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Holger S. P. Müller

Publications and source records attributed to Holger S. P. Müller.

At least 37 records · Page 2Linked to original sources

Atomium: The astounding complexity of the near circumstellar environment of the M-type AGB star R Hydrae. I. Morpho-kinematical interpretation of CO and SiO emission

Evolved low- to intermediate-mass stars are known to shed their gaseous envelope into a large, dusty, molecule-rich circumstellar nebula which typically develops a high degree of structural complexity. Most of the large-scale, spatially correlated structures in the nebula are thought to originate from the interaction of the stellar wind with a companion. As part of the Atomium large programme, we observed the M-type asymptotic giant branch (AGB) star R Hydrae with ALMA. The morphology of the inner wind of R Hya, which has a known companion at ~3500 au, was determined from maps of CO and SiO obtained at high angular resolution. A map of the CO emission reveals a multi-layered structure consisting of a large elliptical feature at an angular scale of ~10'' that is oriented along the north-south axis. The wind morphology within the elliptical feature is dominated by two hollow bubbles. The bubbles are on opposite sides of the AGB star and lie along an axis with a position angle of ~115 deg. Both bubbles are offset from the central star, and their appearance in the SiO channel maps indicates that they might be shock waves travelling through the AGB wind. An estimate of the dynamical age of the bubbles yields an age of the order of 100 yr, which is in agreement with the previously proposed elapsed time since the star last underwent a thermal pulse. When the CO and SiO emission is examined on subarcsecond angular scales, there is evidence for an inclined, differentially rotating equatorial density enhancement, strongly suggesting the presence of a second nearby companion. The position angle of the major axis of this disc is ~70 deg in the plane of the sky. We tentatively estimate that a lower limit on the mass of the nearby companion is ~0.65 Msol on the basis of the highest measured speeds in the disc and the location of its inner rim at ~6 au from the AGB star.

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Toward a global model of the interactions in low-lying states of methyl cyanide: rotational and rovibrational spectroscopy of the $v_4 = 1$ state and tentative interstellar detection of the $v_4 = v_8 = 1$ state in Sgr B2(N)

New and existing rotational spectra of methyl cyanide were analyzed to extend the global model of low-lying vibrational states and their interactions to $v_4=1$ at 920 cm$^{-1}$. The rotational spectra cover large portions of the 36$-$1439 GHz region and reach quantum numbers $J$ and $K$ of 79 and 16, respectively. Information on the $K$ level structure of CH$_3$CN is obtained from IR spectra. A spectrum of $2ν_8$ around 717 cm$^{-1}$, analyzed in our previous study, covered also the $ν_4$ band. The assignments in this band cover 880$-$952 cm$^{-1}$, attaining quantum numbers $J$ and $K$ of 61 and 13, respectively. The most important interaction of $v_4=1$ appears to be with $v_8=3$, $ΔK=0$, $Δl=+3$, a previously characterized anharmonic resonance. We report new analyses of interactions with $ΔK=-2$ and $Δl=+1$, with $ΔK=-4$ and $Δl=-1$, and with $ΔK=-6$ and $Δl=-3$; these four types of interactions connect all $l$ substates of $v_8=3$ in energy to $v_4=1$. A known $ΔK=-2$, $Δl=+1$ interaction with $v_7=1$ was also analyzed, and investigations of the $ΔK=+1$, $Δl=-2$ and $ΔK=+3$, $Δl=0$ resonances with $v_8=2$ were improved, as were interactions between successive states with $v_8\le 3$, mainly through new $v_8\le 2$ rotational data. A preliminary single state analysis of the $v_4=v_8=1$ state was carried out based on rotational transition frequencies and on $ν_4+ν_8-ν_8$ hot band data. A considerable fraction of the $K$ levels was reproduced within uncertainties in its entirety or in part, despite obvious widespread perturbations in $v_4=v_8=1$. We detect rotational transitions of methyl cyanide from within all vibrational states up to $v_4=1$ and $v_4=v_8=1$ tentatively toward the hot molecular core of Sagittarius B2(N) employing the Atacama Large Millimeter Array.

