Mass-selected infrared photodissociation spectroscopy of V4O10+

Asmis, Knut R.; Brümmer, Mathias; Kaposta, Cristina; Santambrogio, Gabriele; Helden, Gert von; Meijer, Gerard; Rademann, Klaus; Wöste, L.

doi:10.1039/b111056j

Cited by 149 publications

(138 citation statements)

References 32 publications

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“…Its operation is very similar to the spectrometer described in Ref. 31 , in particular similar ion production and trapping settings were used, but it makes use of a conceptually different ion extraction / mass analyzing strategy. The h spectrometer, which more efficiently com pulsed laser experiments on the thermalized ions at defined tem description of this instrument will be part of a separate publication.…”

Section: Methodsmentioning

confidence: 99%

Vibrational signatures of hydrogen bonding in the protonated ammonia clusters NH4+(NH3)1−4

Yang

Kühn

Santambrogio

et al. 2008

The Journal of Chemical Physics

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The gas phase vibrational spectroscopy of the protonated ammonia dimer N 2 H 7 + , a prototypical system for strong hydrogen bonding, is studied in the spectral region from 330 to 1650 cm -1 by combining infrared multiple photon dissociation and multidimensional quantum mechanical simulations. The fundamental transition of the antisymmetric proton stretching vibration is observed at 374 cm -1 and assigned on the basis of a six-dimensional model Hamiltonian, which predicts this transition at 403 cm -1 . Photodissociation spectra of the larger protonated ammonia clusters NH 4 + (NH 3 ) n with n=2-4 are also reported for the range from 1050-1575 cm -1 . The main absorption features can be assigned within the harmonic approximation, supporting earlier evidence that hydrogen bonding in these clusters is considerably weaker than for n=1.

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Section: Methodsmentioning

confidence: 99%

Vibrational signatures of hydrogen bonding in the protonated ammonia clusters NH4+(NH3)1−4

Yang

Kühn

Santambrogio

et al. 2008

The Journal of Chemical Physics

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“…Recently, photodissociation spectroscopy [3][4][5][6] as well as resonance-enhanced multiple photon ionization [7][8][9] combined with radiation from a tunable infrared free electron laser have proven very useful in probing the structure of monometallic oxide clusters as a function of the cluster size. Here, we present the first systematic compositiondependent infrared study of bimetallic oxide clusters in the gas phase.…”

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confidence: 99%

Isomorphous Substitution in Bimetallic Oxide Clusters

et al. 2006

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The geometric and electronic structure of bimetallic oxide clusters is studied as a function of their composition with gas phase vibrational spectroscopy. Infrared multiple photon dissociation spectra of titanium-vanadium oxide cluster anions are measured in the 500 to 1200 wave number range and assigned on the basis of harmonic frequencies calculated using density functional theory. Singly substituted V 2 O 5 nÿ1 VTiO 5 ÿ (n 2-4) cluster anions are shown to form polyhedral caged structures similar to those predicted for their isoelectronic counterparts, the neutral V 2 O 5 n clusters. Upon systematic exchange of V by Ti atoms in V 4ÿn Ti n O ÿ 10 (n 1-4), the structure does not change. The stress induced by the isomorphous substitution results in an increased number of unpaired electrons (n ÿ 1) for the Ti-rich systems, leading to a quartet ground state for The size-and composition-dependent properties of gas phase transition metal oxide clusters are intensely studied, for example, to aid in the design of functional building blocks for nanostructured materials [1] and to gain a better understanding of the elementary steps in heterogeneous catalysis [2]. A long sought-after goal, in this regard, has been the tailoring of the electronic and geometric structure of clusters by carefully choosing the cluster composition. This approach has been limited up to now by both the availability of adequate cluster sources as well as structuresensitive characterization techniques.Recently, photodissociation spectroscopy [3-6] as well as resonance-enhanced multiple photon ionization [7][8][9] combined with radiation from a tunable infrared free electron laser have proven very useful in probing the structure of monometallic oxide clusters as a function of the cluster size. Here, we present the first systematic compositiondependent infrared study of bimetallic oxide clusters in the gas phase. The structures of titanium-vanadium oxide cluster anions are characterized by infrared multiple photon photodissociation (IRMPD) in combination with density functional theory (DFT) calculations. By sequentially exchanging V with Ti atoms we exploit the control over the clusters composition to investigate its influence on the electronic and geometric structure. Previously, IRMPD studies demonstrated that negatively charged V 2 O 5 ÿ n clusters (n 2-4) form polyhedral cages made of -O 3 V --O units [4]. Opposite to the neutral V 2 O 5 n cages [10], the anionic clusters are open shell systems; they have one unpaired electron in vanadium d states. While the unpaired electron is fully delocalized over all V atoms in n 2, it localizes on a single atom for the larger clusters [4]. Here we extend this study in two series of experiments. First, a single V atom is replaced by a Ti atom, yielding closed-shell V 2 O 5 nÿ1 VTiO 5 ÿ anions isoelectronic with the neutral V 2 O 5 n clusters. Second, the number of atoms is kept constant, but each V atom in V 4 O ÿ 10 is sequentially exchanged by a Ti atom, i.e., a stepwise removal of valence electrons. For ...

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“…9,10 The second goal is met by employing a cryogenically cooled, gas-filled ion trap. [11][12][13] Multiple collisions with cold He atoms will thermalize the ions close to the trap temperature. For multipole RF ion traps, ion temperatures below 10 K have been reported, sufficient to obtain vibrationally cold ions.…”

Section: Introductionmentioning

confidence: 99%

10 K Ring Electrode Trap—Tandem Mass Spectrometer for Infrared Spectroscopy of Mass Selected Ions

Goebbert

Meijer

Asmis

2009

AIP Conference Proceedings

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Abstract.A novel instrumental setup for measuring infrared photodissociation spectra of buffer gas cooled, mass-selected ions is described and tested. It combines a cryogenically cooled, linear radio frequency ion trap with a tandem mass spectrometer, optimally coupling continuous ion sources to pulsed laser experiments. The use of six independently adjustable DC potentials superimposed over the trapping radio frequency field provides control over the ion distribution within, as well as the kinetic energy distribution of the ions extracted from the ion trap. The scheme allows focusing the ions in space and time, such that they can be optimally irradiated by a pulsed, widely tunable infrared photodissociation laser. Ion intensities are monitored with a time-of-flight mass spectrometer mounted orthogonally to the ion trap axis.

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Mass-selected infrared photodissociation spectroscopy of V4O10+

Cited by 149 publications

References 32 publications

Vibrational signatures of hydrogen bonding in the protonated ammonia clusters NH4+(NH3)1−4

Vibrational signatures of hydrogen bonding in the protonated ammonia clusters NH4+(NH3)1−4

Isomorphous Substitution in Bimetallic Oxide Clusters

10 K Ring Electrode Trap—Tandem Mass Spectrometer for Infrared Spectroscopy of Mass Selected Ions

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