# Photon emission and atomic collision processes in two-phase argon doped with xenon and nitrogen [CL]

We present a comprehensive analysis of photon emission and atomic collision processes in two-phase argon doped with xenon and nitrogen. The dopants are aimed to convert the VUV emission of pure Ar to the UV emission of the Xe dopant in the liquid phase and to the near UV emission of the N2 dopant in the gas phase. Such a mixture is relevant to two-phase dark matter and low energy neutrino detectors, with enhanced photon collection efficiency for primary and secondary scintillation signals. Based on this analysis, we show that the recently proposed hypothesis of the enhancement of the excitation transfer from Ar to N2 species in the two-phase mode is either incorrect or needs assumption about a new extreme mechanism of excitation transfer coming into force at lower temperatures, in particular that of the resonant excitation transfer via ArN2 compound (van der Waals molecule).

A. Buzulutskov
Tue, 14 Feb 17
19/71

Comments: 6 pages, 1 figure, 1 table

# Photo-stability of super-hydrogenated PAHs determined by action spectroscopy experiments [GA]

We have investigated the photo-stability of pristine and super-hydrogenated pyrene cations C$_{16}$H$_{10+m}^+, m = 0,6, \mathrm{\ or\ } 16$) by means of gas-phase action spectroscopy. Optical absorption spectra and photo-induced dissociation mass spectra are presented. By measuring the yield of mass-selected photo-fragment ions as a function of laser pulse intensity, the number of photons (and hence the energy) needed for fragmentation of the carbon backbone was determined. Backbone fragmentation of pristine pyrene ions (C$_{16}$H$_{10}^+$) requires absorption of three photons of energy just below 3 eV, whereas super-hydrogenated hexahydropyrene (C$_{16}$H$_{16}^+$) must absorb two such photons and fully hydrogenated hexadecahydropyrene (C$_{16}$H$_{26}^+$) only a single photon. These results are consistent with previously reported dissociation energies for these ions. Our experiments clearly demonstrate that the increased heat capacity from the additional hydrogen atoms does not compensate for the weakening of the carbon backbone when pyrene is hydrogenated. In photodissociation regions, super-hydrogenated Polycyclic Aromatic Hydrocarbons (PAHs) have been proposed to serve as catalysts for H$_2$-formation. Our results indicate that carbon backbone fragmentation may be a serious competitor to H$_2$-formation at least for small hydrogenated PAHs like pyrene.

M. Wolf, H. Kiefer, J. Langeland, et. al.
Thu, 15 Sep 16
14/56

Comments: 6 pages, 4 figures, accepted in The Astrophysical Journal

# Multipole Traps as Tools in Environmental Studies [CL]

Trapping of microparticles, nanoparticles and aerosols is an issue of major interest for physics and chemistry. We present a setup intended for microparticle trapping in multipole linear Paul trap geometries, operating under Standard Ambient Temperature and Pressure (SATP) conditions. A 16-electrode linear trap geometry has been designed and tested, with an aim to confine a larger number of particles with respect to quadrupole traps and thus enhance the signal to noise ratio, as well as to study microparticle dynamical stability in electrodynamic fields. Experimental tests and numerical simulations suggest that multipole traps are very suited for high precision mass spectrometry measurements in case of different microparticle species or to identify the presence of certain aerosols and polluting agents in the atmosphere. Particle traps represent versatile tools for environment monitoring or for the study of many-body Coulomb systems and dusty plasmas.

B. Mihalcea, C. Stan, L. Giurgiu, et. al.
Fri, 18 Dec 15
13/70

Comments: 17 pages, 8 figures

# Multipole Electrodynamic Ion Trap Geometries for Microparticle Confinement under Standard Ambient Temperature and Pressure Conditions [CL]

Trapping of microparticles and aerosols is of great interest for physics and chemistry. We report microparticle trapping in multipole linear Paul trap geometries, operating under Standard Ambient Temperature and Pressure (SATP) conditions. An 8-electrode and a 12-electrode linear trap geometries have been designed and tested with an aim to achieve trapping for larger number of particles and to study microparticle dynamical stability in electrodynamic fields. We report emergence of planar and volume ordered structures of the microparticles, depending on the a.c. trapping frequency and particle specific charge ratio. The electric potential within the trap was mapped using the electrolytic tank method. Particle dynamics was simulated using a stochastic Langevin equation. We emphasize extended regions of stable trapping with respect to quadrupole traps, as well as good agreement between experiment and numerical simulations.