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Rotational spectroscopy of isotopic cyclopropenone, $c$-H$_2$C$_3$O, and determination of its equilibrium structure

Cyclopropenone was first detected in the cold and less dense envelope of Sagittarius B2(N). It was found later in several cold dark clouds and it may be possible to detect its minor isotopic species in these environments. In addition, the main species may well be identified in warmer environments. We aim to extend existing line lists of isotopologs of c-H2C3O from the microwave to the millimeter region and create one for the singly deuterated isotopolog to facilitate their detections in space. Furthermore, we aim to extend the line list of the main isotopic species to the submillimeter region and to evaluate an equilibrium structure of the molecule. We employed a cyclopropenone sample in natural isotopic composition to investigate the rotational spectra of the main and 18O-containing isotopologs as well as the two isotopomers containing one 13C atom. Spectral recordings of the singly and doubly deuterated isotopic species were obtained using a cyclopropenone sample highly enriched in deuterium. We recorded rotational transitions in the 70-126 GHz and 160-245 GHz regions for all isotopologs and also in the 342-505 GHz range for the main species. Quantum-chemical calculations were carried out to evaluate initial spectroscopic parameters and the differences between ground-state and equilibrium rotational parameters in order to derive semi-empirical equilibrium structural parameters. We determined new or improved spectroscopic parameters for six isotopologs and structural parameters according to different structure models. The spectroscopic parameters are accurate enough to identify minor isotopic species at centimeter and millimeter wavelengths while those of the main species are deemed to be reliable up to 1 THz. Our structural parameters differ from earlier ones. The deviations are attributed to misassignments in the earlier spectrum of one isotopic species.

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Determination of accurate rest frequencies and hyperfine structure parameters of cyanobutadiyne, HC$_5$N

Very accurate transition frequencies of HC$_5$N were determined between 5.3 and 21.4 GHz with a Fourier transform microwave spectrometer. The molecules were generated by passing a mixture of HC$_3$N and C$_2$H$_2$ highly diluted in neon through a discharge valve followed by supersonic expansion into the Fabry-Perot cavity of the spectrometer. The accuracies of the data permitted us to improve the experimental $^{14}$N nuclear quadrupole coupling parameter considerably and the first experimental determination of the $^{14}$N nuclear spin-rotation parameter. The transition frequencies are also well suited to determine in astronomical observations the local speed of rest velocities in molecular clouds with high fidelity. The same setup was used to study HC$_7$N, albeit with modest improvement of the experimental $^{14}$N nuclear quadrupole coupling parameter. Quantum chemical calculations were carried out to determine $^{14}$N nuclear quadrupole and spin-rotation coupling parameters of HC$_5$N, HC$_7$N, and related molecules. These calculations included evaluation of vibrational and relativistic corrections to the non-relativistic equilibrium quadrupole coupling parameters; their considerations improved the agreement between calculated and experimental values substantially.

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Rotational spectroscopy as a tool to investigate interactions between vibrational polyads in symmetric top molecules: low-lying states $v_8 \le 2$ of methyl cyanide, CH$_3$CN

Spectra of methyl cyanide were recorded to analyze interactions in low-lying vibrational states and to construct line lists for radio astronomical observations as well as for infrared spectroscopic investigations of planetary atmospheres. The rotational spectra cover large portions of the 36$-$1627 GHz region. In the infrared (IR), a spectrum was recorded for this study in the region of 2$ν_8$ around 717 cm$^{-1}$ with assignments covering 684$-$765 cm$^{-1}$. Additional spectra in the $ν_8$ region were used to validate the analysis. The large amount and the high accuracy of the rotational data extend to much higher $J$ and $K$ quantum numbers and allowed us to investigate for the first time in depth local interactions between these states which occur at high $K$ values. In particular, we have detected several interactions between $v_8 = 1$ and 2. Notably, there is a strong $Δv_8 = \pm1$, $ΔK = 0$, $Δl = \pm3$ Fermi resonance between $v_8 = 1^{-1}$ and $v_8 = 2^{+2}$ at $K$ = 14. Pronounced effects in the spectrum are also caused by resonant $Δv_8 = \pm1$, $ΔK = \mp2$, $Δl = \pm1$ interactions between $v_8 = 1$ and 2. An equivalent resonant interaction occurs between $K$ = 14 of the ground vibrational state and $K$ = 12, $l = +1$ of $v_8 = 1$ for which we present the first detailed account. A preliminary account was given in an earlier study on the ground vibrational state. From data pertaining to $v_8 = 2$, we also investigated rotational interactions with $v_4 = 1$ as well as $Δv_8 = \pm1$, $ΔK = 0$, $Δl = \pm3$ Fermi interactions between $v_8 = 2$ and 3. We have derived N$_2$- and self-broadening coefficients for the $ν_8$, 2$ν_8 - ν_8$, and 2$ν_8$ bands from previously determined nu4 values. Subsequently, we determined transition moments and intensities for the three IR bands.

