Bradford Michael Mess, John J. Banisaukas III, and Lon B. Knight, Jr.

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Presentation transcript:

Electron Spin Resonance Investigations of Matrix Isolated Metal Clusters at 4 K Bradford Michael Mess, John J. Banisaukas III, and Lon B. Knight, Jr. Department of Chemistry, Furman University, Greenville, SC

Introduction Studying metal clusters is necessary to understand the transition from atomic and molecular properties to metallic bulk properties Metal clusters also play an important role in developing new catalysts

Formation of Metal Clusters Laser Vaporization Thermal Vaporization hν copper electrodes metal atoms metal atoms metal sample tantalum tube Cluster size depends on: Concentration ratio of rare gas to metal vapor Deposition temperature

Deposition Site Metal atom Neon atom Cluster formation Copper target cooled to 4 K

Matrix Isolation Apparatus Gases used: neon argon methane Background pressure: 8 x 10-7 Torr Liquid helium cryostat Metals used: magnesium calcium zinc 8 cm copper electrodes

Magnesium and Calcium Experiments Conditions Deposited in: neon argon methane Deposit length: 1 hour Mg deposits Dilute: grayish-red Medium: dark red Heavy; dark gray Flow rates: 2.4 – 5.0 sccm Deposit temperatures: 4 – 40 K Ca deposits All: gray black Goal: Maximize high spin species

ESR spectra of high spin Mg neutral clusters in neon at 4 K no hyperfine – due to π-bonding g┴ = 1.996(1) g║ = 2.000(1) D (zfs) = 2645(5) MHz

ESR spectra of high spin Ca neutral clusters in neon at 4 K Signals only seen in neon

Zinc Experiments Conditions Deposited in: neon Deposit length: 1 hour Zn deposits Dilute: colorless/light orange Medium: dark orange Heavy; black Average flow rate: 4.4 sccm Goal: control the size of clusters Deposit temperatures: 4 – 40 K X – irradiation: 30 minutes at 60 keV

ESR spectra of zinc dimer and trimer cations in neon at 2.6 K 67Zn+ (4.11 % abundance) I = 5/2 Deposit temperature: 2.6 K Higher Zn concentration Lower Zn concentration

Magnetic parameters (MHz) of zinc monomer, dimer, and trimer, cation radicals

Relative line positions of zinc cations

Acknowledgments Thank you to: Dr. Knight TJ Grant Hendrickson

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