B. Mihalcea, L. Giurgiu, C. Stan, et. al.
Fri, 18 Dec 15
21/70

Comments: 24 pages, 11 figures

# An optical spectrum of a large isolated gas-phase PAH cation: C78H26+ [IMA]

A gas-phase optical spectrum of a large polycyclic aromatic hydrocarbon (PAH) cation – C78H26 +- in the 410-610 nm range is presented. This large all-benzenoid PAH should be large enough to be stable with respect to photodissociation in the harsh conditions prevailing in the interstellar medium (ISM). The spectrum is obtained via multi-photon dissociation (MPD) spectroscopy of cationic C78H26 stored in the Fourier Transform Ion Cyclotron Resonance (FT-ICR) cell using the radiation from a mid-band optical parametric oscillator (OPO) laser. The experimental spectrum shows two main absorption peaks at 431 nm and 516 nm, in good agreement with a theoretical spectrum computed via time-dependent density functional theory (TD-DFT). DFT calculations indicate that the equilibrium geometry, with the absolute minimum energy, is of lowered, nonplanar C2 symmetry instead of the more symmetric planar D2h symmetry that is usually the minimum for similar PAHs of smaller size. This kind of slightly broken symmetry could produce some of the fine structure observed in some diffuse interstellar bands (DIBs). It can also favor the folding of C78H26 + fragments and ultimately theformation of fullerenes. This study opens up the possibility to identify the most promising candidates for DIBs amongst large cationic PAHs.

J. Zhen, G. Mulas, A. Bonnamy, et. al.
Fri, 4 Dec 15
2/64

Comments: 7 pages, 4 figures, 1 table, accepted in Molecular Astrophysics, 2015

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# Failure of hydrogenation in protecting polycyclic aromatic hydrocarbons from fragmentation [GA]

A recent study of soft X-ray absorption in native and hydrogenated coronene cations, C$_{24}$H$_{12+m}^+$ $m=0-7$, led to the conclusion that additional hydrogen atoms protect (interstellar) Polycyclic Aromatic Hydrocarbon (PAH) molecules from fragmentation [Reitsma et al., Phys. Rev. Lett. 113, 053002 (2014)]. The present experiment with collisions between fast (30-200 eV) He atoms and pyrene (C$_{16}$H$_{10+m}^+$, $m=0$, 6, and 16) and simulations without reference to the excitation method suggests the opposite. We find that the absolute carbon-backbone fragmentation cross section does not decrease but increases with the degree of hydrogenation for pyrene molecules.

M. Gatchell, M. Stockett, N. Ruette, et. al.
Wed, 28 Oct 15
47/79

Comments: 10 pages, 5 figures

# Simulating the Formation of Carbon-rich Molecules on an idealised Graphitic Surface [EPA]

There is accumulating evidence for the presence of complex molecules, including carbon-bearing and organic molecules, in the interstellar medium. Much of this evidence comes to us from studies of chemical composition, photo- and mass-spectroscopy in cometary, meteoritic and asteroid samples, indicating a need to better understand the surface chemistry of astrophysical objects. There is also considerable interest in the origins of life-forming and life-sustaining molecules on Earth. Here, we perform reactive molecular dynamics simulations to probe the formation of carbon-rich molecules and clusters on carbonaceous surfaces resembling dust grains and meteoroids. Our results show that large chains form on graphitic surfaces at low temperatures (100K – 500K) and smaller fullerene-like molecules form at higher temperatures (2000K – 3000K). The formation is faster on the surface than in the gas at low temperatures but slower at high temperatures as surface interactions prevent small clusters from coagulation. We find that for efficient formation of molecular complexity, mobility about the surface is important and helps to build larger carbon chains on the surface than in the gas phase at low temperatures. Finally, we show that the temperature of the surface strongly determines what kind of structures forms and that low turbulent environments are needed for efficient formation.

