Production of bimetallic clusters by a dual-target dual-laser vaporization source

Bouwen, Wim; Thoen, Peter; Vanhoutte, Frederik; Bouckaert, Steven; Despa, Florin; Weidele, H.; Silverans, Roger; Lievens, Peter

doi:10.1063/1.1150159

Cited by 164 publications

(116 citation statements)

References 26 publications

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“…The experiments are performed in a molecular beam setup, which contains a dual laser vaporization source 54 and a time-offlight mass spectrometer equipped for infrared (IR) excitation experiments. 55 The setup has been connected to a beamline of the Free Electron Laser for Infrared eXperiments (FELIX) in Nieuwegein, which recently has been moved to the RU Nijmegen, the Netherlands.…”

Section: Experimental Methodsmentioning

confidence: 99%

Structural determination of niobium-doped silicon clusters by far-infrared spectroscopy and theory

Claes

Haertelt

et al. 2016

Phys. Chem. Chem. Phys.

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In this work, the structures of cationic Si n Nb + (n = 4-12) clusters are determined using the combination of infrared multiple photon dissociation (IR-MPD) and density functional theory (DFT) calculations. The experimental IR-MPD spectra of the argon complexes of Si n Nb + are assigned by comparison to the calculated IR spectra of low-energy structures of Si n Nb + that are identified using the stochastic 'random kick' algorithm in conjunction with the BP86 GGA functional. It is found that the Nb dopant tends to bind in an apex position of the Si n framework for n = 4-9 and in surface positions with high coordination numbers for n = 10-12. For the larger doped clusters, it is suggested that multiple isomers coexist and contribute to the experimental spectra. The structural evolution of Si n Nb + clusters is similar to V-doped silicon clusters (J. Am. Chem. Soc., 2010, 132, 15589-15602), except for the largest size investigated (n = 12), since V takes an endohedral position in Si 12 V + . The interaction with a Nb atom, with its partially unfilled 4d orbitals leads to a significant stability enhancement of the Si n framework as reflected, e.g. by high binding energies and large HOMO-LUMO gaps.

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Section: Experimental Methodsmentioning

confidence: 99%

Structural determination of niobium-doped silicon clusters by far-infrared spectroscopy and theory

Claes

Haertelt

et al. 2016

Phys. Chem. Chem. Phys.

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“…Mass spectrometric experiments are performed in a molecular beam setup, which contains a dual target-dual laser vaporization cluster source 19 and a time-of-flight mass spectrometer. Two independent Nd:YAG lasers vaporize the target materials and create a plasma.…”

Section: Experimental Methodsmentioning

confidence: 99%

Nature of the interaction between rare gas atoms and transition metal doped silicon clusters: the role of shielding effects

Ngân

Janssens

Claes

et al. 2015

Phys. Chem. Chem. Phys.

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Mass spectrometry experiments show an exceptionally weak bonding between Si 7 Mn + and rare gas atoms as compared to other exohedrally transition metal (TM) doped silicon clusters and other Si n Mn + (n = 5-10) sizes. The Si 7 Mn + cluster does not form Ar complexes and the observed fraction of Xe complexes is low. The interaction of two cluster series, Si n Mn + (n = 6-10) and Si 7 TM + (TM = Cr, Mn, Cu, and Zn), with Ar and Xe is investigated by density functional theory calculations. The cluster-rare gas binding is for all clusters, except Si 7 Mn + and Si 7 Zn + , predominantly driven by short-range interaction between the TM dopant and the rare gas atoms. A high s-character electron density on the metal atoms in Si 7 Mn + and Si 7 Zn + shields the polarization toward the rare gas atoms and thereby hinders formation of short-range complexes.Overall, both Ar and Xe complexes are similar except that the larger polarizability of Xe leads to larger binding energies.Atomic clusters emerge as interesting materials in the size regime between single atoms and nanoparticles, whose properties are strongly influenced by confinement effects. Understanding of their size and composition dependent structures and properties is primordial for further usage. The interactions between clusters and rare gas (RG) atoms are of crucial importance in many experimental techniques. For example, RG complexes are used for action spectroscopy in cluster science due to the inherent weak interaction, 1 Ar titration and tagging have been used to obtain isomer-specific photoelectron spectra for 2D and 3D gold clusters 2,3 and isomer selective infrared (IR) spectra of niobium clusters. 4 In most experimental studies, it has been assumed that the RG atoms do not significantly influence the intrinsic structure and properties of the bare clusters, and are therefore called messenger or spectator atoms. A negligible influence of the RG atoms is inferred from their low adsorption energies and from insignificant differences in measured IR spectra of elemental clusters and their Ar-complexes, such as for V n + , 5 Nb n + , 6 Ta n + (n = 6-20), 7 Si n + (n = 6-21), 8 as well as for binary Si n V + and Si n Cu + (n = 6-11) clusters. 9 Nevertheless, such an assumption is not always applicable. Stronger cluster-RG interactions, which cause discernible changes in the IR spectra of the bare clusters, were observed for some Co n + , Au n , and doped Au n Y clusters. 10-12 Moreover, the RG tagging of some oxide clusters changes the energetic ordering of the isomers, in which case a low-energetic structural isomer, and thus not the ground state structure of the bare cluster, is probed in the experiment. 13 A simple electrostatic picture was put forward to explain the stronger influence of the RG atom, analogous to models often used to interpret the interaction of RG atoms with metal surfaces 14 or metal complexes. 15 Much effort has been devoted to reveal the nature of interaction between RG and metal surfaces 12,16 or metal-atom complexes. 14,17 There are a...

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“…To produce mixed clusters, various approaches have been demonstrated, such as single targets of alloys [34], binary compounds [35][36][37], pressed mixed powders [38,39], and dual-target (dual-laser) sources [40][41][42][43][44]. The dual-target dual-laser source designs allow for controlling the mixing ratios by changing the laser fluences, laser timing, and the rotation and/or translation speeds of the targets.…”

Section: Introductionmentioning

confidence: 99%

Characterization of neutral boron-silicon clusters using infrared spectroscopy: The case of Si6B

Trường

Haertelt

Jaeger

et al. 2016

International Journal of Mass Spectrometry

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Nano-size clusters are of great interest for understanding of fundamental properties and processes relevant for applied materials science such as heterogeneous catalysis. In this study, we present a newly developed dualtarget dual-laser ablation source, suitable for the production of binary clusters and their spectroscopic characterization. With the current design, an almost arbitrary mixing ratio can be achieved by altering different parameters such as the laser fluences. Boron and silicon targets are chosen for cluster production, illustrating the possibility to control the outcome ranging from pure boron over mixed SinBm to pure silicon clusters. As a test system, Si6B clusters are characterized by means of infrared-ultraviolet two-color ionization (IR-UV2CI) spectroscopy, combined with quantum chemical simulations. The most stable structure of Si6B (Cs, 2 A') predicted in our previous work is confirmed by the present experiment. Doping of Si7 with a single B atom has a drastic impact on the geometric, vibrational, and electronic properties.

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Production of bimetallic clusters by a dual-target dual-laser vaporization source

Cited by 164 publications

References 26 publications

Structural determination of niobium-doped silicon clusters by far-infrared spectroscopy and theory

Structural determination of niobium-doped silicon clusters by far-infrared spectroscopy and theory

Nature of the interaction between rare gas atoms and transition metal doped silicon clusters: the role of shielding effects

Characterization of neutral boron-silicon clusters using infrared spectroscopy: The case of Si6B

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