GGSD

Lab Key visual
Chemical Dynamics at the Gas-Surface Interface – Probing and Controlling Surface Chemistry by Laser Radiation – Quantum State Resolved Surface Reactivity Measurements.

In our group, we study the elementary steps of chemical reactions between gas-phase molecules and solid surfaces such as the chemisorption of methane on a nickel catalyst. We use molecular beams and laser radiation to probe the reaction process at a molecular level by performing quantum state resolved reactivity measurements.

Journal Articles

2023

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

M. Suchodol; H. Vejayan; X. Zhou; B. Jiang; H. Guo et al. 

The Journal of Physical Chemistry Letters. 2023. Vol. 14, p. 7848-7853. DOI : 10.1021/acs.jpclett.3c02004.

Surface-induced vibrational energy redistribution in methane/surface scattering depends on catalytic activity

P. Floss; C. S. Reilly; D. J. Auerbach; R. D. Beck 

Frontiers in Chemistry. 2023. Vol. 11. DOI : 10.3389/fchem.2023.1238711.

Quantum state-resolved methane scattering from Ni(111) and NiO(111) by bolometer infrared laser tagging: The effect of surface oxidation

C. S. Reilly; P. Floss; B-J. Chen; D. J. Auerbach; R. D. Beck 

The Journal of Chemical Physics. 2023. Vol. 158, num. 21. DOI : 10.1063/5.0150009.

2022

Methylidyne Adsorption on Pt(211) Probed by Reflection Absorption Infrared Spectroscopy (RAIRS)

H. Vejayan; A. Gutiérrez-González; M. E. Torio; H. F. Busnengo; R. D. Beck 

The Journal of Physical Chemistry. 2022-12-04. DOI : 10.1021/acs.jpcc.2c07235.

2021

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

X. Zhou; H. Vejayan; R. D. Beck; H. Guo; B. Jiang 

The Journal of Physical Chemistry Letters. 2021-11-10. Vol. 12, num. 45, p. 11164-11169. DOI : 10.1021/acs.jpclett.1c03342.

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

N. Gerrits; J. Geweke; D. J. Auerbach; R. D. Beck; G-J. Kroes 

The Journal of Physical Chemistry Letters. 2021-07-27. Vol. 12, num. 30, p. 7252-7260. DOI : 10.1021/acs.jpclett.1c02093.

Dissociative Sticking Probability of Methane on Pt(110)-(2×1)

I. F. Peludhero; A. Gutiérrez-González; W. Dong; R. D. Beck; H. F. Busnengo 

The Journal of Physical Chemistry. 2021-05-31. Vol. 125, num. 22, p. 11904–11915. DOI : 10.1021/acs.jpcc.1c00807.

2020

State-to-state methane-surface scattering as a probe of catalytic activity

J. Werdecker; B-J. Chen; M. E. van Reijzen; A. Farjamnia; B. Jackson et al. 

Physical Review Research. 2020-11-18. Vol. 2, num. 4, p. 043251. DOI : 10.1103/PhysRevResearch.2.043251.

Quantum state and surface-site-resolved studies of methane chemisorption by vibrational spectroscopies

A. Gutiérrez-González; R. D. Beck 

Physical Chemistry Chemical Physics. 2020-07-29. Vol. 22, num. 31, p. 17448-17459. DOI : 10.1039/D0CP03134H.

2019

Unraveling the complexity of oxygen reactions on Pt surfaces

A. Gutiérrez González; R. D. Beck 

Proceedings of the National Academy of Sciences. 2019-07-02. Vol. 116, num. 28, p. 13727-13728. DOI : 10.1073/pnas.1908295116.

CHD3 Dissociation on the Kinked Pt(210) Surface: A Comparison of Experiment and Theory

H. Chadwick; A. Gutiérrez-González; R. D. Beck; G-J. Kroes 

The Journal of Physical Chemistry C. 2019-05-22. Vol. 123, num. 23, p. 14530-14539. DOI : 10.1021/acs.jpcc.9b03051.

Site Selective Detection of Methane Dissociation on Stepped Pt Surfaces

A. Gutiérrez González; M. E. Torio; H. F. Busnengo; R. D. Beck 

Topics in Catalysis. 2019-04-16. Vol. 62, p. 859–873. DOI : 10.1007/s11244-019-01170-5.

