&lt;em&gt;In Situ&lt;/em&gt; SIMS and IR Spectroscopy of Well-defined Surfaces Prepared by Soft Landing of Mass-selected Ions

Johnson, Grant E.; Gunaratne, K. Don Dasitha; Laskin, Julia

doi:10.3791/51344

Cited by 2 publications

(2 citation statements)

References 131 publications

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“…These soft landing experiments were performed with a custom-built instrument coupled to a commercial TOF-SIMS which has been described in detail previously. 187,202 A schematic illustration of the soft landing instrument is provided in Figure 8. Ligated gold clusters synthesized in solution are introduced into the gas phase using ESI 119 and a high transmission electrodynamic ion funnel.…”

Section: Sl Of Mass-selected Clustersmentioning

confidence: 99%

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Understanding ligand effects in gold clusters using mass spectrometry

Johnson

Laskin

2016

Analyst

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This review summarizes recent research on the influence of phosphine ligands on the size, stability, and reactivity of gold clusters synthesized in solution. Sub-nanometer clusters exhibit size- and composition-dependent properties that are unique from those of larger nanoparticles. The highly tunable properties of clusters and their high surface-to-volume ratio make them promising candidates for a variety of technological applications. However, because "each-atom-counts" toward defining cluster properties it is critically important to develop robust synthesis methods to efficiently prepare clusters of predetermined size. For decades phosphines have been known to direct the size-selected synthesis of gold clusters. Despite the preparation of numerous species it is still not understood how different functional groups at phosphine centers affect the size and properties of gold clusters. Using electrospray ionization mass spectrometry (ESI-MS) it is possible to characterize the effect of ligand substitution on the distribution of clusters formed in solution at defined reaction conditions. In addition, ligand exchange reactions on preformed clusters may be monitored using ESI-MS. Collision induced dissociation (CID) may also be employed to obtain qualitative insight into the fragmentation of mixed ligand clusters and the relative binding energies of differently substituted phosphines. Quantitative ligand binding energies and cluster stability may be determined employing surface induced dissociation (SID) in a custom-built Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR-MS). Rice-Ramsperger-Kassel-Marcus (RRKM) based modeling of the SID data allows dissociation energies and entropy values to be extracted. The charge reduction and reactivity of atomically precise gold clusters, including partially ligated species generated in the gas-phase by in source CID, on well-defined surfaces may be explored using ion soft landing (SL) in a custom-built instrument combined with in situ time of flight secondary ion mass spectrometry (TOF-SIMS). Jointly, this multipronged experimental approach allows characterization of the full spectrum of relevant phenomena including cluster synthesis, ligand exchange, thermochemistry, surface immobilization, and reactivity. The fundamental insights obtained from this work will facilitate the directed synthesis of gold clusters with predetermined size and properties for specific applications.

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Section: Sl Of Mass-selected Clustersmentioning

confidence: 99%

“…These SL experiments were performed with a custom-built instrument coupled to a commercial TOF-SIMS which has been described in detail previously. 187,202 A schematic illustration of the soft landing instrument is provided in Fig. 8.…”

Section: Sl Of Mass-selected Clustersmentioning

confidence: 99%

Understanding ligand effects in gold clusters using mass spectrometry

Johnson

Laskin

2016

Analyst

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Formation and characterization of polymetallic {CrxMy} rings in vacuo

Geue,

Timco,

Whitehead

et al. 2023

Nat. Synth

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Understanding the (dis)assembly mechanisms of large metallosupramolecules is critical in their design, stability and application. The inherent complexity of these structures leads to many potential pathways for combining (or separating) the constituent building blocks, which makes this task difficult. Here we use collision-induced dissociation mass spectrometry to study the disassembly of heterometallic complexes. Collisional activation leads to the formation of a series of previously unknown smaller ring products and we characterize their geometry using ion mobility. The disassembly of both {CrxCu2} hourglass structures (x = 10, 12) and of a {Cr12Gd4} cluster shows the formation of rare closed, heptametallic species {Cr6Cu}, {Cr5Cu2} and {Cr5Gd2} as dominant products, as well as other closed ions such as {Cr5Cu}, {Cr10Cu}, {Cr12Cu}, {Cr10}, {Cr12} and {Cr6Gd2}. The collision cross-section of cyclic products and precursors has a linear correlation with ion mass—a relationship that does not hold for acyclic systems. As these rings are non-trivial to synthesize individually in solution, we propose the presented workflow to identify and characterize feasible molecules for bulk phase synthesis.

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<em>In Situ</em> SIMS and IR Spectroscopy of Well-defined Surfaces Prepared by Soft Landing of Mass-selected Ions

Cited by 2 publications

References 131 publications

Understanding ligand effects in gold clusters using mass spectrometry

Understanding ligand effects in gold clusters using mass spectrometry

Formation and characterization of polymetallic {CrxMy} rings in vacuo

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