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Rotational spectroscopy of singly $^{13}$C substituted isotopomers of propyne and determination of a semi-empirical equilibrium structure

Submillimeter spectra of three isotopomers of propyne containing one $^{13}$C atom were recorded in natural isotopic composition in the region of 426 GHz to 785 GHz. Additional measurements were carried out near 110 GHz. Combining these with earlier data resulted in greatly improved spectroscopic parameters which permit reliable extrapolations up to about 1.5 THz. Coupled cluster quantum-chemical calculations were carried out in order to assess the differences between equilibrium and ground state rotational parameters of these and many other isotopic species to evaluate semi-empirical equilibrium structural parameters. In addition, we estimated the main spectroscopic parameters of the isotopomers of propyne with two $^{13}$C atoms, which have not yet been studied in the laboratory, but which may be detectable in astronomical sources with a large amount of $^{13}$C compared to the dominant $^{12}$C.

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Laboratory rotational spectroscopy of isotopic acetone, CH$_3^{13}$C(O)CH$_3$ and $^{13}$CH$_3$C(O)CH$_3$, and astronomical search in Sagittarius B2(N2)

We want to study the rotational spectra of CH$_3^{13}$C(O)CH$_3$ and $^{13}$CH$_3$C(O)CH$_3$ and search for them in Sagittarius B2(N2). We investigated the laboratory rotational spectrum of isotopically enriched CH$_3^{13}$C(O)CH$_3$ between 40 GHz and 910 GHz and of acetone between 36 GHz and 910 GHz in order to study $^{13}$CH$_3$C(O)CH$_3$ in natural isotopic composition. In addition, we searched for emission lines produced by these species in a molecular line survey of Sagittarius B2(N) carried out with ALMA. Discrepancies between predictions of the main isotopic species and the ALMA spectrum prompted us to revisit the rotational spectrum of this isotopolog. We assigned 9711 new transitions of CH$_3^{13}$C(O)CH$_3$ and 63 new transitions of $^{13}$CH$_3$C(O)CH$_3$ in the laboratory spectra. More than 1000 additional lines were assigned for the main isotopic species. We modeled the ground state data of all three isotopologs satisfactorily with the ERHAM program. We find that models of the torsionally excited states $v _{12} = 1$ and $v _{17} = 1$ of CH$_3$C(O)CH$_3$ improve only marginally. No transition of CH$_3^{13}$C(O)CH$_3$ is clearly detected toward the hot molecular core Sgr B2(N2). However, we report a tentative detection of $^{13}$CH$_3$C(O)CH$_3$ with a $^{12}$C/$^{13}$C isotopic ratio of 27 that is consistent with the ratio previously measured for alcohols in this source. Several dozens of transitions of both torsional states of the main isotopolog are detected as well. Our predictions of CH$_3^{13}$C(O)CH$_3$ and CH$_3$C(O)CH$_3$ are reliable into the terahertz region. The spectrum of $^{13}$CH$_3$C(O)CH$_3$ should be revisited in the laboratory with an enriched sample. Transitions pertaining to the torsionally excited states $v _{12} = 1$ and $v _{17} = 1$ of CH$_3$C(O)CH$_3$ could be identified unambiguously in Sagittarius B2(N2).

