Vanadium(V) oxide clusters synthesized by sublimation from bulk under fully inert conditions

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Abstract

Oxide nanoparticles in the size range of a few nanometers are typically synthesized in solution or via laser ablation techniques, which open numerous channels for structural change via chemical reactions or fragmentation processes. In this work, neutral vanadium oxide nanoparticles are instead synthesized by sublimation from bulk in combination with a pickup by superfluid helium droplets. Mass spectroscopy measurements clearly demonstrate the preservation of the bulk stoichiometric ratio of vanadium to oxygen in He-grown nanoparticles, indicating a tendency towards tetrahedral coordination of the vanadium centers in finite geometries. This unexpected finding opens up new possibilities for a combined on-the-fly synthesis of nanoparticles consisting of metal and metal-oxide layers. In comparison to mass spectra obtained via direct ionization of vanadium oxide in an effusive beam, where strong fragmentation occurred, we observe a clear preference for (V 2 O 5 ) n oligomers with even n inside the He nanodroplets, which is further investigated and explained using the electronic structure theory.

Original languageEnglish
Pages (from-to)3473-3480
Number of pages8
JournalChemical science
Volume10
Issue number12
DOIs
Publication statusPublished - 28 Mar 2019

Fingerprint

Vanadium
Sublimation
Oxides
Nanoparticles
Metals
Superfluid helium
Pickups
Laser ablation
Oligomers
Ionization
Electronic structure
Chemical reactions
Spectroscopy
Oxygen
Geometry

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

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title = "Vanadium(V) oxide clusters synthesized by sublimation from bulk under fully inert conditions",
abstract = "Oxide nanoparticles in the size range of a few nanometers are typically synthesized in solution or via laser ablation techniques, which open numerous channels for structural change via chemical reactions or fragmentation processes. In this work, neutral vanadium oxide nanoparticles are instead synthesized by sublimation from bulk in combination with a pickup by superfluid helium droplets. Mass spectroscopy measurements clearly demonstrate the preservation of the bulk stoichiometric ratio of vanadium to oxygen in He-grown nanoparticles, indicating a tendency towards tetrahedral coordination of the vanadium centers in finite geometries. This unexpected finding opens up new possibilities for a combined on-the-fly synthesis of nanoparticles consisting of metal and metal-oxide layers. In comparison to mass spectra obtained via direct ionization of vanadium oxide in an effusive beam, where strong fragmentation occurred, we observe a clear preference for (V 2 O 5 ) n oligomers with even n inside the He nanodroplets, which is further investigated and explained using the electronic structure theory.",
author = "Maximilian Lasserus and Martin Schnedlitz and Roman Messner and Florian Lackner and Ernst, {Wolfgang E.} and Hauser, {Andreas W.}",
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T1 - Vanadium(V) oxide clusters synthesized by sublimation from bulk under fully inert conditions

AU - Lasserus, Maximilian

AU - Schnedlitz, Martin

AU - Messner, Roman

AU - Lackner, Florian

AU - Ernst, Wolfgang E.

AU - Hauser, Andreas W.

PY - 2019/3/28

Y1 - 2019/3/28

N2 - Oxide nanoparticles in the size range of a few nanometers are typically synthesized in solution or via laser ablation techniques, which open numerous channels for structural change via chemical reactions or fragmentation processes. In this work, neutral vanadium oxide nanoparticles are instead synthesized by sublimation from bulk in combination with a pickup by superfluid helium droplets. Mass spectroscopy measurements clearly demonstrate the preservation of the bulk stoichiometric ratio of vanadium to oxygen in He-grown nanoparticles, indicating a tendency towards tetrahedral coordination of the vanadium centers in finite geometries. This unexpected finding opens up new possibilities for a combined on-the-fly synthesis of nanoparticles consisting of metal and metal-oxide layers. In comparison to mass spectra obtained via direct ionization of vanadium oxide in an effusive beam, where strong fragmentation occurred, we observe a clear preference for (V 2 O 5 ) n oligomers with even n inside the He nanodroplets, which is further investigated and explained using the electronic structure theory.

AB - Oxide nanoparticles in the size range of a few nanometers are typically synthesized in solution or via laser ablation techniques, which open numerous channels for structural change via chemical reactions or fragmentation processes. In this work, neutral vanadium oxide nanoparticles are instead synthesized by sublimation from bulk in combination with a pickup by superfluid helium droplets. Mass spectroscopy measurements clearly demonstrate the preservation of the bulk stoichiometric ratio of vanadium to oxygen in He-grown nanoparticles, indicating a tendency towards tetrahedral coordination of the vanadium centers in finite geometries. This unexpected finding opens up new possibilities for a combined on-the-fly synthesis of nanoparticles consisting of metal and metal-oxide layers. In comparison to mass spectra obtained via direct ionization of vanadium oxide in an effusive beam, where strong fragmentation occurred, we observe a clear preference for (V 2 O 5 ) n oligomers with even n inside the He nanodroplets, which is further investigated and explained using the electronic structure theory.

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