Spectroscopy of the Low Lying States of CaO +
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1 Spectroscopy of the Low Lying States of CaO + 7 nd Interna+onal Symposium on Molecular Spectroscopy FE 09 July 3, 017 Robert A. VanGundy, Michael C. Heaven
2 CaO + Mo8va8on Laser Cooling and Ion Trapping for ultracold molecules Isoelectronic to alkali metals Can be manipulated using external fields 1 Lack of spectroscopic data for CaO + Resonantly Enhanced Mul+photon Dissocia+on intermediates Benchmark calcula+ons Theore+cal Studies Predicted Ground state switch in Alkaline Earth Oxides As bond becomes more ionic, electron removed during ioniza+on expected to change from Π to Σ e - Correctly predicted for BaO + ( Σ + ground state), not experimentally verified for CaO + Ioniza+on Poten+al Refinement Previously referenced in RH05 69 th ISMS 1 J.E.Goeders, C.R. Clark, G. Vi4orini, K.W. Wright. C. R. Viteri, K.R. Brown, J. Phys Chem. A (013) J.H. BartleJ, R.A. VanGundy, M.C. Heaven, J. Chem. Phys. 143 (015) 04430/ /7.
3 Experimental Set-Up Ca rod Photomul+plier Tube Gate valve Skimmer Microchannel plates Dric tube Pulse valve O /He (~1% 60 psi) Charged plates Microchannel plates Diffusion pump (10-6 torr) Turbomolecular pump (10-8 torr)
4 Excita8on Scheme TOFMS-PIE LIF Lambda-Physik ScanMate Pro 355nm pumped pulsed dye laser PFI-ZEKE Con+nuum ND6000 Continuum Minilite 1064nm output 53nm pumped pulsed dye laser with doubling crystal
5 CaO Background CaO has not been thoroughly characterized in the energy region of interest Ioniza+on poten+al Theory: CASSCF/MRCI-Q 6.76eV( cm -1 ) 3 Experiment: Guided Ion beam 6.66(18)eV (53717(1450)cm -1 ) 4 Transi+ons C 1 Σ-X 1 Σ 1-0 through 3-0 iden+fied in through 8-0 reported in F 1 Π-X 1 Σ 6-0 through 13-0 reported in cm -1 C 1 Σ-X 1 Σ F 1 Π-X 1 Σ ν = ν = ν = ν = ν = ν = H. Khalil, F Le Quere, C Lenard, V. Brites, J. Phys. Chem. A 117, 1154 (013) 5. Lagerqvist, A. Ultra-Violet and bluebands of calcium oxide. Ark. För Fys (1954). 4. N.F. Dalleska, P.B. Armentrout, J. Mass Spectrom Ion Process 03-1 (1994) 6. J.T. Stewart, M.N. Sullivan, M.C.Heaven Journal of Molecular Spectroscopy 3 (016) 18 1
6 CaO+ Theory Background CaO + theory at the CASSCF-MRCI-Q theory level have predicted the levels of the ground state ( Π 3/ ) the loca+on of the spin orbit component Π 1/ and the loca+on of the next electronic excited state ( Σ + ) 3 TheorePcal (cm -1 ) Π 3/ Π 1/ Σ + ν = ν = ν = ν = CaO electronic states in black, CaO + and CaO - doublets in red, CaO + quartets in blue. 3. H. Khalil, F Le Quere, C Lenard, V. Brites, J. Phys. Chem. A 117, 1154 (013)
7 Neutral CaO on the path to CaO cm -1 Highest energy intermediate determined using REMPI Photoioniza+on Efficiency Scan using F-X 10-0 as intermediate
8 Pulsed Field Ioniza8on Zero Kine8c Energy Photoelectron Spectroscopy (PFI-ZEKE)
9 CaO + Origin Band CaO ioniza+on energy: 55438(5)cm -1 As predicted and corroborated by the appearance of peak near the predicted spin orbit split, this peak can be assigned as the Π 3/ electronic state.
10 CaO + Full ZEKE Survey Experimental cm -1 Π 3/ Π 1/ Σ + ν = ν = ν = ν = TheorePcal cm -1 Π 3/ Π 1/ Σ + ν = ν = ν = ν =
11 CaO + Conclusion Experimental results CaO ioniza+on poten+al: 55434(5) cm -1 (6.8730eV) Guided Ion beam 6.66(18)eV (53717(1450)cm -1 ) Spin orbit splisng: 140(5) cm -1 Σ + state T 0 = cm -1 Theore+cal predic+ons CaO ioniza+on poten+al: cm -1 (6.79eV) cm -1 Π 3/ v = 0 Spin Orbit Split Σ + v = 0 Experiment 55438(5) 140(5) 5615(5) Theory Spin orbit splisng: 15.cm -1 Σ + state T 0 = cm -1 Theory also predicts large coupling of the CaO + Π 1/ and Σ state which has been iden+fied in the spectra
12 Future Direc8ons Preliminary work on neutral CaOCa as well as CaOH has been completed. Indica+ng intermediates at levels conducive to inves+ga+on with -photon ZEKE. An extremely preliminary ioniza+on energy of (00) cm -1 (5.54±0.0eV) for CaOH has been determined. This falls within the range (5.5±.eV) provided by a guided ion beam study. 7 Inves+ga+ons of CaOCa will be difficult given the apparent break down of larger clusters into the target molecule overwhelming our mass channel in the TOF-MS. Ẽ Σ + - X Σ ~ of the CaOH neutral 7. Murad E., J. Chem Phys 75, 4080 (1981)
13 Acknowledgements Project Dr. Joshua BartleJ Dr. Jacob Stewart Dr. Michael Sullivan Group Dr. Jiande Han Dr. Kyle Mascaritolo Dr. Daniel Frohman Amanda Dermer Mallory Theis Sean Bresler Ryann Khalil Jessica Cifuentes Thank you for ajending!
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