Infrared Spectroscopy of Jet-cooled Cationic Polyaromatic Hydrocarbons: Naphthalene[TSUP]+[/TSUP]

Piest, Hans; Helden, Gert von; Meijer, Gerard

doi:10.1086/312143

Cited by 73 publications

(74 citation statements)

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“…Using this technique, Piest et al have succeeded in measuring the IR spectrum of the naphthalene and phenanthrene cations in the gas phase. [92,93] Of direct interest here is the notable agreement between the infrared spectra obtained using this technique and those measured for the matrix isolated cations. This agreement is illustrated in Table 2 which compares the results of the two techniques for the naphthalene cation, C 10 H 8 + .…”

Section: Interstellar Pahs: the Laboratory Challengementioning

confidence: 73%

“…The excellent agreement between the matrix and gas phase data for this PAH cation validates the matrix isolation approach to this problem. 0.14 a data taken from [92]; b data taken from [57]; c data taken from [72] context of the astrophysical problem, where the natural linewidth of a vibrationally excited PAH emitting under interstellar conditions is ~30 cm -1 . This result reinforces the validity of the use of matrix isolation data for the analysis of the interstellar infrared emission spectra.…”

Section: Interstellar Pahs: the Laboratory Challengementioning

confidence: 99%

See 1 more Smart Citation

From Interstellar Polycyclic Aromatic Hydrocarbons and Ice to Astrobiology

Allamandola

Hudgins

2003

Solid State Astrochemistry

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Tremendous strides have been made in our understanding of interstellar material over the past twenty years thanks to significant, parallel developments in observational astronomy and laboratory astrophysics. Twenty years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds ignored, and the notion of large, abundant, gas phase, carbon rich molecules widespread throughout the interstellar medium (ISM) considered impossible.Today the composition of dust in the diffuse ISM is reasonably well constrained to micron-sized cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. In dense molecular clouds, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose major components are is very well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by earlier interstellar chemistry standards, is widespread throughout the Universe. This paper presents a detailed summary of these disparate interstellar components and ends by considering both of them as important feedstock to the chemical inventory of the primordial Earth. Particular attention is paid to their possible role in the chemistry that led to the origin of life. An extensive reference list is given to allow the student entry into the full depth of the literature.The first part of this paper focuses on interstellar PAHs. The laboratory and theoretical underpinning which supports the PAH model is reviewed in some detail. This is followed by a few specific examples which demonstrate how these data can be used to analyze the interstellar spectra and probe local conditions in different emission zones. These examples include tracing the evolution of carbon as it passes from its birthsite in circumstellar shells through the ISM, determining specifics about the cosmic PAH population in many different environments including PAH size and structure, and probing local conditions in the different emission zones.The second part of this paper summarizes the laboratory and observational background leading to our current understanding of interstellar/precometary ices. Although the most abundant interstellar ice components are the very simple molecules such as H 2 O, CH 3 OH, CO, CO 2 , and NH 3 , more complex species including accreted PAHs and those formed by UV and cosmic ray processing within the ice must also be present. Here we give a detailed summary of the photochemical evolution on those ices 2 found in the densest regions of molecular clouds, the regions where stars and planetary systems are formed. Ultraviolet photolysis of these ices produces a host of new compounds, some of which show intriguing prebiotic behavior.The last part of this paper draws all this information together and considers the possible roles these compounds might have played in early Earth...

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Section: Interstellar Pahs: the Laboratory Challengementioning

confidence: 73%

Section: Interstellar Pahs: the Laboratory Challengementioning

confidence: 99%

From Interstellar Polycyclic Aromatic Hydrocarbons and Ice to Astrobiology

Allamandola

Hudgins

2003

Solid State Astrochemistry

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“…Bandwidths of just a few cm −1 have been obtained for PAH species that are estimated to be expansion cooled to temperatures on the order of 20 K. These methods require the availability of IR laser sources that are continuously tunable in the 5 -15 µm spectral range and thus far free electron lasers and optical parametric oscillators have been used. Moreover, the PAHs need to be entrained in a seeded molecular beam expansion to form the weakly bound PAH-rare gas complexes, which has thus far only been possible for the smallest PAHs naphthalene (Piest et al 1999a;Ricks et al 2009) and phenanthrene (Piest et al 2001).…”

