Cold molecule studies of OH, NH, and metastable CO
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1 ACS, April 2008 p. 1/26 Cold molecule studies of OH, NH, and metastable CO Gerrit C. Groenenboom Theoretical Chemistry Institute for Molecules and Materials Radboud University Nijmegen The Netherlands
2 ACS, April 2008 p. 2/26 Collaborators OH, CO: FHI Berlin Joop Gilijamse Steven Hoekstra Samuel Meek Markus Metsälä Bas van de Meerakker Gerard Meijer NH: Harvard Wes Campbell Hsin-I Lu Edem Tsikata John Doyle
3 ACS, April 2008 p. 3/26 Cold molecule techniques 1998 buffergas cooling John Doyle, CaH 1999 Stark deceleration Gerard Meijer, CO 2001 rotating nozzle Dudley Herschbach, O storage ring Gerard Meijer, ND photoassociation Pierre Pillet, Cs 2 (trapped) 2003 filtering Gerard Rempe, NH Feshbach resonances Rudy Grimm, Li 2 (BEC) 2003 billiard ball collisions Dave Chandler, Ar+NO 2004 optical Stark deceleration Peter Barker, C 6 H reactive collision slowing Hans-Joachim Loesch, K+HBr 2007 Zeeman deceleration Nicolas Vanhaeke, H 2007 molecular synchrotron Gerard Meijer, NH 3... cavity laser cooling Yun Ye, OH (theory)... sympathetic cooling Peter Barker
4 ACS, April 2008 p. 4/26 Xe+OH( 2 Π 3/2f ) collision experiment cooled -70 o C LIF zone PMT Xe Stark decelerator skimmer hexapole detection laser (282 nm) pulsed valve photodissociation laser (193 nm) Bas van de Meerakker, Steven Hoekstra, Joop Gilijamse, Gerard Meijer (Berlin, 2006)
5 ACS, April 2008 p. 5/26 OH X( 2 Π) energy levels cm /2 f e /2 f + e /2 f e /2 N J F 2, X 2 Π 1/2 f - e + ε p 0 1 3/2 N J f + e - ε p F 1, X 2 Π 3/2
6 Xe OH( 2 Π) potentials (cm 1 ) Xe OH (A ) Xe OH (A ) θ (degrees) θ (degrees) R (a 0 ) R (a 0 ) Molpro: RCCSD(T), aug-cc-pvqz+bond orbitals, ECP28MDF ACS, April 2008 p. 6/26
7 ACS, April 2008 p. 7/26 Xe+OH energy dependent cross sections 10 3 F 1 (3/2f) 10 2 F 1 (3/2e) σ (Å 2 ) F (5/2e) 1 F (1/2) 2 F (7/2) 1 F (5/2f) 1 F (3/2) E coll (cm 1 )
8 Xe+OH experimental results ACS, April 2008 p. 8/26
9 ACS, April 2008 p. 9/26 Xe+OH, comparison with experiment 100 σ (%) F 1 (3/2e) F 1 (5/2e) F 1 (5/2f) 0 F 2 (1/2e) E coll (cm 1 ) Gilijamse, Hoekstra, van de Meerakker, Groenenboom, Meijer, Science 313, 1617 (2006)
10 ACS, April 2008 p. 10/26 Xe+OH, convolution and Xe beam σ(e coll ) voh 2 Signal n OH n + v2 Xe Xe v OH v Xe (m/s) FWHM (%) 5
11 ACS, April 2008 p. 11/26 Convergence check Xe+OH: F max /2e 3/2f 5/2e 5/2f 1/2e 1/2f F F l = 45 b = l 2µEcoll 8 bohr
12 ACS, April 2008 p. 12/26 Buffergas loading Buffer-gas Cooling and Loading Hot Molecules 1000 K Superconducting Magnet Coils Cold Walls < 1 K Helium Buffer Gas cm -3 Cold Trapped Molecules John Doyle, Wes Campbell, et al., Harvard Accepts full Boltzmann distribution of source External motion, rotation thermalize quickly Vibration, spin thermalize slowly He provides dissipation in conservative trap potential
13 ACS, April 2008 p. 13/26 NH(v = 1) in trap vs time Number of Trapped NH(v"=1) [arb.] v=1 v"=1 A 3 Π 2 X 3 Σ Time [ms] W. C. Campbell, G. C. Groenenboom, H.-I Lu, E. Tsikata, and J. M. Doyle, Phys. Rev. Lett., 100, (2008)
14 ACS, April 2008 p. 14/26 Measured NH(v = 0, 1) trap lifetime Trapped Molecule Lifetime [ms] v = 0 v = Buffer-Gas Density [10 14 cm -3 ] W. C. Campbell, G. C. Groenenboom, H.-I Lu, E. Tsikata, and J. M. Doyle, Phys. Rev. Lett., 100, (2008)
