Adsorption dynamics of O<sub>2</sub> on Cu(111): a supersonic molecular beam study

Zhang, Diyu; Jansen, C.J.H.; Kleyn, Aart W.; Juurlink, Ludo B. F.

doi:10.1039/d3cp01215h

Cited by 7 publications

(9 citation statements)

References 45 publications

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“…During the expansion, kinetic and rotational energies are converted to translational energy along the beam axis, resulting in an average beam velocity of approximately 587 m/s as determined by time-offlight (TOF) spectrometry (see Supplementary Material S1). The rotational temperature within the beam is cooled to approximately 26 K [see ref (Jansen et al, 2023)].…”

Section: Methodsmentioning

confidence: 99%

“…For this experiment, we tune the laser to the R (4) transition at 4,249.99 nm, where CO 2 molecules are excited from the v = 0, J = 4 state to the v = 1, J = 5 state. This transition was chosen because J = 4 has the highest population at the rotational temperature of the molecular beam [see (Jansen et al, 2023)]. A cylindrical lens in the path of the laser is used to achieve rapid adiabatic passage (Jansen et al, 2023;Chadwick et al, 2014), resulting in nearly full (80%) population inversion.…”

Section: Methodsmentioning

confidence: 99%

“…This transition was chosen because J = 4 has the highest population at the rotational temperature of the molecular beam [see (Jansen et al, 2023)]. A cylindrical lens in the path of the laser is used to achieve rapid adiabatic passage (Jansen et al, 2023;Chadwick et al, 2014), resulting in nearly full (80%) population inversion. Considering the fractional population of the ground rotational state and the level of saturation, we excite approximately 15% of the CO 2 molecules in the molecular beam.…”

Section: Methodsmentioning

confidence: 99%

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State-resolved studies of CO2 sticking to CO2 ice

Jansen,

Juurlink

2023

Front. Chem.

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Internal vibrations may affect the adsorption, scattering, and reactions of molecules impinging onto a surface. The energy of the ν3 antisymmetric stretch vibration of CO2 slightly exceeds the desorption energy of CO2 bound to CO2 ice. We use supersonic molecular beam techniques and rovibrationally state-resolved excitation to determine whether this vibration affects condensation of gas phase CO2 to its ice. We detect sticking and CO2 ice formation using RAIRS and quantify the sticking probability using the King and Wells method with modulation of the vibrational excitation and Fourier transform based detection. We find that the influence of this vibration on the structure of the formed ice and on the sticking probability is negligible under our conditions. Based on our detection limit, we quantify the weighted average sticking probability at approximately 0.9 and the difference between the state-resolved and weighted average sticking probability as below 0.03%.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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State-resolved studies of CO2 sticking to CO2 ice

Jansen,

Juurlink

2023

Front. Chem.

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“…This value for E act agrees well with the one reported in recent sticking measurements of O 2 on Cu(111) using molecular beams. 38,39 Assuming the probability hypothesis of Fig. 1b, in which only those molecules with E kin > E act are active, K would equal the probability ( τ beam ) of about 0.3 eV for a Gaussian distribution with center at E kin = 0.24 eV and a full-width-half-maximum of 0.3 × E kin .…”

Section: Cu(111) Oxidation With Low-energy Molecular Beamsmentioning

confidence: 98%

Simulating high-pressure surface reactions with molecular beams

Taleb,

Schiller,

Vyalikh

et al. 2024

Phys. Chem. Chem. Phys.

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“…Contamination by O 2 is also a source of concern. Although the reactivity of Cu(111) toward dissociation and formation of a copper oxide skin seems mostly limited to defects sites when O 2 is dosed as a bulb gas, we have recently shown using supersonic molecular beam techniques that reactivity is highly dependent on kinetic energy . The dissociative sticking probability on the Cu(111) surface rapidly increases to values near unity in the range of 100–400 meV.…”

Section: Introductionmentioning

confidence: 98%

Characterization of CO Adsorbed to Clean and Partially Oxidized Cu(211) and Cu(111)

Zhang,

Virchenko,

Jansen

et al. 2023

J. Phys. Chem. C

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Copper-based catalysts gain activity through the presence of poorly coordinated Cu atoms and incomplete oxidation at the surface. The catalytic mechanisms can in principle be observed by controlled dosing of reactants to single-crystal substrates. However, the interconnected influences of surface defects, partial oxidation, and adsorbate coverage present a large matrix of conditions that have not been fully explored in the literature. We recently characterized oxygen and carbon monoxide coadsorption on Cu(111), a nominally defect-free surface, and now extend our study to the stepped surface Cu(211). Temperature-programmed desorption of CO adsorbed to bare metal surfaces confirms that two sites dominate desorption from a saturated layer: atop terrace atoms of local (111) character and atop step edge atoms with CO bound more strongly to the latter. At low coverage, discrete CO resonances in reflection adsorption infrared spectra can be assigned to these sites: 2077 cm –1 for extended (111) terraces, 2093 cm –1 for step sites, and additional kink-adsorbed molecules at 2110 cm –1 . With increasing coverage, in contrast to Cu(111), the infrared spectral features on Cu(211) evolve and shift as a consequence of dipole–dipole coupling between differentially occupied types of sites. Auger electron spectroscopy shows that exposure to background O 2 oxidizes the (211) surface at a rate nearly 1 order of magnitude greater than (111); we argue that the resulting surface is stoichiometric Cu 2 O, as previously found for Cu(111). This oxide binds CO less strongly than the bare metal and the underlying crystal cut continues to influence the adsorption sites available to CO. On oxidized (111) terraces, broad absorption peaks at 2115–2120 cm –1 ; on oxidized Cu(211), CO adsorbed to step sites appears as a resolved secondary peak at 2144 cm –1 . This suite of spectroscopic signatures, obtained under carefully controlled conditions, will help to determine the origin and fate of adsorbed species in future studies of reaction mechanisms on copper.

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Adsorption dynamics of O₂ on Cu(111): a supersonic molecular beam study

Abstract: We have studied the adsorption of O2 on Cu(111) using supersonic molecular beam techniques. For incident energies ranging between 100 and 400 meV, we have determined the sticking probability as...

Cited by 7 publications

References 45 publications

State-resolved studies of CO2 sticking to CO2 ice

State-resolved studies of CO2 sticking to CO2 ice

Simulating high-pressure surface reactions with molecular beams

Characterization of CO Adsorbed to Clean and Partially Oxidized Cu(211) and Cu(111)

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Adsorption dynamics of O2 on Cu(111): a supersonic molecular beam study

Abstract: We have studied the adsorption of O2 on Cu(111) using supersonic molecular beam techniques. For incident energies ranging between 100 and 400 meV, we have determined the sticking probability as...

Cited by 7 publications

References 45 publications

State-resolved studies of CO2 sticking to CO2 ice

State-resolved studies of CO2 sticking to CO2 ice

Simulating high-pressure surface reactions with molecular beams

Characterization of CO Adsorbed to Clean and Partially Oxidized Cu(211) and Cu(111)

Contact Info

Product

Resources

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Adsorption dynamics of O₂ on Cu(111): a supersonic molecular beam study