Section: Experimental Methods Comparedmentioning

confidence: 99%

“…Using the free electron laser at the FELIX facility, Meijer and coworkers recorded the gas-phase IR spectra of the naphthalene (Piest et al 1999a) and phenanthrene (Piest et al 2001) cations using a variation of the messenger-atom spectroscopy method (Piest et al 1999b). Van der Waals clusters of the PAH and a rare gas atom (Ar in most cases) were produced in a pulsed molecular beam expansion and they were resonantly ionized using a two-color resonance enhanced multiphoton ionization (REMPI) scheme.…”

Section: Messenger Atom Spectroscopymentioning

confidence: 99%

Laboratory infrared spectroscopy of PAHs

Oomens

2011

EAS Publications Series

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“…As an example of the effect of multiphon broadening versus a one photon tagged-ion spectrum, Figure 6 compares the FEL spectroscopy of naphthalene ion in the mid-IR obtained with IRMPD detection, and one-photon action spectrum of the Ar-tagged naphthalene ion obtained by Piest et al [72]. Both spectra used jet-cooled ions, and both used the FEL as a laser source, so that thermal effects and laser-linewidth effects are similar.…”

Section: B Infrared Spectroscopy Of Ionsmentioning

confidence: 99%

Ion spectroscopy: Where did it come from; where is it now; and where is it going?

Baer¹,

Dunbar

2010

J. Am. Soc. Mass Spectrom.

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a large group of mass spectrometrists working in the area of ion spectroscopy. In this introduction to the field, we provide a brief history, its current state, and where it is going. Ion spectroscopy of intermediate size molecules began with photoelectron spectroscopy in the 1960s, while electronic spectroscopy of ions using the photodissociation "action spectroscopic" mode became active in the next decade. These approaches remained for many years the main source of information about ionization energies, electronic states, and electronic transitions of ions. In recent years, highresolution laser techniques coupled with pulsed field ionization and sample cooling in molecular beams have provided high precision ionization energies and vibrational frequencies of small to intermediate sized molecules, including a number of radicals. More recently, optical parametric oscillator (OPO) IR lasers and free electron lasers have been developed and employed to record the IR spectra of molecular ions in either molecular beams or ion traps. These results, in combination with theoretical ab initio molecular orbital (MO) methods, are providing unprecedented structural and energetic information about gas-phase ions. (J Am Soc Mass Spectrom 2010, 21, 681-693) © 2010 Published by Elsevier Inc. on behalf of American Society for Mass Spectrometry T here are at least three perspectives guiding research in molecular spectroscopy of ions, which have given rise to rather distinct research communities. First is the goal of finding the quantum energy levels (electronic, vibrational, rotational) with high accuracy and energy resolution. Benefiting from experimental convenience, a vast body of results of this sort has been accumulated from photoionization and photoelectron spectroscopy experiments where the initial sample is the neutral molecule corresponding to an ion of interest.Second is the question of "what color" the ion is, that is to say, taking the ion itself as the sample, observing the wavelengths and transition intensities of the optical absorptions or emissions of the ion. These experiments are difficult, but have great interest for the study of ions found in nature, as for instance among the community of astronomers trying to sort out the telescope spectra corresponding to molecular species existing in extraterrestrial environments.Third is the use of spectra as a window to the identification and structural characterization of ionic molecules formed from interesting precursors by any of a variety of ionization, ion-molecule reaction, or ionextraction techniques. Combined with mass spectrometry, this branch of ion spectroscopy has developed into a new structural approach comparable to MS/MS, thanks to its ability to distinguish small conformational or structural differences among iso-mass ions. These studies have been dominated by the use of "action spectroscopy" (multi-photon and ion tagging dissociation techniques) to provide convenient, although indirect, access to the spectra of interesting ions.The three major parts of thi...

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Infrared Spectroscopy of Jet-cooled Cationic Polyaromatic Hydrocarbons: Naphthalene[TSUP]+[/TSUP]

Cited by 73 publications

References 21 publications

From Interstellar Polycyclic Aromatic Hydrocarbons and Ice to Astrobiology

From Interstellar Polycyclic Aromatic Hydrocarbons and Ice to Astrobiology

Laboratory infrared spectroscopy of PAHs

Ion spectroscopy: Where did it come from; where is it now; and where is it going?

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