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Rotational Spectroscopy of the Isotopic Species of Silicon Monosulfide, Sisw

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Rotational Spectroscopy of the Isotopic Species of Silicon Monosulfide, Sisw PAPER www.rsc.org/pccp | Physical Chemistry Chemical Physics Rotational spectroscopy of the isotopic species of silicon monosulfide, SiSw H. S. P. Mu¨ller,*ab M. C. McCarthy,cd L. Bizzocchi,e H. Gupta,cdf S. Esser,g H. Lichau,a M. Caris,a F. Lewen,a J. Hahn,g C. Degli Esposti,e S. Schlemmera and P. Thaddeuscd Received 2nd January 2007, Accepted 23rd January 2007 First published as an Advance Article on the web 20th February 2007 DOI: 10.1039/b618799d Pure rotational transitions of silicon monosulfide (28Si32S) and its rare isotopic species have been observed in their ground as well as vibrationally excited states by employing Fourier transform microwave (FTMW) spectroscopy of a supersonic molecular beam at centimetre wavelengths (13–37 GHz) and by using long-path absorption spectroscopy at millimetre and submillimetre wavelengths (127–925 GHz). The latter measurements include 91 transition frequencies for 28Si32S, 28Si33S, 28Si34S, 29Si32S and 30Si32Sinu = 0, as well as 5 lines for 28Si32Sinu = 1, with rotational quantum numbers J00 r 52. The centimetre-wave measurements include more than 300 newly recorded lines. Together with previous data they result in almost 600 transitions (J00 =0 and 1) from all twelve possible isotopic species, including 29Si36S and 30Si36S, which have fractional abundances of about 7 Â 10À6 and 4.5 Â 10À6, respectively. Rotational transitions were observed from u = 0 for the least abundant isotopic species to as high as u = 51 for the main species. Owing to the high spectral resolution of the FTMW spectrometer, hyperfine structure from the nuclear electric quadrupole moment of 33S was resolved for species containing this isotope, as was much smaller nuclear spin-rotation splitting for isotopic species involving 29Si. By combining the measurements here with previously published microwave and infrared data in one global fit, an improved set of spectroscopic parameters for SiS has been derived which include several terms describing the breakdown of the Born–Oppenheimer approximation. With this parameter set, highly accurate rotational frequencies for this important astronomical molecule can now be predicted well into the terahertz region. 1. Introduction Leo).3 Silicon monosulfide, SiS, is one of the more abundant molecules in this source,5,6 where it is thought to be the More than 130 molecules have been detected in the interstellar progenitor for much of the Si chemistry.4 However, SiS has 1,2 medium or in circumstellar shells. Nearly 10% of these also been observed toward massive star-forming regions such contain silicon, despite the refractory nature of silicon and as Sagittarius B2 near the Galactic centre.5 A total of seven 2,3 many Si-containing molecules. Shock vapourisation has rare isotopic species of SiS, including two doubly-substituted been proposed as the mechanism which releases silicon com- 29Si34S, 30Si34S7 and 28Si36S8 have now been detected in space, 4 pounds from the grains into the interstellar gas. Many Si- as have higher rotationally (J =20À 199,10) and vibrationally bearing molecules have been detected in the shell of the nearby (u =37) excited transitions. Maser activity in the ground carbon-rich asymptotic giant branch star IRC + 10216 (CW vibrational state of 28Si32S was detected toward IRC + 10216 rather early for the J =1À 0 transition11 and very recently for higher-J transitions.12 Even rovibrational spectra have been 13 a I. Physikalisches Institut, Universita¨tzuKo¨ln, Zu¨lpicher Str. 77, recorded toward this carbon-rich star. 50937 Ko¨ln, Germany. E-mail: [email protected] Hoeft et al. studied the pure rotational spectrum of SiS in b Max-Planck-Institut fu¨r Radioastronomie, Auf dem Hu¨gel 69, 53121 the laboratory in a series of papers around 40 years ago.14–17 Bonn, Germany c Transitions from the ground and excited vibrational states of Harvard-Smithsonian Center for Astrophysics, Cambridge, MA 28 32 14,15 02138, USA normal Si S and four singly-substituted species contain- d Division of Engineering and Applied Sciences, Harvard University, ing 29,30Si and 33,34S were reported.14,16,17 The dipole mo- Cambridge, MA 02138, USA ment15,18 and the 33S quadrupole coupling constant16 in the e Dipartimento di Chimica ’G. Ciamician’, Universita` di Bologna, Via F. Selmi, 2, 40126 Bologna, Italy ground vibrational state were also determined, as well as the f Institute for Theoretical Chemistry, Departments of Chemistry and effect of the breakdown of the Born–Oppenheimer approx- Biochemistry, The University of Texas at Austin, Austin, TX 78712 imation.17,19 Rovibrational transitions of SiS were subse- g Institut fu¨r Anorganische Chemie II, Universita¨tzuKo¨ln, Greinstr. 