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Rainer Beck

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Publications associées (44)

Dynamics of methane dissociation on transition metals

Rainer Beck

One of the many contributions of Harold Winters to surface science was his pioneering ultrahigh vacuum study on the kinetics of the technologically important dissociation of CH4 on transition metals in the 1970s. He observed a dramatic activation of the di ...

A V S Amer Inst Physics2017

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

Rainer Beck, Helen Jane Chadwick

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 ...

Royal Society of Chemistry2016

Quantum state resolved molecular beam reflectivity measurements: CH4 dissociation on Pt(111)

Rainer Beck, Helen Jane Chadwick, Ana Gutiérrez González

The King and Wells molecular beam reflectivity method has been used for a quantum state resolved study of the dissociative chemisorption of CH4 on Pt(111) at several surface temperatures. Initial sticking coefficients were measured for incident CH4 prepare ...

American Institute of Physics2016

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

Rainer Beck, Hirokazu Ueta, Li Chen, Helen Jane Chadwick

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 ...

American Chemical Society2015

State-Resolved Methane Dissociation on Pt(111) Studied by Reflection Absorption Infrared Spectroscopy

Rainer Beck, Hirokazu Ueta, Li Chen

The dissociation of methane on Pt(111) was studied using quantum state-resolved methods and reflection absorption infrared spectroscopy (RAIRS), at a surface temperature of 150 K where the nascent reaction products methyl(ads) and H(ads) are stable and acc ...

2015

Bond-Selective and Mode-Specific Dissociation of CH3D and CH2D2 on Pt(111)

Rainer Beck, Phil Morten Hundt, Hirokazu Ueta, Maarten Eduard van Reijzen

Infrared laser excitation of partially deuterated methanes (CH3D and CH2D2) in a molecular beam is used to control their dissociative chemisorption on a Pt(111) single crystal and to determine the quantum state-resolved dissociation probabilities. The excl ...

American Chemical Society2015

Vibrational Activation of Methane Chemisorption: The Role of Symmetry

Rainer Beck, Phil Morten Hundt, Hirokazu Ueta, Maarten Eduard van Reijzen

Quantum state-resolved reactivity measurements probe the role of vibrational symmetry on the vibrational activation of the dissociative chemisorption of CH4 on Pt(111). IR–IR double resonance excitation in a molecular beam is used to prepare CH4 in all thr ...

Amer Chemical Soc2014

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

Rainer Beck, Hirokazu Ueta, Maarten Eduard van Reijzen, Helen Jane Chadwick, Francesco Nattino

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 ...

Amer Chemical Soc2014

Vibrationally Promoted Dissociation of Water on Ni(111)

Rainer Beck, Phil Morten Hundt, Maarten Eduard van Reijzen

Water dissociation on transition-metal catalysts is an important step in steam reforming and the water-gas shift reaction. To probe the effect of translational and vibrational activation on this important heterogeneous reaction, we performed state-resolved ...

American Association for the Advancement of Science2014

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

Rainer Beck, Bruce Yoder, Phil Morten Hundt, Maarten Eduard van Reijzen, Helen Jane Chadwick

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 ...

American Institute of Physics2014

Quantum state-resolved CH4 dissociation on Pt(111): coverage dependent barrier heights from experiment and density functional theory

Rainer Beck, Hirokazu Ueta, Li Chen

The dissociative chemisorption of CH4 on Pt(111) was studied using quantum state-resolved methods at a surface temperature (Ts) of 150 K where the nascent reaction products CH3(ads) and H(ads) are stable and accumulate on the surface. Most previous experim ...

Royal Society of Chemistry2013

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

Rainer Beck, Régis Bisson, Hirokazu Ueta, Li Chen

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 ...

American Institute of Physics2013

Vibrationally bond-selected chemisorption of methane isotopologues on Pt(111) studied by reflection absorption infrared spectroscopy

Rainer Beck, Régis Bisson, Hirokazu Ueta, Li Chen

Reflection absorption infrared spectroscopy (RAIRS) was used to probe for vibrational bond-selectivity in the dissociative chemisorption of three partially deuterated methane isotopologues on a Pt(111) surface. While a combination of incident translational ...

Royal Society of Chemistry2012

The sticking probability of D2O-water on ice: Isotope effects and the inﬂuence of vibrational excitation

Rainer Beck, Régis Bisson, Phil Morten Hundt

The present study measures the sticking probability of heavy water (D2O) on H2O- and on D2O-ice and probes the inﬂuence of selective OD-stretch excitation on D2O sticking on these ices. Molecular beam techniques are combined with infrared laser excitation ...

American Institute of Physics2012

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

Rainer Beck, Régis Bisson, Bruce Yoder, Phil Morten Hundt

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 ...

American Institute of Physics2011

Steric Effects in the Chemisorption of Vibrationally Excited Methane on Ni(100)

Rainer Beck, Régis Bisson, Bruce Yoder

Newly available, powerful infrared laser sources enable the preparation of intense molecular beams of quantum-state prepared and aligned molecules for gas/surface reaction dynamics experiments. We present a stereodynamics study of the chemisorption of vibr ...

American Association for the Advancement of Science2010

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

Rainer Beck, Marco Sacchi, Régis Bisson

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 ...

American Physical Society2010

State-resolved reactivity of CH4 on Pt(110)-(1 x 2): The role of surface orientation and impact site

Rainer Beck, Marco Sacchi, Régis Bisson

The reactivity of methane (CH4) on Pt(110)-(1×2) has been studied by quantum state-resolved surface reactivity measurements. Ground state reaction probabilities, S0(v=0) ~ S0(laser-off), as well as state-resolved reaction probabilities S0(2v3), for CH4 exc ...

2010

Vibrational Activation in Direct and Precursor-Mediated Chemisorption of SiH4 on Si(100)

Rainer Beck, Thanh Tung Dang, Marco Sacchi, Régis Bisson

The quantum state-resolved reactivity S0 of SiH4 on Si(100)-2x1 has been measured for the first time for two vibrationally excited Si-H stretch local mode states (|2000> and |1100>) as well the ground state S0 as a function of translational energy En and s ...

2008

Cavity ring-down spectroscopy of jet-cooled silane isotopologues in the Si-H stretch overtone region

Rainer Beck, Thanh Tung Dang, Marco Sacchi, Régis Bisson

Absorption spectra of silane in the region of the first overtone of the Si-H stretch vibration have been recorded in a seeded supersonic jet expansion by cavity ring-down spectroscopy as well as in a static gas cell at room temperature by photoacoustic spe ...

2007

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