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June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Direct Measurements of the Fundamental Rotational Transitions of CD and 13 CH.

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Presentation on theme: "June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Direct Measurements of the Fundamental Rotational Transitions of CD and 13 CH."— Presentation transcript:

1 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Direct Measurements of the Fundamental Rotational Transitions of CD and 13 CH (X 2 Π r ) D. T. Halfen, L. M. Ziurys Dept. of Chemistry Dept. of Astronomy Steward Observatory University of Arizona J.C. Pearson, and B.J. Drouin Jet Propulsion Laboratory California Institute of Technology

2 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Importance of CH in Astrophysics CH observed in many interstellar environments Tracer of Diffuse Gas at UV, optical wavelengths  One of original four interstellar species  Detected via electronic spectra Observed optically in Comets Also found towards many Denser Clouds  studied via lambda-doubling transition in J = ½ level ( 3 hyperfine components)  limited observations of rotational transitions in Far-IR (Kuiper Airborne Observatory) CH: F-X Band: X Per CH: Hale-Bopp CH at 3 GHz: hf components of Lambda-doublet

3 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Importance of CD and 13 CH CH in many interstellar environments Fundamental building block of interstellar carbon chemistry Useful to measure 12 C/ 13 C ratios via 13 CH/ 12 CH  tracer of Galactic Chemical Evolution D/H ratio also significant  indicator of fractionation  follow chemical pathways Effective avenue to measure such ratios  Observing rotational spectra  Become very feasible with Herschel, SOFIA KAO CH spectrum Herschel Space Observatory

4 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Energy Level Diagram: case (b) CD: Brown and Evenson (1989) Wienkoop et al. (2003)  LMR, FTIR measurements  in mid, far IR 13 CH: Davidson et al (2004)  LMR of rotational transitions McCarthy et al. (2006)  FTMW measurements of several lambda-doublets with hf This work: measure rotational transitions directly CD and 13 CH: N = 1→1 CD: N = 1 →2 Past Rotational Spectroscopy

5 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy T R * (K) Frequency (GHz) SO 2 CH 3 OH HOOCH 3 U CH 3 OCH 3 CH 3 CH 2 CN NH 2 CHO U CH 2 CHCN U U U U CH 3 OCH 3 U U HCOOH & CH 3 CH 2 CN Are such measurements necessary ?? SgrB2(N)

6 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Millimeter Direct Absorption with AC Longitudinal Discharge

7 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy JPL Instrumental Details Source developments thanks to Herschel/HIFI Direct Absorption, DC discharge

8 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Detector Gas Cell Reactant Radiation Source Arizona System

9 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Gas-Phase Production of CD and 13 CH Arizona Studies Precursor gas: CD 4 or 13 CH 4 –Pressure: 1-5 mTorr Carrier Gas: 40 mTorr Argon AC discharge for –200 W at 600  –Pink-purple glow JPL CD synthesis - 5 mTorr CH 4 /20 mTorr D 2 with 100 mTorr He - DC discharge

10 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Arizona Data JPL Data Hyperfine Structure Resolved in N = 1→1 Spectrum Halfen et al Ap.J., in press

11 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Resolved 13 C and H hf structure Arizona Data

12 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Observed Transition Frequencies of CD (X 2  r ) N  NN J  JJ F  FF Parity obs (MHz) obs -  calc (MHz) 1  11.5  0.5 1.5  +   439255.608 a -0.076 2.5  1.5+   439257.449 a 0.101 0.5  +   439271.905 a 0.093 1.5  0.5+   439272.694 a -0.117 1  11.5  0.5 2.5  1.5   +439794.923-0.027 1.5    +439800.0050.003 1.5  0.5   +439803.008-0.015 0.5    +439806.0930.039 2  11.5  0.5  1.5   + 884764.787 a 0.093 0.5    + 884764.787 a -0.906 1.5  2.5   + 884770.707 a 0.984 1.5    + 884770.707 a -0.680 1.5  0.5   + 884772.903 a 0.517 2.5  1.5   + 884781.449 a -1.095 2.5    + 884781.449 a 0.570 2  11.5  2.5  +   887230.8400.000 2  12.5  1.5 3.5  2.5   + 915851.970 a -0.196 2.5  1.5   + 915854.900 a 0.196 2  12.5  1.5 3.5  2.5+   916954.496 a 0.617 2.5  1.5+   916954.496 a -0.617 a Blended lines. CD

