Temperature programmed desorption of weakly bound adsorbates on Au(111)

Engelhart, Daniel P.; Wagner, Roman J. V.; Meling, Artur; Wodtke, Alec M.; Schäfer, Tim

doi:10.1016/j.susc.2015.06.010

Cited by 33 publications

(57 citation statements)

References 33 publications

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“…Based on previous temperature programmed desorption (TPD) results for CO on Au(111) under low coverage situations (relevant for our work), the values of and des have been reported to be 2×10 15 Hz and 0.18 eV, respectively. 2 We point out that this previously published frequency factor (2×10 15 Hz) is erroneous, possibly due to a typographical error. As a consequence, we have re-analyzed the previously reported TPD results and find = 3 × 10 17 Hz.…”

Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 79%

“…We note that this value is consistent with that reported previously. 2 Using the relation = / , we obtain = 3 × 10 17 Hz.…”

Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 99%

“…For des , we obtain 0.18 eV, the same value as reported previously. 2 The TPD measurements in Ref 2 have been evaluated using the heating rate variation method, where a series of TPD traces are measured at several heating rates. For first order desorption processes (as is the case for CO/Au(111)) the following relation holds true:…”

Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 99%

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Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface

et al. 2018

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The most common mechanism of catalytic surface chemistry is that of Langmuir and Hinshelwood (LH). In the LH mechanism, reactants adsorb, become thermalized with the surface, and subsequently react. The measured vibrational (relaxation) lifetimes of molecules adsorbed at metal surfaces are in the range of a few picoseconds. As a consequence, vibrational promotion of LH chemistry is rarely observed, with the exception of LH reactions occurring via a molecular physisorbed intermediate. Here, we directly detect adsorption and subsequent desorption of vibrationally excited CO molecules from a Au(111) surface. Our results show that CO (v = 1) survives on a Au(111) surface for ~1 × 10 s. Such long vibrational lifetimes for adsorbates on metal surfaces are unexpected and pose an interesting challenge to the current understanding of vibrational energy dissipation on metal surfaces. They also suggest that vibrational promotion of surface chemistry might be more common than is generally believed.

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Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 79%

“…We note that this value is consistent with that reported previously. 2 Using the relation = / , we obtain = 3 × 10 17 Hz.…”

Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 99%

Section: (3) Estimating the Residence Time Of Co On Au(111) Surfacementioning

confidence: 99%

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Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface

et al. 2018

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“…46; NO on Au(111) (0.24 eV binding energy) is from ref. 47; and CO on Au(111) (0.18 eV binding energy 48 ) is from ref. 49.…”

Section: Discussionmentioning

confidence: 99%

An axis-specific rotational rainbow in the direct scatter of formaldehyde from Au(111) and its influence on trapping probability

Park

Krüger

Meyer

et al. 2017

Phys. Chem. Chem. Phys.

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The conversion of translational to rotational motion often plays a major role in the trapping of small molecules at surfaces, a crucial first step for a wide variety chemical processes that occur at gas-surface interfaces. However, to date most quantum-state resolved surface scattering experiments have been performed on diatomic molecules, and little detailed information is available about how the structure of nonlinear polyatomic molecules influences the mechanisms for energy exchange with surfaces. In the current work, we employ a new rotationally resolved 1 + 1' resonance-enhanced multiphoton ionization (REMPI) scheme to measure the rotational distribution in formaldehyde molecules directly scattered from the Au(111) surface at incidence kinetic energies in the range 0.3-1.2 eV. The results indicate a pronounced propensity to excite a-axis rotation (twirling) rather than b- or c-axis rotation (tumbling or cartwheeling), and are consistent with a rotational rainbow scattering model. Classical trajectory calculations suggest that the effect arises-to zeroth order-from the three-dimensional shape of the molecule (steric effects). Analysis suggests that the high degree of rotational excitation has a substantial influence on the trapping probability of formaldehyde at incidence translational energies above 0.5 eV.

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“…[10][11][12] Conversely, TPD requires the signal to be maximized, therefore a short sample detector distance, typically 1 mm, with a large entrance aperture is required. 13 Although TPD and MBS have been previously reported with the same detector, it has been at the expense of resolution. 14,15 This has led to systems being designed either for MBS or TPD or having separate chambers for TPD and MBS.…”

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confidence: 99%

Note: A versatile mass spectrometer chamber for molecular beam and temperature programmed desorption experiments

Tonks

Galloway

King

et al. 2016

Review of Scientific Instruments

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A dual purpose mass spectrometer chamber capable of performing molecular beam scattering (MBS) and temperature programmed desorption (TPD) is detailed. Two simple features of this design allow it to perform these techniques. First, the diameter of entrance aperture to the mass spectrometer can be varied to maximize signal for TPD or to maximize angular resolution for MBS. Second, the mass spectrometer chamber can be radially translated so that it can be positioned close to the sample to maximize signal or far from the sample to maximize angular resolution. The performance of this system is described and compares well with systems designed for only one of these techniques

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Temperature programmed desorption of weakly bound adsorbates on Au(111)

Cited by 33 publications

References 33 publications

Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface

Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface

An axis-specific rotational rainbow in the direct scatter of formaldehyde from Au(111) and its influence on trapping probability

Note: A versatile mass spectrometer chamber for molecular beam and temperature programmed desorption experiments

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