A Chirped Pulse Fourier Transform Microwave (CP-FTMW) Spectrometer with Laser Ablation Source to Search for Actinide-Containing Molecules and Noble Metal.

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Presentation transcript:

A Chirped Pulse Fourier Transform Microwave (CP-FTMW) Spectrometer with Laser Ablation Source to Search for Actinide-Containing Molecules and Noble Metal Clusters F. E. Marshall, David Joseph Gillcrist, Thomas D. Persinger, Nicole Moon, and G. S. Grubbs II 71st International Symposium on Molecular Spectroscopy June 20-24, 2016, Urbana-Champaign, IL, USA; MJ12

Systems of Interest- Actinide-Containing Molecules Spin-Orbit Interactions Computational Difficulties f-electron Chemistry

Systems of Interest- Noble Metal Clusters Picture taken from D. J. Frohman, G. S. Grubbs II, Z. Yu and S. E. Novick, "Probing the Chemical Nature of Dihydrogen Complexation to Transition Metals, a Gas Phase Case Study: H2–CuF." Inorg. Chem. 2013, 52, 816-822. Picture taken from K. Duanmu and D. G. Truhlar, "Partial Ionic Character beyond the Pauling Paradigm: Metal Nanoparticles." J. Phys. Chem. C 2014, 118, 28069-28074. Heterogeneous Catalysis (preferential sites for CO + O2 to give CO2, etc.) Fundamental Interest (dipole moments that break the Pauling Model; typical vdW bonding interactions with Noble Metal species have resulted in covalent bond tendencies)

Previous Work- Brooks Pate

Previous Work- Brooks Pate C. Pérez, M. T. Muckle, D. P. Zaleski, N. A. Seifert, B. Temelso, G. C. Shields, Z. Kisiel, B. H. Pate, Science, 336(2012), No. 6083, 897.

Previous Work- Steve Cooke

Previous Work- Steve Cooke G. S. Grubbs II, C. T. Dewberry, K. C. Etchison, K. E Kerr, and S. A. Cooke Rev. Sci. Instr. 78 (2007) 096106.

Our CP-FTMW

Our CP-FTMW Top: A 9-15 GHz sweep of 3% OCS in Ar after 30,000 averaging cycles. Transitions have been identified for minor isotopologue and vibrationally excited species of OCS as well as Ar and H2O dimer species. Bottom: A zoom-in of the 11800 MHz to 12150 MHz region showing isotopic and quadrupole levels of resolution with the technique.

Our CP-FTMW Schematic of the CP-FTMW with laser ablation source. The components are: 1. SRS® FS725 10 MHz Rb frequency standard; 2. SRS® FS725 Signal Distributor; 3. Tektronix® AWG70001A 20 GHz/50 GS/s Arbitrary Waveform Generator; 4. Microsemi® L0618-46-T680 6-18 GHz, 40W Power Amplifier; 5. Q-par® QWH-SL-2-18-S-HG-R 2-18 GHz High Gain, Broadband Horn Antennae; 6. Advanced Technical Materials® S1517D 0.5-18 GHz, 75 W Pin Diode SPST Switch; 7. Miteq® AMF-7D-01001800-22-10P Low Noise Amplifier, 55 dB, 1-18 GHz; 8. Tektronix® DPO72304DX 23 GHz/100 GS/s Digital Phosphor Oscilloscope; 9. Quantum Composers® 9514+ Pulse Generator; 10. Parker® Series 9 Solenoid Valve with Walker-Gerry Ablation Attachment; 11. Continuum® Minilite II 50 mJ@1064 nm pulsed Nd:YAG Laser, 15 Hz.

Laser Ablation Setup LASER

Laser Ablation Setup

Laser Ablation Setup

Laser Ablation Setup

Our LA-CMB-CP-FTMW

Acknowledgements Missouri S&T Startup UM Research Board Grant