Ion chemistry of the stratosphere

Ferguson, E. E.; Arnold, Frank

doi:10.1021/ar00071a001

Cited by 116 publications

(74 citation statements)

References 32 publications

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“…We examine extensions of this chemistry to involve molecular ionic clusters. This is quite natural because the importance of ion clusters in Earth's atmosphere was a dominant theme in the work of Eldon Ferguson (19)(20)(21)(22). cosmic bodies.…”

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confidence: 99%

“…Recent laboratory and theoretical work highlighted the properties of radical complexes with water with potentially significant chemical effects in the atmosphere (34)(35)(36)(37)47). In the D region of Earth's atmosphere, hydrated molecular clusters such as the protonated water cluster H 3 O ϩ (H 2 O) n have been observed (17,(19)(20)(21)(22). Laboratory studies suggest that series of reactions starting with NO ϩ and O 2 ϩ , formed in the atmosphere by cosmic-ray ionization (48), are responsible for their formation.…”

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confidence: 99%

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Molecular complexes in close and far away

Klemperèr

Vaida

2006

Proc. Natl. Acad. Sci. U.S.A.

110

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In this review, gas-phase chemistry of interstellar media and some planetary atmospheres is extended to include molecular complexes. Although the composition, density, and temperature of the environments discussed are very different, molecular complexes have recently been considered as potential contributors to chemistry. The complexes reviewed include strongly bound aggregates of molecules with ions, intermediate-strength hydrogen bonded complexes (primarily hydrates), and weakly bonded van der Waals molecules. In low-density, low-temperature environments characteristic of giant molecular clouds, molecular synthesis, known to involve gas-phase ion-molecule reactions and chemistry at the surface of dust and ice grains is extended here to involve molecular ionic clusters. At the high density and high temperatures found on planetary atmospheres, molecular complexes contribute to both atmospheric chemistry and climate. Using the observational, laboratory, and theoretical database, the role of molecular complexes in close and far away is discussed.P lanetary atmospheres and interstellar media have traditionally been lumped together; they are complex dynamical entities whose understanding has been and continues to be a challenge. That this subject is new may be appreciated by the fact that the knowledge that hydrogen is the abundant element of the universe is less than 100 years old. Hydrogen and helium comprise more than 99% of the universe. Thus, interstellar chemistry must be quite different from that of the atmospheres of the minor planets Mars, Earth, and Venus. Conceding the dominance of hydrogen and helium on the cosmic scale and even in the major planets, more complex molecules than H 2 attract our attention and dominate our thinking (1-4).An understanding of the chemistry of the universe must involve a wide range of processes. A bit of history with respect to interstellar chemistry is relevant to our perspective. The observed interstellar molecules, CH, CH ϩ , and CN, are quantitatively discussed by Herbig (5) in his classic study of z Oph. These species have optical transitions in spectral regions where Earth's atmosphere is transparent. It was assumed that in interstellar clouds, which were translucent and thus bathed in the galactic radiation field, the major components were atomic. Because the average density of the galaxy is 1 atom cm Ϫ1 (6) three-body processes were readily dismissed. Kramers and ter Haar (7) in 1946 presented a calculation for the formation of CH by the radiative association of C and H, i.e., C ϩ H ϭ CH ϩ photon. In 1951 Bates and Spitzer (8) showed that the CH calculated formation rate was seriously incorrect and with that ruled out synthesis by gas-phase association. Their concluding statement ushered in a lengthy period with emphasis on molecular synthesis on grain surfaces under a variety of conditions (3,(9)(10)(11).With the advent of molecular radioastronomy (12) the molecular character of giant molecular clouds could be examined. These are the largest structures within the gala...

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confidence: 99%

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Molecular complexes in close and far away

Klemperèr

Vaida

2006

Proc. Natl. Acad. Sci. U.S.A.

110

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“…The main features of the chemistry of the low-pressure region have been known for many years and are the subject of numerous reviews and will not be discussed here (1)(2)(3)(4)(5)(6)(7)(8)(9)(10). In contrast, the in situ ion composition measurements of the stratosphere and especially the troposphere have come about relatively recently, and progress is continually being made.…”

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confidence: 99%

“…These include photoionization, collisions with energetic particles and cosmic rays, and at ground level ionization from energetic particles released from radioactive decay of radon and other gases (1)(2)(3)(4)(5)(6)(7)(8)(9)(10). Although the ionization process varies, the primary ions are usually similar.…”

Section: Introductionmentioning

confidence: 99%

In situmass spectrometry and ion chemistry in the stratosphere and troposphere

Viggiano

1993

Mass Spectrometry Reviews

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“…The study of molecular ions is important in a number of fields, including physical chemistry, combustion chemistry, atmospheric chemistry, 1 and astrochemistry. 2,3 Ions are transient and reactive species, so even in plasma discharges, neutral molecules are typically ∼6 orders of magnitude more abundant than the ions of interest.…”

Section: Introductionmentioning

confidence: 99%

Ultra-sensitive high-precision spectroscopy of a fast molecular ion beam

Mills

Siller

Porambo

et al. 2011

The Journal of Chemical Physics

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Direct spectroscopy of a fast molecular ion beam offers many advantages over competing techniques, including the generality of the approach to any molecular ion, the complete elimination of spectral confusion due to neutral molecules, and the mass identification of individual spectral lines. The major challenge is the intrinsic weakness of absorption or dispersion signals resulting from the relatively low number density of ions in the beam. Direct spectroscopy of an ion beam was pioneered by Saykally and co-workers in the late 1980s, but has not been attempted since that time. Here, we present the design and construction of an ion beam spectrometer with several improvements over the Saykally design. The ion beam and its characterization have been improved by adopting recent advances in electrostatic optics, along with a time-of-flight mass spectrometer that can be used simultaneously with optical spectroscopy. As a proof of concept, a noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) setup with a noise equivalent absorption of ∼2 × 10 −11 cm −1 Hz −1/2 has been used to observe several transitions of the Meinel 1-0 band of N + 2 with linewidths of ∼120 MHz. An optical frequency comb has been used for absolute frequency calibration of transition frequencies to within ∼8 MHz. This work represents the first direct spectroscopy of an electronic transition in an ion beam, and also represents a major step toward the development of routine infrared spectroscopy of rotationally cooled molecular ions.

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Ion chemistry of the stratosphere

Cited by 116 publications

References 32 publications

Molecular complexes in close and far away

Molecular complexes in close and far away

In situmass spectrometry and ion chemistry in the stratosphere and troposphere

Ultra-sensitive high-precision spectroscopy of a fast molecular ion beam

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