15 ACS, April 2008 p. 15/26 NH X 3 Σ (v = 1) lifetime (ms) τ 1 = f 4αω 3 3c 2 v = 0,N = 1 µ(r) v = 1,N = 0 2 e2 Rosmus, Werner, 1980, PNO-CEPA 28.7 Dodd et al., 1991, MRCI/RKR 19.3 (23.9) CASSCF/MRCI aug-cc-pvtz rotation cc-pv6z active space (6σ, 3π) core-correlation aug-cc-pv6z RHF+RCCSD(T) finite field 37.4 buffergas cooling experiment: 37.0 ± 0.5 ms
16 ACS, April 2008 p. 16/26 NH( 3 Σ ) permanent dipole moment (v = 0) Experiment, Scarl and Dalby (1974) 0.543± ea 0 CASSCF+MRCI aug-cc-pv6z: Paldus and Li (1996): Conclusion: 30% more N on our sun
17 Radiative lifetime of OH X 2 Π 3/2 (v = 1) Van de Meerakker, Vanhaecke, van der Loo, Groenenboom, and Meijer, Phys. Rev. Lett., 95, (2005) ACS, April 2008 p. 17/26
18 ACS, April 2008 p. 18/26 Radiative lifetime of OH X 2 Π 3/2 (v = 1) Molpro: aug-cc-pv6z, 1σ 5σ, 1π 2π CASSCF/MRCI year τ (ms) Decay in trap ±2 Present calculation (57.2) HITRAN D. D. Nelson et al S. R. Langhoff et al S. R. Langhoff et al H.-J. Werner et al M. van der Loo and G. C. Groenenboom, J. Chem. Phys. 126, (2007)+erratum Application to OH Meinel system: Decrease in atomic hydrogen over the summer pole, D. E. Siskind et al., Geophys. Res. Lett. (2008), submitted
19 ACS, April 2008 p. 19/26 CO(a 3 Π 1 ) lifetime model h a (r) 1 cm h A,a (r) µ X,A (r) 0.5 a.u. τ 1 = v X A vx,v a ev A( 1 Π) a( 3 Π) X( 1 Σ + ) A vx,v a = 4αω3 v a,v X 3c 2 e 2 c 2 Ω,1 v A v X µ X,A v A v A h A,a v a E va E va r (a 0 ) Thomas James, JCP 1971
20 ACS, April 2008 p. 20/26 CO(a 3 Π 1 ) lifetime results (ms) Experiment: 2.63 ± 0.03 Thomas James (JCP 1971): % Ab initio + RKR potentials: % Sykora and Vidal (JCP 1999): % Jongma, Berden, Meijer (JCP 1997): 3.67± % 3.4± % J. Gilijamse et al., J. Chem. Phys., 127, (2007)
21 ACS, April 2008 p. 21/26 CO(a 3 Π 1 ) lifetime extended model lower level calculation (MCSCF/aug-cc-pVTZ) extra 1 Π intermediate states result scaled to 3.16 ms for single intermediate state ms 20.0% ms 27.0% ms 2.4% ms 10.3% ms 3.4% Experiment: 2.63 ms
22 ACS, April 2008 p. 22/26 Check of spin-orbit coupling CO (a 3 Π Ω ) v a Ab initio Experiment error (%) R. W. Field et al., J. Mol. Spectrosc. (1972)
23 ACS, April 2008 p. 23/26 CO A 1 Π X 1 Σ + transition dipole moment µ X,A (ea 0 ) present Spielfiedel (1999) Kirby (1989) EOM HF EOM MCSCF r = 2.0 a 0 r = 2.5 a 0 present (ea 0 ) Spielfiedel [1] 91.6% 99.1% Kirby [2] 94.9% 99.6% 0.25 CCSD-EOM(HF) 93.4% 98.0% EOM(MCSCF) 93.6% 99.4% r (a ) 0 [1] A. Spielfiedel et al., Astron. Astrophys. (1999) [2] K. Kirby and D. L. Cooper, J. Chem. Phys. (1989)
24 ACS, April 2008 p. 24/26 CO A 1 Π X 1 Σ + oscillator strength f osc = v A 2 3 (E v A E vx ) µ va,v X 2 Present % Experiment (1993) Other experiments: Spielfiedel (1999) % Kirby (1989) % W. F. Chan et al., Chem. Phys. (1993) Electron energy loss spectrosc. + TRK sum-rule (7-200 ev)
25 CO A 1 Π(v ) dependent lifetimes (ns) Experiment Fit τ (ns) Ab initio v Experiment: R. W. Field et al., J. Chem. Phys. (1983) Using fitted dipole: τ(co a 3 Π 1 ) = 3.66 ms. ACS, April 2008 p. 25/26
26 ACS, April 2008 p. 26/26 Conclusions Xe+OH: towards crossed controlled beams NH(v = 1) lifetime: 30 % more N on our sun OH(v = 1) lifetime benchmark: Meinel system CO(a 3 Π 1 ) lifetime: nonorthogonality essential, measured A 1 Π(v ) lifetimes wrong
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