Frank Lewen

Phase locked backward wave oscillator pulsed beam spectrometer in the submillimeter wave range

We have developed a new submillimeter wave pulsed molecular beam spectrometer with phase stabilized backward wave oscillators (BWOs). In the frequency ranges of 260–380 and 440–630 GHz, the BWOs output power varies between 3 and 60 mW. Part of the radiation was coupled to a novel designed harmonic mixer for submillimeter wavelength operation, which consists of an advanced whiskerless Schottky diode driven by a harmonic of the reference synthesizer and the BWO radiation. The resulting intermediate frequency of 350 MHz passed a low noise high electron mobility transistor amplifier, feeding the phase lock loop (PLL) circuit. The loop parameters of the PLL have been carefully adjusted for low phase noise. The half power bandwidth of the BWO radiation at 330 GHz was determined to be as small as 80 MHz, impressively demonstrating the low phase noise operation of a phase locked BWO. A double modulation technique was employed by combining an 80 Hz pulsed jet modulation and a 10–20 kHz source modulation of the BWO...

Millimeter-wave intracavity-jet OROTRON-spectrometer for investigation of van der Waals complexes

A highly sensitive intracavity millimeter-wave spectrometer was developed for the investigation of the absorption spectra of van der Waals complexes in a supersonic jet. The key element of the spectrometer is a tunable oscillator, called OROTRON, which generates the millimeter-wave radiation through the interaction of an electron beam with the electromagnetic field of a high quality (Q≈104) Fabry–Perot resonant cavity. This cavity consists of a movable spherical mirror and a fixed planar mirror with the periodic structure imprinted on its surface. The electron beam moves along the periodic structure of the plane mirror. This part separated from the rest of the resonator by a mica foil is kept under ultrahigh vacuum conditions. The molecular jet is injected by a pulsed valve into the other part of the resonator. The absorption in the jet is sensitively detected by measuring the electric current in a special collector circuit of the OROTRON. The spectral purity of the OROTRON radiation is 10–15 kHz providin...

Detection of the millimeter wave spectra of the weakly bound complexes 3He–CO and 4He–CO

For the first time, millimeter wave absorption spectra of the van der Waals complexes 3He–CO and 4He–CO were detected in a supersonic jet. Altogether four rotational transitions of 3He–CO and six rotational transitions of 4He–CO were recorded between 110 GHz and 127 GHz with an intracavity spectrometer based on the millimeter wave generator, called OROTRON. The obtained results were included in a global fit together with previously known data enabling a more precise determination of the energy levels of the 3He–CO and 4He–CO complexes. In extremely cold, dark, and dense interstellar clouds the He–CO complex may have astrophysical relevance.

Discovery of the rotational spectrum of the weakly bound complex CO–H2

Rotational transitions of the CO–H2 van der Waals complex have been measured between 108 and 125 GHz in a supersonic jet. Three absorption lines were recorded and assigned as belonging to CO–paraH2 with a new highly sensitive intracavity spectrometer based on the millimeter wave generator, called OROTRON. The results provide confirmation of the recent infrared data of McKellar at 4.7 μm, enabling a more precise determination of the energies of the rotational levels with different parity in the vibrational ground state. The measured millimeter wave transitions provide precise frequencies for an astronomical search of CO–paraH2.

Interstellar Detection of CCC and High-Precision Laboratory Measurements near 2 THz

We describe more fully our original tentative interstellar detection of the triatomic pure carbon chain molecule, CCC, in absorption toward the Galactic center source Sgr B2. C3 was detected with the Kuiper Airborne Observatory (KAO) by observing the R(2) bending vibration-rotation transition (0, 1 1 ,0 0, 0 0 , 0) near 65.7 cm 1 during one ) R ( of the last flights of KAO. The R(2) absorption line detected toward Sgr B2 is centered at 63.7(5) km s 1 , with km s 1 and a peak absorption of 18(3)%. This original tentative interstellar detection of C 3 DV(FWHM)p 8.3(9) has recently been confirmed by J. Cernicharo et al. through observation of a total of nine absorption lines, including the same R(2) line with the Infrared Space Observatory . We also present highly precise new laboratory measurements of 10 rovibrational transition frequencies of the n2 bending mode of C3, which have been obtained with the Cologne Sideband Spectrometer for Terahertz Application. Subject headings: ISM: individual (Sagittarius B2) — ISM: molecules — line: identification — methods: laboratory — techniques: spectroscopic On-line material: color figure

Application of superlattice multipliers for high-resolution terahertz spectroscopy

Frequency multipliers based on superlattice (SL) devices as nonlinear elements have been developed as radiation sources for a terahertz (THz) laboratory spectrometer. Input frequencies of 100 and 250 GHz from backward wave oscillators have been multiplied up to the 11th harmonic, producing usable frequencies up to 2.7 THz. Even at these high frequencies the output power is sufficient for laboratory spectroscopy. Comparisons to conventional high-resolution microwave spectroscopy methods reveal several superior features of this new device such as very high line frequency accuracies, broadband tunability, high output power levels at odd harmonics of the input frequency up to high orders, and a robust applicability.