Transferability of the SRP32-vdW specific reaction parameter functional to CHD3 dissociation on Pt(110)-(2 × 1)

H. Chadwick; A. Gutiérrez-González; R. D. Beck; G-J. Kroes 

The Journal of Chemical Physics. 2019-03-25. Vol. 150, num. 12, p. 124702. DOI : 10.1063/1.5081005.

2018

Incident Angle Dependence of CHD3 Dissociation on the Stepped Pt(211) Surface

H. J. Chadwick; A. Gutiérrez González; D. Migliorini; R. D. Beck; G-J. Kroes 

Journal Physical Chemistry C. 2018-08-16. Vol. 122, num. 34, p. 19652-19660. DOI : 10.1021/acs.jpcc.8b05887.

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

A. Gutiérrez González; F. F. Crim; R. D. Beck 

Journal of Chemical Physics. 2018-08-16. Vol. 149, p. 074701. DOI : 10.1063/1.5041349.

Vibrational Energy Redistribution in a Gas-Surface Encounter: State-to-State Scattering of CH4 from Ni(111)

J. Werdecker; M. E. van Reijzen; B-J. Chen; R. D. Beck 

Physical Review Letters. 2018-01-31. Vol. 120, num. 5, p. 053402. DOI : 10.1103/PhysRevLett.120.053402.

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

H. Chadwick; H. Guo; A. Gutiérrez González; J. P. Menzel; B. Jackson et al. 

Journal of Chemical Physics. 2018. Vol. 148, p. 014701-9. DOI : 10.1063/1.5008567.

2017

Surface Reaction Barriometry: Methane Dissociation on Flat and Stepped Transition-Metal Surfaces

D. Migliorini; H. Chadwick; F. Nattino; A. Gutieŕrez-Gonzaĺez; E. Dombrowski et al. 

Journal of Physical Chemistry Letters. 2017. Vol. 8, p. 4177-82. DOI : 10.1021/acs.jpclett.7b01905.

Quantum State–Resolved Studies of Chemisorption Reactions

H. Chadwick; R. D. Beck 

Annual Review of Physical Chemistry. 2017. Vol. 68, p. 39-61. DOI : 10.1146/annurev-physchem-052516-044910.

Dynamics of methane dissociation on transition metals

A. C. Luntz; R. D. Beck 

Journal of Vacuum Science and Technology A. 2017. Vol. 35, num. 5, p. 05C201-05C206. DOI : 10.1116/1.4980145.

Quantum-state-resolved reactivity of overtone excited CH4 on Ni(111): Comparing experiment and theory

P. M. Hundt; M. E. van Reijzen; R. D. Beck; H. Guo; B. Jackson 

Journal of Chemical Physics. 2017. Vol. 146, p. 054701. DOI : 10.1063/1.4975025.

2016

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

H. J. Chadwick; A. Gutiérrez-Gonzalez; R. D. Beck 

Journal of Chemical Physics. 2016. Vol. 145, p. 174707. DOI : 10.1063/1.4966921.

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

H. J. Chadwick; R. D. Beck 

Chemical Society Reviews. 2016. Vol. 45, num. 13, p. 3576-3594. DOI : 10.1039/C5CS00476D.

2015

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

H. Ueta; L. Chen; R. D. Beck 

Journal of the surface science society of Japan. 2015. Vol. 36, num. 12, p. 614-619. DOI : 10.1380/jsssj.36.614.

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

P. M. Hundt; H. Ueta; M. E. Van Reijzen; B. Jiang; H. Gou et al. 

Journal of Physical Chemistry A. 2015. Vol. 119, num. 50, p. 12442-12448. DOI : 10.1021/acs.jpca.5b07949.

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

L. Chen; H. Ueta; H. J. Chadwick; R. D. Beck 

Journal of Physical Chemistry C. 2015. Vol. 119, num. 26, p. 14499-14505. DOI : 10.1021/jp5064897.

2014

Vibrational Activation of Methane Chemisorption: The Role of Symmetry

P. M. Hundt; M. E. Van Reijzen; H. Ueta; R. D. Beck 

Journal of Physical Chemistry Letters. 2014. Vol. 5, p. 1963-67. DOI : 10.1021/jz500728d.