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Rotational spectroscopy of isotopic species of methyl mercaptan at millimeter and submillimeter wavelengths: CH$_3$$^{34}$SH

Methyl mercaptan (CH$_3$SH) is an important sulfur-bearing species in the interstellar medium, terrestrial environment, and potentially in planetary atmospheres. The aim of the present study is to provide accurate spectroscopic parameters for the most abundant minor isotopolog CH$_3$$^{34}$SH to support radio astronomical observations at millimeter and submillimeter wavelengths. The rotational spectrum of CH$_3$$^{34}$SH, which is complicated by the large-amplitude internal rotation of the CH$_3$ group versus the $^{34}$SH frame, was investigated in the 49$-$510 GHz and 1.1$-$1.5 THz frequency ranges in natural isotopic abundance. The analysis of the spectrum was performed up to the second excited torsional state, and the obtained data were modeled with the RAM36 program. A fit within experimental accuracy was obtained with a RAM Hamiltonian model that uses 72 parameters. Predictions based on this fit are used to search for CH$_3$$^{34}$SH with the Atacama Large Millimeter/submillimeter Array (ALMA) toward the hot molecular core Sgr B2(N2), but blends with emission lines of other species prevent its firm identification in this source.

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Spectroscopic line parameters of NO, NO$_2$, and N$_{2}$O for the HITEMP database

This work describes the update of NO along with the incorporation of NO$_{2}$ and N$_{2}$O to the HITEMP database. Where appropriate, the HITRAN line lists for the same molecules have also been updated. This work brings the current number of molecules provided by HITEMP to seven. The initial line lists originating from \textit{ab initio} and semi-empirical methods for each molecule have been carefully validated against available observations and, where necessary, adjustments have been made to match observations. We anticipate this work will be applied to a variety of high-temperature environments including astronomical applications, combustion monitoring, and non-local thermodynamic equilibrium conditions.

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Rotational spectroscopy, dipole moment and $^{14}$N nuclear hyperfine structure of $iso$-propyl cyanide

Rotational transitions of $iso$-propyl cyanide, (CH$_3$)$_2$CHCN, also known as $iso$-butyronitrile, were recorded using long-path absorption spectroscopy in selected regions between 37 and 600 GHz. Further measurements were carried out between 6 and 20 GHz employing Fourier transform microwave (FTMW) spectroscopy on a pulsed molecular supersonic jet. The observed transitions reach $J$ and $K_a$ quantum numbers of 103 and 59, respectively, and yield accurate rotational constants as well as distortion parameters up to eighth order. The $^{14}$N nuclear hyperfine splitting was resolved in particular by FTMW spectroscopy yielding spin-rotation parameters as well as very accurate quadrupole coupling terms. In addition, Stark effect measurements were carried out in the microwave region to obtain a largely revised $c$-dipole moment component and to improve the $a$-component. The hyperfine coupling and dipole moment values are compared with values for related molecules both from experiment and from quantum chemical calculations.

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Rotational spectra of isotopic species of methyl cyanide, CH$_3$CN, in their ground vibrational states up to terahertz frequencies

Methyl cyanide is an important trace molecule in star-forming regions. It is one of the more common molecules used to derive kinetic temperatures in such sources. As preparatory work for Herschel, SOFIA, and in particular ALMA we want to improve the rest frequencies of the main as well as minor isotopologs of methyl cyanide. The laboratory rotational spectrum of methyl cyanide in natural isotopic composition has been recorded up to 1.63 THz. Transitions with good signal-to-noise ratio could be identified for CH$_3$CN, $^{13}$CH$_3$CN, CH$_3^{13}$CN, CH$_3$C$^{15}$N, CH$_2$DCN, and $^{13}$CH$_3^{13}$CN in their ground vibrational states up to about 1.2 THz. The main isotopic species could be identified even in the highest frequency spectral recordings around 1.6 THz. The highest $J'$ quantum numbers included in the fit are 64 for $^{13}$CH$_3^{13}$CN and 89 for the main isotopic species. Greatly improved spectroscopic parameters have been obtained by fitting the present data together with previously reported transition frequencies. The present data will be helpful to identify isotopologs of methyl cyanide in the higher frequency bands of instruments such as the recently launched Herschel satellite, the upcoming airplane mission SOFIA or the radio telescope array ALMA.