Exploring molecular complexity with ALMA (EMoCA): Alkanethiols and alkanols in Sagittarius B2(N2)

Context. Over the past five decades, radio astronomy has shown that molecular complexity is a natural outcome of interstellar chemistry, in particular in star forming regions. However, the pathways that lead to the formation of complex molecules are not completely understood and the depth of chemical complexity has not been entirely revealed. In addition, the sulfur chemistry in the dense interstellar medium is not well understood. Aims. We want to know the relative abundances of alkanethiols and alkanols in the Galactic center source Sagittarius B2(N2), the northern hot molecular core in Sgr B2(N), whose relatively small line widths are favorable for studying the molecular complexity in space. Methods. We investigated spectroscopic parameter sets that were able to reproduce published laboratory rotational spectra of ethanethiol and studied effects that modify intensities in the predicted rotational spectrum of ethanol. We used the Atacama Large Millimeter Array (ALMA) in its Cycles 0 and 1 for a spectral line survey of Sagittarius B2(N) between 84 and 114.4 GHz. These data were analyzed by assuming local thermodynamic equilibrium (LTE) for each molecule. Our observations are supplemented by astrochemical modeling; a new network is used that includes reaction pathways for alkanethiols for the first time. Results. We detected methanol and ethanol in their parent 12 C species and their isotopologs with one 12 C atom substituted by 13 C; the latter were detected for the first time unambiguously in the case of ethanol. The 12 C/ 13 C ratio is ~25 for both molecules. In addition, we identified CH 3 18 OH with a 16 O/ 18 O ratio of ~180 and a 13 CH 3 OH/CH 3 18 OH ratio of ~7.3. Upper limits were derived for the next larger alkanols normal - and iso -propanol. We observed methanethiol, CH 3 SH, also known as methyl mercaptan, including torsionally excited transitions for the first time. We also identified transitions of ethanethiol (or ethyl mercaptan), though not enough to claim a secure detection in this source. The ratios CH 3 SH to C 2 H 5 SH and C 2 H 5 OH to C 2 H 5 SH are ≳21 and ≳125, respectively. In the process of our study, we noted severe discrepancies in the intensities of observed and predicted ethanol transitions and propose a change in the relative signs of the dipole moment components. In addition, we determined alternative sets of spectroscopic parameters for ethanethiol. The astrochemical models indicate that substantial quantities of both CH 3 SH and C 2 H 5 SH may be produced on the surfaces of dust grains, to be later released into the gas phase. The modeled ratio CH 3 SH/C 2 H 5 SH = 3.1 is lower than the observed value of ≳21; the model value appears to be affected most by the underprediction of CH 3 SH relative to CH 3 OH and C 2 H 5 OH, as judged by a very high CH 3 OH/CH 3 SH ratio. Conclusions. The column density ratios involving methanol, ethanol, and methanethiol in Sgr B2(N2) are similar to values reported for Orion KL, but those involving ethanethiol are significantly different and suggest that the detection of ethanethiol reported toward Orion KL is uncertain. Our chemical model presently does not permit the prediction of sufficiently accurate column densities of alkanethiols or their ratios among alkanethiols and alkanols. Therefore, additional observational results are required to establish the level of C 2 H 5 SH in the dense and warm interstellar medium with certainty.

Millimetre-wave spectrum of the Ar± CO complex: the K = 2 ¬ 1 and 3 ¬ 2 subbands

The K a = 2←1 and 3←2 subbands of the pure rotational spectrum of the weakly bound van a der Waals complex Ar–CO have been studied by direct absorption of millimetre and submillimetre radiation in a supersonic jet. A total of 77 transitions were observed in the 138–265 GHz (2←1 band) and 308–361 GHz (3←2 band) regions. These transitions were incorporated in a global fit of existing infrared, microwave and millimetre-wave data in order to determine a refined set of molecular parameters for Ar-CO. It was found that the form of the simple Hamiltonian used for this fit had to be modified, so that the rotational dependence of the K-type splitting terms was given by (J + K)!/(J - K)!,in order to fit accurately the asymmetry doubling of the K a = 3 levels for lower J values. The theory of the splitting terms is explained a in some detail. The present results provide a more precise foundation on which to base the continuing study of the fundamental complex Ar–CO.

High accuracy measurements on the ground state rotational spectrum of formaldehyde (H2CO) up to 2 THz

In making use of the Cologne Sideband spectrometer for Terahertz Applications (COSSTA), the pure rotational spectrum of H2CO in its ground vibrational state has been investigated in the frequency range from 1.76 to 2.01 THz with an absolute frequency accuracy ranging from 20 to 50 kHz for strong, isolated lines. Additionally, the rotational spectrum has been reinvestigated in the 0.830 to 0.957 THz region with the Cologne Terahertz spectrometer. The accurate new line frequencies were subjected to a combined fit with previously published data employing standard A- and S-reduced Watson-type Hamiltonians.

Laboratory Precision Measurements of the Rotational Spectrum of 12C17O and 13C17O

High-precision millimeter and submillimeter wave measurements were performed on two 17O isotopically substituted carbon monoxide species, i.e., 12C17O and 13C17O. Covering the frequency region from 100 GHz to 1 THz, the accuracy achievable is estimated to be ±5 kHz in the Doppler-limited mode and ±1 kHz for sub-Doppler-resolution measurements. From a weighted least-squares fit, the following molecular rotational parameters for 12C17O and 13C17O were obtained: for 12C17O, and for 13C17O, in both instances, the H0 values were kept fixed to IR data. The oxygen 17O nucleus exhibits a sizeable electric nuclear quadrupole moment, which has been measured for both isotopomers, i.e., eQq(12C17O) = 4.298(44) MHz and eQq(13C17O) = 4.355(182) MHz. The high precision of the Lamb dip measurements allowed us to observe additional small hyperfine effects caused by the magnetic moment of the 17O nucleus. These precision measurements allowed the determination of the nuclear spin-rotation constant CI(17O) = -31.60(72) Hz for 12C17O, solely from the Cologne data set. The highly precise transition frequencies reported here should warrant deep interstellar searches for the two molecules 12C17O and 13C17O. The latter has not been detected in space until very recently. On the basis of our laboratory data, we were able to report the discovery of 13C17O (by Bensch and coworkers) along with the observations of two additionalrare CO isotopomers including 12C17O and 12C18O toward core C of the ρ Ophiucus molecular cloud.