Vibrationally Promoted Dissociation of Water on Ni(111)

P. M. Hundt; B. Jiang; V. Reijzen; M. Eduard; H. Guo et al. 

Science. 2014. Vol. 344, num. 6183, p. 504-507. DOI : 10.1126/science.1251277.

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

F. Nattino; H. Ueta; H. J. Chadwick; V. Reijzen; M. Eduard et al. 

Journal of Physical Chemistry Letters. 2014. Vol. 5, p. 1294−1299. DOI : 10.1021/jz500233n.

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

H. J. Chadwick; P. M. Hundt; V. Reijzen; M. Eduard; B. L. Yoder et al. 

Journal of Chemical Physics. 2014. Vol. 140, p. 034321. DOI : 10.1063/1.4861054.

2013

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

H. Ueta; L. Chen; R. D. Beck; I. Colon-Diaz; B. Jackson 

Physical Chemistry Chemical Physics. 2013. Vol. 15, p. 20526-20535. DOI : 10.1039/c3cp52244j.

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

L. Chen; H. Ueta; R. Bisson; R. D. Beck 

Review of Scientific Instruments. 2013. Vol. 84, p. 053902. DOI : 10.1063/1.4803933.

2012

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

P. M. Hundt; R. Bisson; R. D. Beck 

Journal of Chemical Physics. 2012. Vol. 137, p. 074701. DOI : 10.1063/1.4742914.

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

L. Chen; H. Ueta; R. Bisson; R. D. Beck 

Faraday Discussions- Royal Society of Chemistry. 2012. Vol. 157, p. 285-295. DOI : 10.1039/C2FD20007D.

2011

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

B. Yoder; R. Bisson; P. M. Hundt; R. D. Beck 

Journal of Chemical Physics. 2011. Vol. 135, p. 224703. DOI : 10.1063/1.3665136.

2010

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

R. Bisson; M. Sacchi; R. D. Beck 

Physical Review -Series B-. 2010. Vol. 82, num. 12, p. 121404(R). DOI : 10.1103/PhysRevB.82.121404.

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

B. Yoder; R. Bisson; R. D. Beck 

Science. 2010. Vol. 329, p. 553. DOI : 10.1126/science.1191751.

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

R. Bisson; M. Sacchi; R. D. Beck 

Journal of Chemical Physics. 2010. Vol. 132, num. 9, p. 094702. DOI : 10.1063/1.3328885.

2008

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

R. Bisson; T. T. Dang; M. Sacchi; R. D. Beck 

Journal of Chemical Physics. 2008. Vol. 129, num. 8, p. 081103. DOI : 10.1063/1.2976563.

2007

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

R. Bisson; M. Sacchi; T. T. Dang; B. Yoder; P. Maroni et al. 

Journal of Physical Chemistry A. 2007. Vol. 111, num. 49, p. 12679-12683. DOI : 10.1021/jp076082w.

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

R. Bisson; T. T. Dang; M. Sacchi; R. D. Beck 

Journal of Chemical Physics. 2007. Vol. 127, num. 24, p. 244301. DOI : 10.1063/1.2819072.

2006

Efficient Stimulated Raman Pumping for Quantum-State Resolved Surface Reactivity Measurements

P. Maroni; D. Papageorgopoulos; A. Ruf; R. D. Beck; T. R. Rizzo 

Review of Scientific Instruments. 2006. Vol. 77, p. 054103. DOI : 10.1063/1.2200876.

Infrared spectroscopy of hydrated amino acids in the gas phase: protonated and lithiated valine

A. Kamariotis; O. V. Boyarkin; S. R. Mercier; R. D. Beck; M. F. Bush et al. 

Journal of the American Chemical Society. 2006. Vol. 128, p. 905. DOI : 10.1021/ja056079v.

2005

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

P. Maroni; D. C. Papageorgopoulos; M. Sacchi; T. T. Dang; R. D. Beck et al. 

Physical Review Letters. 2005. Vol. 94, num. 24, p. 246104. DOI : 10.1103/PhysRevLett.94.246104.

2004

Quantum state resolved studies of gas/surface reaction dynamics

R. D. Beck; T. Rizzo 

Chimia. 2004. Vol. 58, num. 5, p. 306-310. DOI : 10.2533/000942904777677867.