D. Marshall and H. Sadeghpour
Wed, 21 Oct 15
54/66

Comments: 13 pages, 14 figures; the manuscript has been submitted to MNRAS for publication

# Electronic transitions of jet-cooled SiC2, Si2Cn (n=1-3), Si3Cn (n=1,2), and SiC6H4 between 250 and 710 nm [CL]

Electronic transitions of the title molecules were measured between 250 and 710 nm using a mass-resolved 1+1′ resonant two-photon ionization technique at a resolution of 0.1 nm. Calculations at the B3LYP/aug-cc-pVQZ level of theory support the analyses. Because of their spectral properties, SiC$_2$, linear Si$_2$C$_2$, Si$_3$C, and SiC$_6$H$_4$ are interesting target species for astronomical searches in the visible spectral region. Of special relevance is the Si–C$_2$–Si chain, which features a prominent band at 516.4 nm of a strong transition ($f=0.25$). This band and one from SiC$_6$H$_4$ at 445.3 nm were also investigated at higher resolution (0.002 nm).

M. Steglich and J. Maier
Wed, 18 Mar 15
15/59

Comments: 15 pages, 9 figures, 5 Tables

# The electronic spectra of protonated PANH molecules [SSA]

Aims. This study was designed to examine the viability of protonated nitrogen-substituted polycyclic aromatic hydrocarbons (H+PANHs) as candidates for the carriers of the diffuse interstellar bands (DIBs). Methods. We obtained the electronic spectra of two protonated PANH cations, protonated acridine and phenanthridine, using parent ion photo-fragment spectroscopy and generated theoretical electronic spectra using ab initio calculations. Results. We show that the spectra of the two species studied here do not correspond to known DIBs. However, based on the general properties derived from the spectra of these small protonated nitrogen-substituted PAHs, we propose that larger H+PANH cations represent good candidates for DIB carriers due to the expected positions of their electronic transitions in the UV-visible and their narrow spectral bands.

J. Noble, C. Dedonder and C. Jouvet
Thu, 12 Mar 15
3/57

Comments: 7 pages, 2 figures, accepted for publication in A&A

# Rotational spectroscopy as a tool to investigate interactions between vibrational polyads in symmetric top molecules: low-lying states v8 <= 2 of methyl cyanide, CH$_3$CN [GA]

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 2nu8 around 717 cm-1 with assignments covering 684-765 cm-1. Additional spectra in the nu8 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 v8 = 1 and 2. Notably, there is a strong Delta(v8) = +- 1, Delta(K) = 0, Delta(l) = +-3 Fermi resonance between v8 = 1^-1 and v8 = 2^+2 at K = 14. Pronounced effects in the spectrum are also caused by resonant Delta(v8) = +- 1, Delta(K) = -+ 2, Delta(l) = +- 1 interactions between v8 = 1 and 2. An equivalent resonant interaction occurs between K = 14 of the ground vibrational state and K = 12, l = +1 of v8 = 1 for which we present the first detailed account. A preliminary account was given in an earlier study on the ground vibrational state. Similar resonances were found for CH3CCH and, more recently, for CH3NC, warranting comparison of the results. From data pertaining to v8 = 2, we also investigated rotational interactions with v4 = 1 as well as Delta(v8) = +- 1, Delta(K) = 0, Delta(l) = +-3 Fermi interactions between v8 = 2 and 3.
We have derived N2- and self-broadening coefficients for the nu8, 2nu8 – nu8, and 2nu8 bands from previously determined nu4 values. Subsequently, we determined transition moments and intensities for the three IR bands.

H. Muller, L. Brown, B. Drouin, et. al.
Wed, 25 Feb 15
46/55

Comments: 20 pages, 12 figures, astract abbreviated; Journal of Molecular Spectroscopy, accepted

Fri, 20 Dec 13
10/56