13 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Observed Transition Frequencies of 13 CH (X 2  r ) a N  NN J  JJ F1F1  F1F1 F  FF Parity obs (MHz) obs -  calc (MHz) 1  11.5  0.5 1  1  1.5+   531859.975-0.565 1  11.5  +   531862.711-0.182 1  10.5  +   531910.901-0.142 1  11.5  0.5+   531913.4710.076 2  11.5  +   532083.360-0.238 2  12.5  1.5+   532086.2510.316 2  11.5  0.5+   532134.7400.640 1  00.5  +   532224.939-0.479 1  01.5  0.5+   532227.528-0.242 1  11.5  0.5 1  01.5  0.5   +536005.0940.173 1  00.5    +536024.9690.567 1  11.5    +536026.6430.144 1  10.5  1.5   +532046.4770.497 1  10.5    +536057.8260.133 2  12.5  1.5   +536101.144-0.373 2  11.5    +536121.0350.030 2  11.5  0.5   +536132.344-0.374 a Coupling scheme: J = N + S; F 1 = J + I 1 ; F = F 1 + I 2 ; where I 1 and I 2 are the 13 C and H nuclear spins, respectively. 13 CH

14 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Spectroscopic Constants for CD (X 2  r ) ParameterThis work (MHz)Wienkoop et al. ( MHz) B230895.03(80)230896.08(13) D12.698(90)12.8216(36) H0.0004751 c A842308.59 c 842308.59(90)  -424.049(91)-423.80(23) p544.89(27)544.41(57) pDpD -0.047 c -0.047(39) q339.424(97)339.45(18) qDqD -0.082(34)-0.0761(69) a (D)8.74(27)8.05(99) b F (D)-8.797(72)-8.99(87) c (D)9.26(81)8.9(1.6) d (D)7.054(87)7.06(90) eqQ(D)-0.69(41) - C Held fixed. Deuterium eqQ determined Improved D hf constants Improved fine structure constants Good agreement with past work

15 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy Spectroscopic Constants for 13 CH (X 2  r ) a ParameterThis work (MHz)McCarthy et al. (MHz)Davidson et al. (MHz) B422962.011(18)422966.125(270)422966.021(285) D43.3319 a 43.3319(150)43.3291(144) A843799.80 a 843799.80(1.14)843799.44(1.23)  -765.26 a -765.26(33)-765.10(36) p997.674(53)998.12(48)998.39(72) pDpD -0.298 a -0.298(54)-0.305(69) q1146.056(10)1145.971(81)1146.073(132) qDqD -0.4476 d -0.4476(78)-0.4554(117) a ( 13 C)217.752(85)218.20(57)218.10(1.26) b F ( 13 C)41.989(91)41.83(90)41.99(84) c ( 13 C)-129.83(19)-131.02(1.17)-131.0(3.6) d ( 13 C)276.67(16)275.14(1.20)275.54(78) d D ( 13 C)-0.393(24)-0.166(177) a (H)54.410(88)54.2169(39)54.006 a b F (H)-57.60(10)-57.855 a -57.777 a c (H)57.19(23)56.266 a 56.52 a d (H)43.841(41)43.836(54)43.513 a d D (H)0.0836(50)0.0826(78) a Held fixed. Proton b F and c established Improved 13 C hyperfine and lambda-doubling constants 4 MHz discrepancy in B

16 June 16-20, 2008 63 rd International Symposium on Molecular Spectroscopy In Conclusion Lowest energy rotational transitions of CD and 13 CH measured Precision of 200-500 kHz Determination of hyperfine parameters (eqQ(D), b F (H), c(H)) Improvement of other spectroscopic constants Important for upcoming Herschel, SOFIA observations Used to establish 12 C/ 13 C ratios Degree of deuterium enhancement in fundamental building block CH ACKNOWLEDGEMENTS: NASA Lab Astrophysics Program

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