational energy (Et) below 50 kJ/mol, CH3D dissociates onl ...

We report a combined experimental and theoretical study comparing methane dissociation on three di erent platinum surfaces Pt(111), Pt(211), and Pt(110)-(1 × 2). Re ection absorption infrared spectroscopy (RAIRS) was used to detect chemisorbed methyl speci ...

Reflection–absorption infrared spectroscopy (RAIRS) is widely used to identify molecular adsorbates on metals during surface chemical reactions, but the interpretation of RAIRS data can be difficult with experiment alone. Here, we reveal from first-princip ...

The presence of chemisorbed oxygen on the Cu(111) surface is known to strongly reduce the activation barrier for water dissociation as compared to bare Cu(111). Here, we present direct experimental evidence for the hydrogen abstraction mechanism responsibl ...

We report the design and characterization of a new molecular-beam/surface-science apparatus for quantum state-resolved studies of gas/surface reaction dynamics combining optical state-specific reactant preparation in a molecular beam by rapid adiabatic pas ...

The dissociative chemisorption of methane on metal surfaces is of fundamental and practical interest, being a rate-limiting step in the steam reforming process. The reaction is best modeled with quantum dynamics calculations, but these are currently not gu ...

We report a molecular beam study of the effect of vibrational excitation on the physisorption of methane on a Pt(111) surface. Our experiments use a continuous molecular beam of CH4, prepared in its antisymmetic C-H stretch mode ν3 by infrared laser pumpin ...

Rainer Beck

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Highly Efficient Activation of HCl Dissociation on Au(111) via Rotational Preexcitation

State-resolved gas-surface reactivity of methane in the symmetric C-H stretch vibration on Ni(100)

State-Resolved Reactivity of CH4(2ν3) on Pt(111) and Ni(111): Effects of Barrier Height and Transition State Location

Double-resonance overtone photofragment spectroscopy of trans-HONO. II. State- and time-resolved dissociation and OH-product state distributions

Double-resonance overtone photofragment spectroscopy of trans-HONO. I. Spectroscopy and intramolecular dynamics

Unraveling the complexity of oxygen reactions on Pt surfaces

Quantum state specific reactant preparation in a molecular beam by rapid adiabatic passage

Quantum state resolved gas–surface reaction dynamics experiments: a tutorial review

Quantum-State Resolved Gas/Surface Dynamics Experiments

Alignment dependent chemisorption of vibrationally excited CH4(3) on Ni(100), Ni(110), and Ni(111)

Mode-specific reactivity of CH4 on Pt(110)-(1×2): The concerted role of stretch and bend excitation

Methane dissociation on the steps and terraces of Pt(211) resolved by quantum state and impact site

Bond selective dissociation of methane (CH3D) on the steps and terraces of Pt(211)

Site Selective Detection of Methane Dissociation on Stepped Pt Surfaces

Infrared Activities of Adsorbed Species on Metal Surfaces: The Puzzle of Adsorbed Methyl (CH3)

Probing Water Dissociation and Oxygen Replacement on Partially Oxygen-Covered Cu(111) by Reflection Absorption Infrared Spectroscopy

Quantum state-resolved gas/surface reaction dynamics probed by reflection absorption infrared spectroscopy

Ab Initio Molecular Dynamics Calculations versus Quantum-State- Resolved Experiments on CHD3 + Pt(111): New Insights into a Prototypical Gas−Surface Reaction

The Negligible Role of C-H Stretch Excitation in the Physisorption of CH4 on Pt(111)

Quantum state-resolved studies of gas/surface reaction dynamics by vibrational spectroscopies