A velocity map imaging study of gold-rare gas complexes: Au–Ar, Au–Kr, and Au–Xe

Hopkins, W. Scott; Woodham, Alex P.; Plowright, Richard J.; Wright, Timothy G.; Mackenzie, Stuart R.

doi:10.1063/1.3432127

Cited by 20 publications

(43 citation statements)

References 37 publications

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“…The resulting parameters have been compiled in Table 1 and compared with experimental data. 44 Table 1 and Figure 1 show that the DFT-based results are mainly out of the range from the RCCSD(T) CBS counterpart. The revPBE and PBE well depths are more than 8 meV less attractive whereas D e (PBEsol) is too large by more than 7 meV, with the equilibrium distance r e being ∼0.5 Å too short.…”

Section: The Isolated Ar + Au Diatomic Systemmentioning

confidence: 88%

“…Only the vdWOptB86b approach produces D e and r e values in close agreement with the RCCSD(T) CBS benchmarking. However, the medium-and long-range attractive tail of the vdW-OptB86b 44 18.5 ± 2 a REMPI exp 45 16.12 ± 2 a RCCSD(Val,T)/d-awCV∞Z 46 22.91 3.711 potential decays much more slowly than that of the RCCSD(T) CBS potential (Figure 1), as reflected in the large differences between the C 6 and C 8 values ( Table 1). As can be seen in Table 1, the values of the PBE-D3 and vdW-DF2 C 6 coefficients are the closest ones to the corresponding RCCSD(T) CBS value.…”

Section: The Isolated Ar + Au Diatomic Systemmentioning

confidence: 90%

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Argon Interaction with Gold Surfaces: Ab Initio-Assisted Determination of Pair Ar–Au Potentials for Molecular Dynamics Simulations

Grenier

Lara‐Castells

et al. 2015

J. Phys. Chem. A

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Global potentials for the interaction between the Ar atom and gold surfaces are investigated and Ar-Au pair potentials suitable for molecular dynamics simulations are derived. Using a periodic plane-wave representation of the electronic wave function, the nonlocal van-der-Waals vdW-DF2 and vdW-OptB86 approaches have been proved to describe better the interaction. These global interaction potentials have been decomposed to produce pair potentials. Then, the pair potentials have been compared with those derived by combining the dispersionless density functional dlDF for the repulsive part with an effective pairwise dispersion interaction. These repulsive potentials have been obtained from the decomposition of the repulsive interaction between the Ar atom and the Au2 and Au4 clusters and the dispersion coefficients have been evaluated by means of ab initio calculations on the Ar+Au2 complex using symmetry adapted perturbation theory. The pair potentials agree very well with those evaluated through periodic vdW-DF2 calculations. For benchmarking purposes, CCSD(T) calculations have also been performed for the ArAu and Ar+Au2 systems using large basis sets and extrapolations to the complete basis set limit. This work highlights that ab initio calculations using very small surface clusters can be used either as an independent cross-check to compare the performance of state-of-the-art vdW-corrected periodic DFT approaches or, directly, to calculate the pair potentials necessary in further molecular dynamics calculations.

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Section: The Isolated Ar + Au Diatomic Systemmentioning

confidence: 88%

Section: The Isolated Ar + Au Diatomic Systemmentioning

confidence: 90%

Argon Interaction with Gold Surfaces: Ab Initio-Assisted Determination of Pair Ar–Au Potentials for Molecular Dynamics Simulations

Grenier

Lara‐Castells

et al. 2015

J. Phys. Chem. A

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“…Unlike in the case of Au-RG dimers we have studied previously, [21] no dissociation of the bound A ( 2 ) state levels was observed.…”

Section: Methodsmentioning

confidence: 57%

“…[20,21,26] Briefly, silver atoms are generated by laser ablation of a rotating silver metal target and entrained in a pulsed molecular beam of either pure or mixed rare gases delivered via a Jordan valve. For the studies of Ag-Ar pure argon carrier gas was used.…”

