On the iron oxide neutral cluster distribution in the gas phase. I. Detection through 193 nm multiphoton ionization.
Iron oxide (FemOn) neutral clusters are generated in the gas phase through laser ablation of the metal and reaction with various concentrations of O2 in He. The mixture of expansion gas and neutral FemOn cluster species is expanded through a supersonic nozzle into a vacuum system, in which the clusters are ionized by an ArF excimer laser at 193 nm, and the ions are detected and identified in a time-of-flight mass spectrometer. In this report, the experimental parameters that influence the observed cluster distributions, such as ablation laser power, expansion pressure, vacuum system pressure, and 193 nm ArF ionization laser power, are explored. In the second paper in this series, the effect of the ionization laser wavelength (355 nm, 193 nm, 118 nm) on the observed cluster ion distribution is explored. The cluster ion distribution observed employing 193 nm laser ionization, is sensitive to the neutral cluster distribution as evidenced by the change in the observed time-of-flight mass spectra with changes in laser power, growth conditions, and expansion conditions. The thermodynamically stable neutral clusters for saturated O2 growth conditions are suggested to be of the forms FemOm, FemO(m+1), and FemO(m+2); which one of these series of neutral clusters is most stable depends on the size of the cluster. For m < 10, FemOm is the most stable neutral cluster series, for 10 < or = m < or = 20, FemO(m+1) is the most stable neutral cluster series, and for 21 < or = m < = 30, FemO(m+2) is the most stable neutral cluster series. Some neutral cluster fragmentation is clearly present for 193 nm ionization due to multiphoton absorption in both the neutral and ionic cluster species.
Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523-1872, USA.
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Shin
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Matsuda
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Bernstein