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The Spectroscopy of UF and UF + Joshua Bartlett, Ivan Antonov, Dr. Michael Heaven Emory University, Department of Chemistry 1515 Dickey Drive, Atlanta.

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Presentation on theme: "The Spectroscopy of UF and UF + Joshua Bartlett, Ivan Antonov, Dr. Michael Heaven Emory University, Department of Chemistry 1515 Dickey Drive, Atlanta."— Presentation transcript:

1 The Spectroscopy of UF and UF + Joshua Bartlett, Ivan Antonov, Dr. Michael Heaven Emory University, Department of Chemistry 1515 Dickey Drive, Atlanta GA 30322

2 Motivation Spectra of gas-phase uranium fluoride have been obtained for the first time by LIF, REMPI, and ZEKE techniques. Actinide compounds have unique bonding characteristics in which the role of f-electrons is not thoroughly understood. Spectroscopic results are benchmarked against high-level computational efforts.

3 Some Related Studies L. Kaledin and M. Heaven, J. Mol. Spec. 185 (1997) Electronic spectroscopy of UO  Proposed LFT application to actinides R. Hunt et al., Inorg. Chem. 33 (1994) Matrix IR spectra of the products from F 2, ClF, and Cl 2 reactions with pulsed-laser evaporated uranium atoms  Similar setup but Ar(s) is insufficient D. G. Fedorov et al., J. Chem. Phys. 118 (2003) An ab initio study of excited states of U and UF  CASCI with SO-MCQDPT at aug-cc-VTZ level

4 Experimental

5 Extractor Repeller -5.1 V -7.1 V 1.7 μs Experimental Pulsed-field ionization REMPI or ZEKE lasers LIF laser Ablation laser Gas pulse t Extractor Repeller ~ -4 V 1 st laser 2 nd laser 1.7 μs ~ -5 V 0.1% SF 6 /He 1064nm YAG @ 20-30 mJ 1 st chamber, vertical detection 1+1' or 1+1/2 techniques ~ -4 V Near-zero field

6 PUFI-ZEKE Two-photon excitation to Rydberg levels Ionization by pulsed external field Detection of low KE electrons after several μ s Pulsed field ionization

7 Photoionization TOF Mass Spectrum

8 15.51 μs Temporal gates enable facile REMPI probe to find two-photon ionizing resonances, confirmed to belong to UF states

9 LIF Spectrum Q branch P (4.5) P (5.5) R (6.5)

10 Dispersed Fluorescence Spectrum Taken from pump of Q-line V=1 appearance confirms assignment from Hunt et al. [1] [1] R. Hunt et al., Inorg. Chem. (1994)

11 PIE-determined IP * *

12 * *

13 Resolved Ground State (UF + ) IP = 51137(1) cm -1

14 ZEKE Survey Λ(Ω)

15 ZEKE Survey Λ(Ω)

16 ZEKE Survey Λ(Ω) Ω=4, v=5 Ω=5, v=3

17 Resolved Excited State (UF + )

18

19 UF + Parameters and Term Energies Λ(Ω)ωeωe ωeχeωeχe ΩBTeTe X(4)653.212.323540.240 1(3)652.943.135830.24511.821 1(2)645.961.745020.24738.836 1(1) and 1(?)645.621.71701, (?)0.24, (?)771.718 1(5)651.812.308550.2451011.263 2(4)648.361.498040.241512.147 2(2), 2(1)2, 11780.388 2(3)643?30.241835.555 3(3)33067. 1(6)63232. 2(5)53321. All values in cm -1.

20 UF + Parameters and Term Energies Λ(Ω)ωeωe ωeχeωeχe ΩBTeTe X(4)653.212.323540.240 1(3)652.943.135830.24511.821 1(2)645.961.745020.24738.836 1(1) and 1(?)645.621.71701, (?)0.24, (?)771.718 1(5)651.812.308550.2451011.263 2(4)648.361.498040.241512.147 2(2), 2(1)2, 11780.388 2(3)643?30.241835.555 3(3)33067. 1(6)63232. 2(5)53321. All values in cm -1. f2s2?f2s2?

21 UF + versus UO Λ(Ω)UF + T e UO T e [1] X(4)00 1(3)511.821651.12 1(2)738.836958.66 1(1)771.718- 1(5)1011.2631043.00 2(5)3321.- 2(4)1512.1472096.00 1(6)3232.4469(5) 3(3)3067.1941.48 [1] Kaledin, L. and Heaven, M. J. Mol. Spec. (1997)

22 UF + versus UO f 2 s 2 for UF + ? [1] Kaledin, L. and Heaven, M. J. Mol. Spec. (1997) Λ(Ω)UF + T e UO T e [1] X(4)00 1(3)511.821651.12 1(2)738.836958.66 1(1)771.718- 1(5)1011.2631043.00 2(5)3321.- 2(4)1512.1472096.00 1(6)3232.4469(5) 3(3)3067.1941.48

23 UF + versus UO 3(4) state not observed! [1] Kaledin, L. and Heaven, M. J. Mol. Spec. (1997) Λ(Ω)UF + T e UO T e [1] X(4)00 1(3)511.821651.12 1(2)738.836958.66 1(1)771.718- 1(5)1011.2631043.00 2(5)3321.- 2(4)1512.1472096.00 1(6)3232.4469(5) 3(3)3067.1941.48

24 CASSCF/PT2 Calculations aug-cc-VTZ basis Relativistic PP on U (4d in core) [1] [1] Dolg, M. and Cao, X. J. Phys. Chem. A. (2009)

25 CASSCF/PT2 Calculations Overestimation of SO contributions Smooth Ω progression for J=4 but less so for J=5

26 Future Work Complete assignment of UF + states Calculations encompassing f 2 s 2 configuration and alternate PP sizes Investigate additional actinide compounds with 3 rd row p-block elements

27 Acknowledgments Michael Heaven's research group (Ivan, Kyle, Jiande, Sullivan, Keith) and Xiaohong Wang Funding from U.S. Department of Energy

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