2003

Vibrational mode-specific reaction of methane on a nickel surface

R. D. Beck; P. Maroni; D. Papageorgopoulos; T. Dang; M. Schmid et al. 

Science. 2003. Vol. 302, num. 5642, p. 98. DOI : 10.1126/science.1088996.

Molecular-beam/surface-science apparatus for state-resolved chemisorption studies using pulsed-laser preparation

M. P. Schmid; P. Maroni; R. D. Beck; T. R. Rizzo 

Review of Scientific Instruments. 2003. Vol. 74, num. 9, p. 4110-4120. DOI : 10.1063/1.1599064.

2002

Surface reactivity of highly vibrationally excited molecules prepared by pulsed laser excitation: CH4 (2 nu(3)) on Ni(100)

M. Schmid; P. Maroni; R. D. Beck; T. Rizzo 

Journal of Chemical Physics. 2002. Vol. 117, num. 19, p. 8603-8606. DOI : 10.1063/1.1519860.

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

F. Reiche; B. Abel; R. D. Beck; T. Rizzo 

Journal of Chemical Physics. 2002. Vol. 116, num. 23, p. 10267. DOI : 10.1063/1.1471236.

2000

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

F. Reiche; B. Abel; R. D. Beck; T. R. Rizzo 

Journal of Chemical Physics. 2000. Vol. 112, num. 20, p. 8885-8898. DOI : 10.1063/1.481502.

Conference Papers

2019

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

R. Beck 

2019-03-31. National Meeting of the American-Chemical-Society (ACS), Orlando, FL, Mar 31-Apr 04, 2019.

Theses

2023

Gas/Surface reactions probed by reflection absorption infrared spectroscopy

H. Vejayan / R. Beck (Dir.)  

Lausanne, EPFL, 2023. 

2022

State-to-state surface scattering of methane studied by bolometric infrared laser tagging detection

B-J. Chen / R. Beck (Dir.)  

Lausanne, EPFL, 2022. 

2019

Scattering HCl Molecules from Au(111) and Ag(111) Surfaces

J. D. Geweke / A. Wodtke; R. Beck (Dir.)  

Lausanne, EPFL, 2019. 

Bond-selective and surface-site-specific dissociation of methane on platinum

A. Gutiérrez González / R. Beck (Dir.)  

Lausanne, EPFL, 2019. 

2018

Vibrationally and Rotationally Inelastic Scattering of Methane from Ni(111)

J. Werdecker / R. D. Beck; A. Wodtke (Dir.)  

Lausanne, EPFL, 2018. 

2016

State-to-state scattering of CH₄ from Ni(111) and Gr/Ni(111)

M. E. van Reijzen / R. D. Beck (Dir.)  

Lausanne, EPFL, 2016. 

2014

Quantum-state resolved gas/surface reaction dynamics of water and methane

P. M. Hundt / R. D. Beck (Dir.)  

Lausanne, EPFL, 2014. 

2012

Vibrationally Bond-Selective Chemisorption of Methane Isotopologues on Pt(111) Studied by Reflection Absorption Infrared Spectroscopy

L. Chen / R. D. Beck (Dir.)  

Lausanne, EPFL, 2012. 

2010

Steric Effects in the Chemisorption of Vibrationally Excited Methane on Nickel

B. Yoder / R. D. Beck (Dir.)  

Lausanne, EPFL, 2010. 

2008

The effect of molecular vibrations and surface structure on the chemisorption of methane on platinum

M. Sacchi / R. D. Beck (Dir.)  

Lausanne, EPFL, 2008. 

2007

Quantum state-resolved studies of direct and precursor-mediated dissociative chemisorption of silane on Si(100)

T. T. Dang / R. D. Beck (Dir.)  

Lausanne, EPFL, 2007. 

2005

Bond- and mode-specific reactivity of methane on Ni(100)

P. Maroni / R. D. Beck (Dir.)  

Lausanne, EPFL, 2005. 

Book Chapters

2013

Quantum-State Resolved Gas/Surface Dynamics Experiments

R. D. Beck; A. L. Utz 

Dynamics of Gas-Surface Interactions: Atomic-level Understanding of Scattering Processes at Surfaces; Springer, 2013. p. 179-212.