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Millimeter and Submillimeter Wave Spectroscopy of Propanal

The rotational spectra of the two stable conformers syn- and gauche-propanal (CH$_3$CH$_2$CHO) were studied in the millimeter and submillimeter wave regions from 75 to 500 GHz with the Cologne (Sub-)Millimeter wave Spectrometer. Furthermore, the first excited states associated with the aldehyde torsion and with the methyl torsion, respectively, of the $syn$-conformer were analyzed. The newly obtained spectroscopic parameters yield better predictions, thus fulfill sensitivity and resolution requirements in new astronomical observations in order to unambiguously assign pure rotational transitions of propanal. This is demonstrated on a radio astronomical spectrum from the Atacama Large Millimeter/submillimeter Array Protostellar Interferometric Line Survey (ALMA-PILS). In particular, an accurate description of observed splittings, caused by internal rotation of the methyl group in the $syn$-conformer and by tunneling rotation interaction from two stable degenerate $gauche$-conformers, is reported. The rotational spectrum of propanal is of additional interest because of its two large amplitude motions pertaining to the methyl and the aldehyde group, respectively.

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The spectroscopic parameters of sodium cyanide, NaCN (X 1A'), revisited

The study of the rotational spectrum of NaCN (X $^1$A') has recently been extended in frequency and in quantum numbers. Difficulties have been encountered in fitting the transition frequencies within experimental uncertainties. Various trial fits traced the difficulties to the incomplete diagonalization of the Hamiltonian. Employing fewer spectroscopic parameters than before, the transition frequencies could be reproduced within experimental uncertainties on average. Predictions of $a$-type $R$-branch transitions with $K_a \le 7$ up to 570 GHz should be reliable to better than 1 MHz. In addition, modified spectroscopic parameters have been derived for the 13C isotopic species of NaCN.

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Submillimeter spectroscopy of H$_2$C$^{17}$O and a revisit of the rotational spectra of H$_2$C$^{18}$O and H$_2$C$^{16}$O

The rotational spectrum of the formaldehyde isotopologue H$_2$C$^{17}$O was investigated between 0.56 and 1.50 THz using a sample of natural isotopic composition. In addition, transition frequencies were determined for H$_2$C$^{18}$O and H$_2$C$^{16}$O between 1.37 and 1.50 THz. The data were combined with critically evaluated literature data to derive improved sets of spectroscopic parameters which include $^{17}$O or H nuclear hyperfine structure parameters.

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Deuterated methyl mercaptan (CH$_3$SD): Laboratory rotational spectroscopy and search toward IRAS 16293-2422 B

Methyl mercaptan (also known as methanethiol), CH3SH, has been found in the warm and dense parts of high -- as well as low -- mass star-forming regions. The aim of the present study is to obtain accurate spectroscopic parameters of the S-deuterated methyl mercaptan CH$_3$SD to facilitate astronomical observations by radio telescope arrays at (sub)millimeter wavelengths. We have measured the rotational spectrum associated with the large-amplitude internal rotation of the methyl group of methyl mercaptan using an isotopically enriched sample in the 150-510 GHz frequency range using the Köln millimeter wave spectrometer. The analysis of the spectra has been performed up to the second excited torsional state. We present modeling results of these data with the RAM36 program. CH$_3$SD was searched for, but not detected, in data from the Atacama Large Millimeter/submillimeter Array (ALMA) Protostellar Interferometric Line Survey (PILS) of the deeply embedded protostar IRAS 16293-2422. The derived upper limit corresponds to a degree of deuteration of at most ~18%.

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Linking interstellar and cometary O$_2$: a deep search for $^{16}$O$^{18}$O in the solar-type protostar IRAS 16293--2422

Recent measurements carried out at comet 67P/C-G with the ${\it Rosetta}$ probe revealed that molecular oxygen, O$_2$, is the fourth most abundant molecule in comets. Models show that O$_2$ is likely of primordial nature, coming from the interstellar cloud from which our Solar System was formed. However, gaseous O$_2$ is an elusive molecule in the interstellar medium with only one detection towards quiescent molecular clouds, in the $ρ$ Oph A core. We perform a deep search for molecular oxygen, through the $2_1 - 0_1$ rotational transition at 234 GHz of its $^{16}$O$^{18}$O isotopologue, towards the warm compact gas surrounding the nearby Class 0 protostar IRAS 16293--2422 B with the ALMA interferometer. The targeted $^{16}$O$^{18}$O transition is surrounded by two brighter transitions at $\pm 1$ km s$^{-1}$ relative to the expected $^{16}$O$^{18}$O transition frequency. After subtraction of these two transitions, residual emission at a 3$σ$ level remains, but with a velocity offset of $0.3 - 0.5$ km s$^{-1}$ relative to the source velocity, rendering the detection "tentative". We derive the O$_2$ column density for two excitation temperatures $T_{\rm ex}$ of 125 and 300 K, as indicated by other molecules, in order to compare the O$_2$ abundance between IRAS16293 and comet 67P/C-G. Assuming that $^{16}$O$^{18}$O is not detected and using methanol CH$_3$OH as a reference species, we obtain a [O$_2$]/[CH$_3$OH] abundance ratio lower than $2-5$, depending on the assumed $T_{\rm ex}$, a three to four times lower abundance than the [O$_2$]/[CH$_3$OH] ratio of $5-15$ found in comet 67P/C-G. Such a low O$_2$ abundance could be explained by the lower temperature of the dense cloud precursor of IRAS16293 with respect to the one at the origin of our Solar System that prevented an efficient formation of O$_2$ in interstellar ices.

