Photoionization spectroscopy of Ag–rare gas van der Waals complexes

Brock, L. R.; Duncan, M. A.

doi:10.1063/1.470031

Cited by 57 publications

(43 citation statements)

References 59 publications

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“…When a bound molecule crosses the Landau-Zener region, it spin flips with a probability calculated using Eqn. (24). Spin flips can occur both from the trapped to the untrapped state and vice versa.…”

Section: Adiabatic Transitionsmentioning

confidence: 99%

“…Examples include studies of NaNe and KAr via microwave spectroscopy 22,23 , CuAr 26 , AgAr 24 , and Ag 2 Ar 27 via two-photon ionization spectroscopy, AgAr via laser-induced fluorescence excitation spectroscopy 25 , and AuRg via multiphoton ionization spectroscopy 28,29 . These studies provide valuable spectroscopic information on fine and hyperfine interactions in vdW molecules in their ground 22,23 and excited 28,29 electronic states.…”

mentioning

confidence: 99%

“…(1) In a typical molecular beam experiment, vdW clusters are produced in a supersonic expansion of M + Rg mixtures and probed via laser spectroscopy [21][22][23][24][25] . Examples include studies of NaNe and KAr via microwave spectroscopy 22,23 , CuAr 26 , AgAr 24 , and Ag 2 Ar 27 via two-photon ionization spectroscopy, AgAr via laser-induced fluorescence excitation spectroscopy 25 , and AuRg via multiphoton ionization spectroscopy 28,29 .…”

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confidence: 99%

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Formation and dynamics of van der Waals molecules in buffer-gas traps

Brahms

Tscherbul

Zhang

et al. 2011

Phys. Chem. Chem. Phys.

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We show that weakly bound He-containing van der Waals molecules can be produced and magnetically trapped in buffer-gas cooling experiments, and provide a general model for the formation and dynamics of these molecules. Our analysis shows that, at typical experimental parameters, thermodynamics favors the formation of van der Waals complexes composed of a helium atom bound to most open-shell atoms and molecules, and that complex formation occurs quickly enough to ensure chemical equilibrium. For molecular pairs composed of a He atom and an S-state atom, the molecular spin is stable during formation, dissociation, and collisions, and thus these molecules can be magnetically trapped. Collisional spin relaxations are too slow to affect trap lifetimes. However, 3 He-containing complexes can change spin due to adiabatic crossings between trapped and untrapped Zeeman states, mediated by the anisotropic hyperfine interaction, causing trap loss. We provide a detailed model for Ag 3 He molecules, using ab initio calculation of Ag-He interaction potentials and spin interactions, quantum scattering theory, and direct Monte Carlo simulations to describe formation and spin relaxation in this system. The calculated rate of spin-change agrees quantitatively with experimental observations, providing indirect evidence for molecular formation in buffer-gas-cooled magnetic traps.The ability to cool and trap molecules holds great promise for new discoveries in chemistry and physics [1][2][3][4] . Cooled and trapped molecules yield long interaction times, allowing for precision measurements of molecular structure and interactions, tests of fundamental physics 5,6 , and applications in quantum information science 7 . Chemistry shows fundamentally different behavior for cold molecules 8 , and can be highly controlled based on the kinetic energy, external fields 9 , and quantum states 10 of the reactants.Experiments with cold molecules have thus far involved two classes of molecules: Feshbach molecules and deeply bound ground-state molecules. Feshbach molecules are highly vibrationally excited molecules, bound near dissociation, which interact only weakly at long range, due to small dipole moments. They are created by binding pairs of ultracold atoms using laser light (photoassociation), ac magnetic fields (rf as- . By contrast, ground-state heteronuclear molecules often have substantial dipole moments and are immune to spontaneous decay and vibrational relaxation, making these molecules more promising for applications in quantum information processing 7 and quantum simulation 11 . These molecules are either cooled from high temperatures using techniques such as buffer-gas cooling or Stark deceleration, or are created via coherent deexcitation of Feshbach molecules.This article introduces a third family to the hierarchy of trappable molecules -van der Waals (vdW) complexes. VdW molecules are bound solely by long-range dispersion interactions, leading to the weakest binding energies of any groundstate molecules, on the order of a wavenum...

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Section: Adiabatic Transitionsmentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Formation and dynamics of van der Waals molecules in buffer-gas traps

Brahms

Tscherbul

Zhang

et al. 2011

Phys. Chem. Chem. Phys.

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“…The curves shown are for Ag-Ar and represent those states explored experimentally by Jouvet et al [13] and by Brock and Duncan. [14] The same states have recently been the subject of a detailed computational study at the spin-unrestricted coupled cluster level (UCCSD(T)) by Loreau et al. [15] A different excited state labelling is employed by Loreau et al but we have adopted labels consistent with Brock and Duncan.…”

Section: Introductionmentioning

confidence: 99%

“…[13] The same transitions were subsequently studied by Brock and Duncan in a wider range of Ag-RG (RG=Ar, Kr, Xe) dimers by resonant two-photon ionization (R2PI). [14] Again, BirgeSponer and/or LeRoy-Bernstein [16,17] extrapolations were used to estimate the excited state dissociation thresholds which were then coupled with the well-known atomic energy levels permitting determination of the ground state dissociation energies.…”

Section: Introductionmentioning

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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