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1、The 66th International Symposium on Molecular Spectroscopy, June 2010Fang Wang ,Anh Lee and Timothy C. Steimle Dept. Chem. & BioChem., Arizona State University, Tempe, AZ,USAFunded by: NSF Spectroscopy of thorium monoxide,ThOin support of Particle Physics Michael C. HeavenDept. Chem. , Emory Uni
2、versity, Atlanta, Georgia, USAGoals: permanent electric dipole momentsa Franck-Condon prediction/intensity lifetimeOutlineExperimental setupAnalysis/Results Observation-Spectraa. Dispersed Fluorescenceb. Lifetime (Decay curve)c. Stark DiscussionMotivationSummaryaF. Wang, A. Lee, T.C.Steimle and M.C.
3、 Heaven, J.Chem. Phys, 134, 031102(2011)MotivationNeeded in scheme to test of elementary particle physics beyond the Standard Model via measurement of electric dipole moment of electron, de.Chemists view of an electron: Point ChargePhysists view of an electron: Point Charge with distributionDipole m
4、oment of an electron, deExperimental limita: |de| 1.6 10-27 e cmaB. Regan, E. Commins, C. Schmidt, D. DeMille, PRL 88, 071805 (2002)Based on thallium atom.Note dipole moment of HCl 6 D= 1.2 10-8 e.cmHow big is de? Standard Model de10-41 ecm10-19 times smallervAmplifying the electric field Eint with
5、a polar molecule Why ThO?Energy= -EintdeEint= electric field near the nucleusvSmall W-doublingvThe W=1 component of the 3D state is non-magnetic.Heavy polar molecular:Smaller systematic errorsThe metastable H3D D1 state:Eint 2Z3 e/a02 100 GV/cm:Polarizability factorZ: Atomic numbercomplete polarizat
6、ion with very small fields Experimental SetupLaser ablation source and supersonic expansion, Laser Induced Fluorescence (LIF) detector Well collimatedmolecular beamMetal target(Th foil)Pulse valveskimmerAblation laserO2& Ar(carrier gas)Pulsed dye laser Single freq. tunable laser radiationFluores
7、cencePMTMonochromator PMTStark platesOptical Stark spectroscopyExcitation spectraHigh resolution spectraThorium foilO2DF spectraObserved electronic states and transitions in ThOG.Edvinsson and A. Lagerqvist(1985)E(0+)-X1SF(0+)-X1SF-H3D613nm545nm760nmR-H3DG-H3DE&H same Th2+(7s6d)O2 configurationa
8、.aV.Goncharov, J. Han, L.A.Kaledin, and M.C.Heaven, J.C.P 122,204311(2005)Pulsed Dye Laser Observation: Excitation & DFP-branchR-Branch17145.4cm-1DF SpectraP-branchR-Branch18337.5cm-1Excitation SpectraExcitation SpectraDF SpectraE(0+)-X1S(1,0)F(0+)-X1S(0,0)u”010uLaseru”u13210LaserLifetime measur
9、ementE(0+)-X1S(1,0)F(0+)-X1S(0,0)LaserdecayLaserdecayacbE=0V/cm E=3600.7V/cmE=0V/cmE=3662.4 V/cm1) Franck-Condon factor predictionProf. LeRoys Suite of Program: “RKR1 v2.0” & “Level v8.0”u,u1,01,11,21,3E(0+)-X1S+0.1350.6020.2330.0286u,u0,00,10,20,3F(0+)-X1S+0.8290.1490.02110.0015(0,0)(0,1)F1(0+)
10、-X1S(u,u)E1(0+)-X1S(u,u)(1,0)(1,1)(1,2)(1,3)Analysis/ResultsFit to:Four parameters:y0, A1, x0, t1t1 is lifetime2) Radiative lifetime measurementE(0+)-X1S(1,0)F(0+)-X1S(0,0)t1=0.2594(5) mst1=0.574(9) msAnalysis/Results (Conti.)m1,0(E-X) Basis function:HRot=BJ2Field-Free Spectrum T10 =17144.98069(36)
11、cm-1; B”= 0.331967(27) cm-1 ; B= 0.321185(27) cm-1 Stark Spectrum 8 8 representation ( J=0-7)m (X1S+) = 2.782 (12) Dm (E(0+) = 3.534 (10) DDiscussionPermanent electric dipole momentThe larger dipole moment of the E state results from the circumstance that the 6d orbital is less polarizable than the
12、7S. LessPolarizableTheorya 13.9(CASSCF)Theoryb 22.93(RCCSD(T)aC. M. Marian, U. Wahlgren, O. Gropen, and P. Pyykko, THEOCHEM 46, 339 (1988).bA.A. Buchahenko,J. Chem. Phys. 133, 041102(2010)Th2+(7s6d)O2Th2+(7s2)O2Summary and Future work Franck-Condon prediction matches the experimental intensity prett
13、y well.The lifetimes for F(0+)-X1S+(0,0) and E(0+)-X1S+(1,0) bands are measured. The transition moments were estimated for both bands.c) Dipole moments were determined for both E(0+) and X1S+ states. The dipole moment for the H3D1 state will be approximately that of the E(0+) state because the two states are derived from the same Th2+(7s6d)O2 config
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