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The Submillimeter Spectrum of UO Jennifer A. Holt Christopher F. Neese Frank C. De Lucia June 17, 2014.

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Presentation on theme: "The Submillimeter Spectrum of UO Jennifer A. Holt Christopher F. Neese Frank C. De Lucia June 17, 2014."— Presentation transcript:

1 The Submillimeter Spectrum of UO Jennifer A. Holt Christopher F. Neese Frank C. De Lucia June 17, 2014

2 Experimental Setup

3 High Temperature Furnace Vacuum Water cooled shield Radiation Shields Furnace Tube Power Supply

4 Production of NdO vs UO High temperature decomposition of Nd 2 O 3 – ~2200K – Run times of ~3 hours UO from mixed metal and oxide – Starts with mixed metal and oxide – Highly aggressive to furnace – Short runtimes of ~20 minutes – Temperature ~2000K

5 Experimental Changes for UO Graphite tube with tungsten liner and Y 2 O 3 painted coating – Increased furnace durability and runtimes – Increased S/N Sample consists of U metal with UO 2 Powder – Materials mixed and pressed into pellet – Pellet placed in the center of the furnace tube

6 Graphite Furnace Tube

7 Spectral Coverage

8 Example Lines

9 (1)3(v=0)R31

10 Spectroscopy of UO vs NdO NdO has 3 isotopes with similar natural abundance, UO has one. UO has a second low lying electronic configuration. J. Chem. Phys. 124, 184317 (2006) © 2006 American Institute of Physics Kaledin et al., J. Mol. Spectr. 164, 27-64 (1994)

11 UO LFT UO is a Hund’s case C molecule, (minimal information). LFT gives an alternate description with a U 2+ cation perturbed by a O 2- ligand. U 2+ has two low lying electronic configurations: [5f 3 7s], [5f 2 7s 2 ]. Approximate quantum numbers J f and J a from SO and J-J coupling. LFT allows for the calculation of an energy map of the low lying electronic states. Hund’s Case C Coupling

12 Energy Map Kaledin et al., J. Mol. Spectr. 164, 27-64 (1994)

13 Line Assignments Vibronic StateB (GHz)D (KHz)σ ν (KHz) (1)3(v=0)9.831265.8688626.2 (1)3(v=1)9.790565.906747.35 (1)3(v=2)9.750225.9397939.2 (1)3(v=3)9.710005.9287663.7 (1)5(v=0)9.893496.0383843.6 (1)5(v=1)9.853546.068119.6 (1)5(v=2)9.824755.4080240.4 (1)5(v=3)9.798895.5104532.3 X4(v=0)9.9927810.2945470 X4(v=1)9.896096.96244254 X4(v=2)9.840155.761915.9 (2)4(v=0)10.37782.14331372 (2)4(v=1)10.38895.81611172 [5f 3 7s] [5f 2 7s 2 ]

14 UO Line Stats 285 observed lines from 510 GHz to 652 GHz 13 series identified and assigned 3 series identified, but not assigned 200 unassigned lines

15 Ongoing work Continue line assignments Dunham fits over vibrational states

16 Acknowledgements Michael Heaven Ivan Medvedev We would also like to thank the Missile Defense Agency and the Army Research Office for their support of this work

17 Supplemental Slides

18 Material Properties (W) Highest melting point metal: 3695K Very hard and brittle Difficult to work Does not spot-weld with any equipment we have Moderately expensive

19 Material Properties (Mo) Melting point 2896K Softer and more ductile than tungsten Can spot-weld with difficulty Fairly inexpensive

20 Material Properties (Ta) Melting point 3290K Very ductile and easy to work Easily spot-welds Expensive

21 Material Graphite (C) Sublimation point 3915K Machines easily, but very brittle Conductivity lower than metals, allows better electrical match to power supply Forms carbides with U at high temperatures Reacts with Y 2 O 3 at high temperatures

22 Material Yttria (Y 2 O 3 ) Melting point 2698K Very stable chemically, holds up well to molten uranium Reacts with carbon at high temperatures Transparent in SMM region


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