6, quently measured by Fourier transform emission 50939 Ko¨ln, Germany 20 21 w Electronic supplementary information (ESI) available: Final SiS spectroscopy and by diode laser infrared spectroscopy. data set. See DOI: 10.1039/b618799d Both studies involved the four most abundant isotopic species This journal is c the Owner Societies 2007 Phys. Chem. Chem. Phys., 2007, 9, 1579–1586 | 1579 Table 1 Summary of the SiS data set used in the final fit showing the isotopic species and their relative abundances. The number of lines,a the 17,20–22 maximum rotational Jmax and vibrational quantum number umax from previous (prev.) investigations and from the present (new) one are also provided. Values for rotational and rovibrational data are given separately a No. of lines Jmax umax Species Abundance Prev New Prev New Prev New Rotational data 28Si32S 8.8 Â 10À1 101 49 3 51 51 51 29Si32S 4.5 Â 10À2 109 29 3 50 29 31 30Si32S 2.9 Â 10À2 2 70 3 53 1 33 28Si33S 6.9 Â 10À3 — 128 — 2 — 16 29Si33S 3.5 Â 10À4 —41—2—3 30Si33S 2.3 Â 10À4 —25—2—2 28Si34S 4.0 Â 10À2 62 15 3 51 31 0 29Si34S 2.0 Â 10À3 —29—2— 10 30Si34S 1.3 Â 10À3 —22—2— 6 28Si36S 1.4 Â 10À4 —10—2— 4 29Si36S 7.0 Â 10À6 —4—2— 0 30Si36S 4.5 Â 10À6 —3—2— 1 Rovibrational data 28Si32S 1451 — 150 — 10 — 29Si32S 361 — 107 — 4 — 30Si32S 289 — 101 — 4 — 28Si34S 348 — 104 — 4 — a Overlapping hyperfine components have been counted as one line. 20 (see Table 1) and went to fairly high rotational (Jmax = 139 of the five most abundant isotopic species of SiS, including 21 20 or 150 ) and vibrational quantum numbers (umax =7 transitions within the u = 1 excited vibrational state for or 1021). 28Si32S, up to almost 1 THz to high accuracy—to better than A few years ago, several of us measured the two lowest 1 ppm—so that astronomical observations with the existing rotational transitions of the three most abundant isotopic APEX (Atacama Pathfinder Experiment) or SMA (Sub-Milli- species of silicon monosulfide, 28Si32S, 29Si32S and 28Si34S.22 meter Array) instruments or the upcoming Herschel Space The use of a pulsed molecular beam Fourier transform Observatory, SOFIA (Stratospheric Observatory For Infrared microwave (FTMW) spectrometer equipped with an electric Applications) or ALMA (Atacama Large Millimeter Array) discharge nozzle permitted the detection of rotational transi- can be undertaken with precise laboratory support. tions in highly excited vibrational levels up to u =51for 28Si32S, which corresponds to an energy of about 30 000 cmÀ1, nearly 60% of the dissociation limit. 2. Experimental details and observed spectra The present investigation extends previous FTMW mea- surements to all 12 stable SiS isotopic species. Silicon possesses Submillimetre-wave transitions of SiS were studied in Ko¨ln three naturally occurring isotopes, 28Si, 29Si and 30Si, with using the Cologne Terahertz Spectrometer, which is described relative abundances of 0.922, 0.047 and 0.031, respectively, in detail elsewhere.24 Phase-locked backward-wave oscillators while four isotopes occur for sulfur, 32S, 33S, 34S and 36S, with were used as sources and a liquid helium cooled hot-electron abundances of 0.95, 0.0075, 0.043 and 0.00015, respectively.23 InSb bolometer as detector. The 3 m long absorption cell Each isotopic species has been detected in natural abundance, was kept at room temperature. Di(t-butylsulfanyl)silane, 29 36 30 36 25,26 including Si S and Si S with fractional abundances of ((CH3)3CS)2SiH2, was subjected to a flash pyrolysis in an À6 À6 about 7 Â 10 and 4.5 Â 10 , respectively (see Table 1). A effort to record rotational spectra of silanethione, H2SiS. by-product of the present work is the determination of the 29Si While no transitions of this molecule were detected, strong and 33S hyperfine structure (hfs) as a function of vibrational lines of SiS, a plausible decomposition product, were ob- excitation. served. Transitions were recorded between 399 and 923 GHz Even though the lower rotational transitions of SiS have for 28Si32S in its ground vibrational state. Excited u =1 been fairly accurately determined from previous studies (un- transitions as well as ground state transitions of 28Si34S, certainties of 2 kHz22 or only a few kilohertz17), frequency 29Si32S and 30Si32S were recorded in the frequency range predictions in the millimetre-wave and submillimetre-wave 827–925 GHz. These frequencies are well above the Boltzmann bands have to be handled with caution, because these are peak at 300 K, which falls near 580 GHz. extrapolated from measurements which are quite limited in Millimetre- and submillimetre-wave transitions of SiS in the rotational excitation—to only J =2À 1 or possibly 3 À 2. ground vibrational state were observed in Bologna in a Inclusion of the infrared transitions20,21 only slightly improves negative glow discharge cell27 in the frequency range predictions of the rotational lines because the infrared data 127–743 GHz for 28Si32S with a source modulation millimetre have large uncertainties (0.5 Â 10À3 cmÀ1 or E15 MHz at wave spectrometer.28 Transitions of 29Si32S, 30Si32S, 28Si33S best).
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