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1.  Biological Cluster Mass Spectrometry 
This article reviews the new physics and new applications of secondary ion mass spectrometry using cluster ion probes. These probes, particularly C60, exhibit enhanced molecular desorption with improved sensitivity owing to the unique nature of the energy-deposition process. In addition, these projectiles are capable of eroding molecular solids while retaining the molecular specificity of mass spectrometry. When the beams are microfocused to a spot on the sample, bioimaging experiments in two and three dimensions are feasible. We describe emerging theoretical models that allow the energy-deposition process to be understood on an atomic and molecular basis. Moreover, experiments on model systems are described that allow protocols for imaging on biological materials to be implemented. Finally, we present recent applications of imaging to biological tissue and single cells to illustrate the future directions of this methodology.
PMCID: PMC2859288  PMID: 20055679
secondary ion mass spectrometry; bioimaging; molecular depth profiling; three-dimensional molecular imaging; C60; molecular dynamics
2.  Internal energy of molecules ejected due to energetic C60 bombardment 
Analytical chemistry  2009;81(6):2260-2267.
The early stages of C60 bombardment of octane and octatetraene crystals are modeled using molecular dynamics simulations with incident energies of 5-20 keV. Using the AIREBO potential, which allows for chemical reactions in hydrocarbon molecules, we are able to investigate how the projectile energy is partitioned into changes in potential and kinetic energy as well as how much energy flows into reacted molecules and internal energy. Several animations have been included to illustrate the bombardment process. The results show that the material near the edge of the crater can be ejected with low internal energies and that ejected molecules maintain their internal energies in the plume, in contrast to a collisional cooling mechanism previously proposed. In addition, a single C60 bombardment was able to create many free and reacted H atoms which may aid in the ionization of molecules upon subsequent bombardment events.
PMCID: PMC2666284  PMID: 19228010
3.  Sputtering Yields for C60 and Au3 Bombardment of Water Ice as a Function of Incident Kinetic Energy 
Analytical chemistry  2007;79(12):4493-4498.
The total sputtering yields for water ice due to kiloelectronvolt cluster bombardment have been measured and compared to the predictions made by the mesoscale energy deposition footprint (MEDF) model. For C60 bombardment the experimental yield varies almost linearly from 820 water molecule equivalents at an incident kinetic energy of 10 keV to 10100 water molecule equivalents at a kinetic energy of 120 keV. For Au3 bombardment the experimental yield varies almost linearly from 630 water molecule equivalents at an incident energy of 10 keV and rises to 1200 water molecule equivalents at 25 keV. The MEDF model is used to calculate relative yield trends with respect to incident energy using short time molecular dynamics simulations. The results of these calculations indicate that the model can effectively predict the yield trends observed for these two clusters in experiments, although there is a consistent overestimate of the predicted induced C60 yield. It is hypothesized that this overestimate can be explained by the absence of reactions and ionization processes in the current simulations. Despite this omission experimental yield trends can be accurately predicted using relatively small amounts of computer time. The success of the model in predicting the yield of water from ice films using a variety of energies and projectiles suggests this approach may greatly aid in the optimization of experimental configurations.
PMCID: PMC2553706  PMID: 17503768
4.  Fluid Flow and Effusive Desorption: Dominant Mechanisms of Energy Dissipation after Energetic Cluster Bombardment of Molecular Solids 
The angular distribution of intact organic molecules desorbed by energetic C60 primary ions was probed both experimentally and with molecular dynamics computer simulations. For benzo[a]pyrene, the angular distribution of intact molecules is observed to peak at off-normal angles. Molecular dynamics computer simulations on a similar system show the mechanism of desorption involves fast deposition of energy followed by fluid-flow and effusive-type emission of intact molecules. The off-normal peak in the angular distribution is shown to arise from emission of intact molecules from the rim of a crater formed during the cluster impact. This signature is unique for molecules because fragmentation processes remove molecules that would otherwise eject at directions near-normal to the surface.
PMCID: PMC3158660  PMID: 21860689
angular distribution; fluid-flow desorption; effusive desorption; C60 sputtering; molecular dynamics computer simulations; tof-snms; photoionization

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