Section: Methodsmentioning

confidence: 99%

Dissociation energies of Ag–RG (RG = Ar, Kr, Xe) and AgO molecules from velocity map imaging studies

Cooper¹,

Kartouzian

Gentleman³

et al. 2015

The Journal of Chemical Physics

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The near ultraviolet photodissociation dynamics of silver atom -rare gas dimers have been studied by velocity map imaging. Ag-RG (RG = Ar, Kr, Xe) species generated by laser ablation are excited in the region of the C ( 2  + )  X ( 2  + ) continuum leading to direct, near-threshold dissociation generating Ag* ( 2 P 3/2 ) + RG ( 1 S 0 ) products. Images recorded at excitation wavelengths throughout the C ( 2  + )  X ( 2  + ) continuum, coupled with known atomic energy levels, permit determination of the ground X ( 2  + ) state dissociation energies of 85.9 ± 23.4 cm -1 (Ag-Ar), 149.3 ± 22.4 cm -1 (Ag-Kr) and 256.3 ± 16.0 cm -1 (Ag-Xe). Three additional photolysis processes, each yielding Ag atom photoproducts, are observed in the same spectral region. Two of these are markedly enhanced in intensity upon seeding the molecular beam with nitrous oxide, and are assigned to photodissociation of AgO at the two-photon level. These features yield an improved ground state dissociation energy for AgO of 15965  81 cm -1 , which is in good agreement with high level calculations. The third process results in Ag atom fragments whose kinetic energy shows anomalously weak photon energy dependence and is assigned tentatively to dissociative ionization of the silver dimer Ag 2 .3

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“…No attempt was made to clean up the polarization after the lens but we believe any polarization spoiling to be minimal as we have previously observed limiting values for anisotropy parameters with its use in this spectral region. 10,11 The instrument operates in both linear time-of-flight and VMI modes. In linear ToF mode, the mass resolving power of the instrument is sufficient to observe the different isotopes (isotopologues) of Xe (Xe 2 ).…”

mentioning

confidence: 99%

Communication: Imaging wavefunctions in dissociative photoionization

Hopkins

Mackenzie²

2011

The Journal of Chemical Physics

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The dissociative ionization dynamics of excited electronic states of the xenon dimer, Xe2, have been studied using velocity map ion imaging (VMI). A one-colour, (2+1) resonant excitation scheme was employed to first excite and then ionize selected vibrational levels of the Xe2 6p 2[1/2]0 $0_g^ +$0g+ Rydberg state. Cationic fragments were then detected by the VMI. The data provide an outstanding example of the reflection principle in photodissociation with the full nodal structure of the Rydberg state wavefunctions clearly observed in the final Xe+ kinetic energy distributions without the need for scanning the excitation energy. Fitting of the observed distributions provides detailed and precise information on the form of the Xe2+ I(1/2g) potential energy curve involved which is in excellent agreement with the results of photoelectron imaging studies [Shubert and Pratt, J. Chem. Phys. 134, 044315 (2011) 10.1063/1.3533361]. Furthermore, the anisotropy of the product angular distributions yields information on the evolution of the electronic character of the ionic state with internuclear separation, R. The combination of the nature of dissociative ionization and the extent of the bound state wavefunctions provide information over an unusually wide range of internuclear separation R (ΔR > 0.75 Å). This would normally require scanning over a considerable energy region but is obtained in these studies at a fixed excitation energy.

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A velocity map imaging study of gold-rare gas complexes: Au–Ar, Au–Kr, and Au–Xe

Cited by 20 publications

References 37 publications

Argon Interaction with Gold Surfaces: Ab Initio-Assisted Determination of Pair Ar–Au Potentials for Molecular Dynamics Simulations

Argon Interaction with Gold Surfaces: Ab Initio-Assisted Determination of Pair Ar–Au Potentials for Molecular Dynamics Simulations

Dissociation energies of Ag–RG (RG = Ar, Kr, Xe) and AgO molecules from velocity map imaging studies

Communication: Imaging wavefunctions in dissociative photoionization

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