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The ALMA-PILS survey: The sulphur connection between protostars and comets: IRAS 16293-2422 B and 67P/Churyumov-Gerasimenko

The evolutionary past of our Solar System can be pieced together by comparing analogous low-mass protostars with remnants of our Protosolar Nebula - comets. Sulphur-bearing molecules may be unique tracers of the joint evolution of the volatile and refractory components. ALMA Band 7 data from the large unbiased Protostellar Interferometric Line Survey (PILS) are used to search for S-bearing molecules in the outer disc-like structure, 60 au from IRAS 16293-2422 B, and are compared with data on 67P/C-G stemming from the ROSINA instrument aboard Rosetta. Species such as SO$_{2}$, SO, OCS, CS, H$_{2}$CS, H$_{2}$S and CH$_{3}$SH are detected via at least one of their isotopologues towards IRAS 16293-2422 B. The search reveals a first-time detection of OC$^{33}$S towards this source and a tentative first-time detection of C$^{36}$S towards a low-mass protostar. The data show that IRAS 16293-2422 B contains much more OCS than H$_{2}$S in comparison to 67P/C-G; meanwhile, the SO/SO$_{2}$ ratio is in close agreement between the two targets. IRAS 16293-2422 B has a CH$_{3}$SH/H$_{2}$CS ratio in range of that of our Solar System (differences by a factor of 0.7-5.3). It is suggested that the levels of UV radiation during the initial collapse of the systems may have varied and have potentially been higher for IRAS 16293-2422 B due to its binary nature; thereby, converting more H$_{2}$S into OCS. It remains to be conclusively tested if this also promotes the formation of S-bearing complex organics. Elevated UV levels of IRAS 16293-2422 B and a warmer birth cloud of our Solar System may jointly explain the variations between the two low-mass systems.

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Rotational and high-resolution infrared spectrum of HC$_3$N: global ro-vibrational analysis and improved line catalogue for astrophysical observations

HC$_3$N is an ubiquitous molecule in interstellar environments, from external galaxies, to Galactic interstellar clouds, star forming regions, and planetary atmospheres. Observations of its rotational and vibrational transitions provide important information on the physical and chemical structure of the above environments. We present the most complete global analysis of the spectroscopic data of HC$_3$N. We have recorded the high-resolution infrared spectrum from 450 to 1350 cm$^{-1}$, a region dominated by the intense $ν_5$ and $ν_6$ fundamental bands, located at 660 and 500 cm$^{-1}$, respectively, and their associated hot bands. Pure rotational transitions in the ground and vibrationally excited states have been recorded in the millimetre and sub-millimetre regions in order to extend the frequency range so far considered in previous investigations. All the transitions from the literature and from this work involving energy levels lower than 1000 cm$^{-1}$ have been fitted together to an effective Hamiltonian. Because of the presence of various anharmonic resonances, the Hamiltonian includes a number of interaction constants, in addition to the conventional rotational and vibrational l-type resonance terms. The data set contains about 3400 ro-vibrational lines of 13 bands and some 1500 pure rotational lines belonging to 12 vibrational states. More than 120 spectroscopic constants have been determined directly from the fit, without any assumption deduced from theoretical calculations or comparisons with similar molecules. An extensive list of highly accurate rest frequencies has been produced to assist astronomical searches and data interpretation. These improved data, have enabled a refined analysis of the ALMA observations towards Sgr B2(N2).

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